DE-FE0029787 High Energy Systems for Transforming CO2 to … · 13-07-2017 · Research is 90% Kinetics ... • Software: Kintecus Chemical Modeling Plug flow reactor. huge # number
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Project Kickoff Meeting DE-FE0029787 High Energy Systems for Transforming CO 2 to Valuable Products > July 13 th , 2017 Osman M. Akpolat Gas Technology Institute
Project Kickoff MeetingDE-FE0029787High Energy Systems for Transforming CO2 to Valuable Products
gt July 13th 2017
Osman M AkpolatGas Technology Institute
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 2
Meeting Objectives
bull Introduction of Project Team Members
bull Short Primer on the Science and Technology of Electron Beam Deposition into Gas
bull Discussion of Electron Beam Technology and Technical Aspects of the Project
bull Quick Overview of Administrative Efforts
bull Comments and Questions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 3
Meeting Agenda
bull 100 PM Introductions
bull 110 PM Background Information on Project Team Members
bull 130 PM Technical Approach Discussion
bull 230 PM Project Structure Task description
bull 240 PM Schedule
bull 250 PM Budget
bull 300 PM Comments and Questions
bull 400 PM Adjourn
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 4
gt Independent not-for-profit research institute established by the natural gas industry
gt GTI tackles tough energy challenges turning raw technology into practical solutions
gt Downhole to the burner tip including energy conversion technologies
GTI Overview
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 5
Diverse Customers from Industry and Government
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
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063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
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127
127
111
063
095
159
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079
111
111
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143
111
143
127
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111
238
111
095
079
111
111
111
111
159
159
143
127
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127
111
111
127
127
127
111
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175
19
175
19
111
111
143
143
111
127
127
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206
206
222
206
143
079
111
127
063
127
095
222
238
238
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238
159
063
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095
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286
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079
159
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349
381
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111
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111
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254
365
413
413
444
206
111
111
111
079
175
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429
46
476
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254
127
127
127
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238
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524
571
508
302
159
127
143
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206
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413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
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778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
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Asia
10
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30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 2
Meeting Objectives
bull Introduction of Project Team Members
bull Short Primer on the Science and Technology of Electron Beam Deposition into Gas
bull Discussion of Electron Beam Technology and Technical Aspects of the Project
bull Quick Overview of Administrative Efforts
bull Comments and Questions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 3
Meeting Agenda
bull 100 PM Introductions
bull 110 PM Background Information on Project Team Members
bull 130 PM Technical Approach Discussion
bull 230 PM Project Structure Task description
bull 240 PM Schedule
bull 250 PM Budget
bull 300 PM Comments and Questions
bull 400 PM Adjourn
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 4
gt Independent not-for-profit research institute established by the natural gas industry
gt GTI tackles tough energy challenges turning raw technology into practical solutions
gt Downhole to the burner tip including energy conversion technologies
GTI Overview
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 5
Diverse Customers from Industry and Government
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
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127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
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238
159
063
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063
095
095
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27
286
302
143
079
159
143
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111
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111
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111
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254
365
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111
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111
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175
063
317
429
46
476
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254
127
127
127
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238
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524
571
508
302
159
127
143
048
206
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413
556
619
667
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381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
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825
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73
46
254
175
175
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127
095
635
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952
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81
54
286
175
159
079
095
063
698
984
1079
1032
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603
333
206
143
079
095
063
73
1159
1238
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952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
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1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
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413
111
095
032
13921
8984
627
4778
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2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
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397
079
095
032
12032
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4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
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60
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3413
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181
1079
571
27
048
143
079
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546
4032
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2429
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048
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095
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4921
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30
227
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968
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238
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5111
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127
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27
175
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095
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365
238
159
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111
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683
921
1016
10
841
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302
19
143
079
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619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
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143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
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476
27
143
127
127
079
222
095
286
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127
127
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429
19
095
111
111
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238
286
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349
143
095
143
127
048
127
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222
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254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 3
Meeting Agenda
bull 100 PM Introductions
bull 110 PM Background Information on Project Team Members
bull 130 PM Technical Approach Discussion
bull 230 PM Project Structure Task description
bull 240 PM Schedule
bull 250 PM Budget
bull 300 PM Comments and Questions
bull 400 PM Adjourn
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 4
gt Independent not-for-profit research institute established by the natural gas industry
gt GTI tackles tough energy challenges turning raw technology into practical solutions
gt Downhole to the burner tip including energy conversion technologies
GTI Overview
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 5
Diverse Customers from Industry and Government
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
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063
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159
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111
111
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127
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238
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111
111
111
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159
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254
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27
048
111
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9635
6746
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3714
273
2016
119
667
302
079
079
048
10619
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5048
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2111
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698
333
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063
11524
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4143
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2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
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6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
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381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
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6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
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6016
4476
3381
219
1175
54
143
048
016
18048
11492
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6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
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524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
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219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
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6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
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1159
492
127
048
016
18159
11492
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6032
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2175
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111
048
032
17968
11492
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6032
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219
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127
063
032
1781
11444
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1159
524
143
048
016
17619
11333
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4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
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2175
1159
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143
063
048
17238
11127
7921
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143
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048
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6032
4444
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127
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111
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127
111
048
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3238
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143
111
016
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10556
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427
3175
2048
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508
127
111
016
15921
10429
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3095
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127
111
048
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10286
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111
063
15492
10127
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3016
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1032
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14635
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127
032
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048
11175
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10222
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286
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143
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111
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095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
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541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
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3423
2673
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1031
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332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
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6166
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1223
681
402
315
315
0
7965
6567
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4384
3301
227
1258
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315
332
0
8821
69
5729
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2305
1258
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437
332
332
1817
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349
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366
1951
12191
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1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 4
gt Independent not-for-profit research institute established by the natural gas industry
gt GTI tackles tough energy challenges turning raw technology into practical solutions
gt Downhole to the burner tip including energy conversion technologies
GTI Overview
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 5
Diverse Customers from Industry and Government
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
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Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 5
Diverse Customers from Industry and Government
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
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127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
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206
206
222
206
143
079
111
127
063
127
095
222
238
238
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238
159
063
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095
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111
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111
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111
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175
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317
429
46
476
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254
127
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127
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524
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302
159
127
143
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556
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667
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381
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127
159
063
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063
476
635
714
73
635
429
222
159
19
048
143
079
556
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73
46
254
175
175
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127
095
635
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952
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81
54
286
175
159
079
095
063
698
984
1079
1032
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603
333
206
143
079
095
063
73
1159
1238
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952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
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857
1587
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81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
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46
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111
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238
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127
143
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206
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127
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127
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111
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127
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079
095
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127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
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3179
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315
315
0
7965
6567
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4384
3301
227
1258
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402
315
332
0
8821
69
5729
4506
3388
2305
1258
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437
332
332
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9729
7231
5939
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349
7091
10672
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4716
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2376
1362
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437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
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6254
4821
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241
1415
734
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315
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19475
12209
8122
6254
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1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
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699
437
349
384
12733
11213
7965
627
4838
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1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 6
GTI provides solutions to clients in the private sector federal government and state government agencies gt 300+ active projectsgt 20 patents issuedgt 10 patent applications
2016 Results
Business Highlights
DIVERSE CUSTOMER BASE
NEWBUSINESS
CONTRACTS
FEDERAL
INDUSTRYUTILITIES
STATELOCAL
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 7
1940 1950 1960 1970 1980 1990 2000 2010
Oil Crisis
1976Federal Power Commission approved surcharge on pipeline transmission for research funding and Gas Research Institute (GRI) formed1973
1941Institute for Gas Technology (IGT) formed at the Illinois Institute of Technology (IIT)
Company History
FERC Order No 636 Restructuring Rule mandated unbundling to separate sales from transportation services
1992
GRI and IGT combined to form the Gas Technology Institute (GTI)
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
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159
063
095
095
238
254
27
286
302
143
079
159
143
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111
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333
349
381
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111
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111
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254
365
413
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444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
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238
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524
571
508
302
159
127
143
048
206
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413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
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825
825
73
46
254
175
175
048
127
095
635
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952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
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952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
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327
2413
146
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397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Protect Enhance and Save Lives - 16 -
IBA Industrial250+ Electron beam accelerators installed worldwide
Americas55
Asia14
EMEA28
ROW3
IBA Installed base
Crosslinking72
RampD9
Sterilization
18
Other1
Applications
36 +Rhodotron
200 +Dynamitron
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
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095
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032
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127
111
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111
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
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454
175
0
0
0
0
0
0
0
366
978
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489
315
0
0
0
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28
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1118
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402
14
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262
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035
0
0
0
1275
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559
384
419
14
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0
2131
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2008
1572
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244
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0
2602
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454
384
332
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152
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193
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475
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11
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384
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2008
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0
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315
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2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Protect Enhance and Save Lives - 17 -
IBArsquos product portfolio
Dynamitron05 -gt 5 MeV | 160 mA
Electron beam
Rhodotron3 -gt 10 MeV | 245 kW
Electron beam and X-rays
eXelis5 ndash 7 MeV | 560kW
X-rays
Main application E-beam Crosslinking Main application E-beam box sterilization Main application X-ray pallet sterilization
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
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0
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Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Protect Enhance and Save Lives - 18 -
Rhodotron and Dynamitron product ranges
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
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127
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206
206
222
206
143
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111
127
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127
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222
238
238
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238
159
063
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095
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159
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381
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111
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111
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365
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206
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111
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175
063
317
429
46
476
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254
127
127
127
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238
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524
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508
302
159
127
143
048
206
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556
619
667
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381
175
127
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063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
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73
46
254
175
175
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127
095
635
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81
54
286
175
159
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095
063
698
984
1079
1032
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603
333
206
143
079
095
063
73
1159
1238
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683
381
238
159
063
127
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778
1349
1429
1302
1111
73
429
27
175
063
175
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857
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81
476
27
159
048
19
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952
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181
1651
1349
889
556
302
159
032
159
095
1127
2238
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146
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317
19
032
159
079
1397
2651
2317
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1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
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381
222
048
127
063
2968
3556
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246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
5667
4175
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
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6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
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5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
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2952
1841
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46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
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4937
3635
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1651
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111
095
032
13921
8984
627
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841
397
127
111
063
13381
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111
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397
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032
12032
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73
397
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079
048
11175
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30
2175
1333
73
349
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095
063
10222
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2825
2079
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317
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079
063
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1952
1143
635
286
079
079
063
8175
60
4365
3413
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1079
571
27
048
143
079
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546
4032
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254
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19
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6206
4921
3714
30
227
1619
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508
238
032
159
095
5111
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46
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143
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73
413
238
032
143
063
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2905
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119
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365
222
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127
2476
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1048
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032
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1413
952
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016
159
095
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173
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1317
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524
286
143
032
175
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1492
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1413
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444
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063
19
079
762
127
1349
1238
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397
27
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063
159
095
714
1095
1159
1111
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365
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063
111
079
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10
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143
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492
286
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175
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524
683
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127
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444
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667
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397
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143
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143
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381
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635
54
349
159
111
159
048
19
063
333
46
492
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476
27
143
127
127
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222
095
286
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429
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111
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143
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143
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111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Protect Enhance and Save Lives - 19 -
IBA Industrial Inc ndash Markets
Sterilization Crosslinking
Food Sterile Insect
Cargo screeningMail Sanitization
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
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Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Chart1
Dynamitron Market by Product
13
31
17
24
9
6
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
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095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
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127
127
111
063
095
159
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079
111
111
095
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111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
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127
111
111
127
127
127
111
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175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
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238
159
063
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095
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079
159
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111
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111
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429
46
476
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254
127
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127
143
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667
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381
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73
635
429
222
159
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048
143
079
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46
254
175
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127
095
635
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81
54
286
175
159
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063
698
984
1079
1032
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603
333
206
143
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095
063
73
1159
1238
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381
238
159
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127
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778
1349
1429
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73
429
27
175
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857
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476
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159
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19
079
952
1889
181
1651
1349
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556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
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1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
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1079
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1984
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159
111
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10
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46
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19
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127
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206
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127
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206
111
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127
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111
111
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127
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111
111
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127
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143
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111
095
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127
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127
111
127
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063
048
079
095
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111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
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366
978
734
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315
0
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0
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28
874
1118
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14
0
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262
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035
0
0
0
1275
2096
1817
1449
943
559
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419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
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2777
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3057
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2026
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3354
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193
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105
0
1555
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209
0
3109
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3423
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1031
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349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
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3179
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1223
681
402
315
315
0
7965
6567
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4384
3301
227
1258
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315
332
0
8821
69
5729
4506
3388
2305
1258
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437
332
332
1817
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7231
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437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
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1362
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437
349
384
12733
11213
7965
627
4838
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349
384
6638
1041
772
6148
4803
3545
2445
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402
332
366
1187
9502
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5991
4734
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241
1327
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384
315
332
0
8594
6935
5764
4594
3423
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1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Others
Wire and Cable
Shrink Tube
Shrink Film
Tires
Service Centers
Continent
Dynamitron Market by Continent
10
30
60
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
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063
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063
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159
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111
111
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127
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238
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111
111
111
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159
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254
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111
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6746
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3714
273
2016
119
667
302
079
079
048
10619
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5048
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2111
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698
333
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063
11524
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1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
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079
048
13048
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5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
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3444
2508
1571
825
397
127
127
063
14095
9095
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4841
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1619
857
397
127
111
063
14444
9365
6556
50
3683
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1683
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413
111
095
032
14746
9603
6714
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381
2794
1746
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413
159
143
048
15048
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6889
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3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
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10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
2175
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54
127
079
048
17317
11159
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6032
446
3365
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524
143
079
048
17524
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6016
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508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
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6016
4476
3381
219
1175
54
143
048
016
18048
11492
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6048
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524
127
048
032
18238
11492
7921
6032
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508
111
048
016
18413
11476
7905
6032
4429
3381
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524
127
095
016
18619
11476
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6032
446
3381
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524
143
159
032
18889
11476
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6032
4492
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524
175
159
048
19048
11444
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6032
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524
175
143
032
19032
11476
8016
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556
222
159
032
19016
1146
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6032
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219
1175
524
159
127
032
18794
11476
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6032
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175
175
048
18524
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6032
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524
143
143
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18349
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6032
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492
127
048
016
18159
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032
17968
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6032
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127
063
032
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143
048
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11333
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4492
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508
127
032
032
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11206
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143
063
048
17238
11127
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143
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127
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111
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143
111
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427
3175
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127
111
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15921
10429
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111
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111
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15492
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1032
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11175
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111
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095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
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3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
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402
315
332
0
8821
69
5729
4506
3388
2305
1258
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437
332
332
1817
9729
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437
332
349
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241
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332
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315
366
200
12313
814
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2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Asia
Europe
USA
Sheet1
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
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Asia
10
Europe
30
USA
60
Others
13
Wire and Cable
31
Shrink Tube
17
Shrink Film
24
Tires
9
Service Centers
6
Sheet2
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
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063
095
095
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27
286
302
143
079
159
143
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111
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238
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333
349
381
159
111
143
111
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048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
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952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
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2413
146
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397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
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1032
556
254
048
19
095
6206
4921
3714
30
227
1619
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508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
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1952
1349
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444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
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119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
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651
365
238
159
063
111
079
683
921
1016
10
841
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302
19
143
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063
619
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889
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492
286
175
175
063
095
079
524
683
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778
698
46
254
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175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
Sheet3
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 20
SUNY - Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
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063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
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095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
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127
127
111
063
095
159
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079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
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127
111
111
127
127
127
111
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175
19
175
19
111
111
143
143
111
127
127
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206
206
222
206
143
079
111
127
063
127
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238
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238
159
063
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095
095
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111
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111
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429
46
476
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254
127
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127
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429
222
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048
143
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46
254
175
175
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127
095
635
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81
54
286
175
159
079
095
063
698
984
1079
1032
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603
333
206
143
079
095
063
73
1159
1238
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381
238
159
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127
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778
1349
1429
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73
429
27
175
063
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857
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476
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159
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19
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952
1889
181
1651
1349
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556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
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1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
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5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
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111
095
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627
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2571
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841
397
127
111
063
13381
8714
60
4603
3381
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154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
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30
2175
1333
73
349
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095
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10222
7016
4937
3857
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2079
1254
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317
079
079
063
9222
6556
4651
3635
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1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
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1286
73
413
238
032
143
063
1667
2905
2476
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119
667
365
222
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143
063
127
2476
2222
1952
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1048
619
317
206
032
159
095
1032
2095
1952
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952
587
317
175
016
159
095
905
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173
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524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 21
SUNY-Environmental Science and Forestry
bull 8 Departments (Bio Paper Sci Forestry Landscape Arch Env Studies Sci Eng
bull 2000 undergrads 550 grad students
Chemistry MS and PhD bull Biochemistrybull Environmental Chemistrybull Organic Natural Products bull Polymer Chemistry
15 Faculty40 grad students
Theodore S Dibble SUNY
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
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0
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297
454
053
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175
0
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0
366
978
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315
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035
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2008
1572
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332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 22
Professor of ChemistrySUNY-Environmental Science amp Forestry
(tsdibbleesfedu)bull SUNY-ESF
1 of 7 PhD-granting SUNY campusesLocated in Syracuse
bull My Training PhD (Physical Chemistry) U Michigan 1992
bull My Research Group 1 MS 1 PhD 1 undergrad(1 MS and 1 PhD student arriving in Fall)
Theodore S Dibble SUNY
Theodore S Dibble
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 23
Research is 90 Kineticsbull Tools Experiment Theory Kinetic Models
Lasers to generate and monitor radicalsGas chromatography-mass spectrometryInfrared spectroscopyQuantum chemistry theoretical kineticsReaction mechanismsLarge kinetic models
bull TopicsAtmospheric ozone and mercuryCombustionElectron beams
Theodore S Dibble SUNY
Research Background
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
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063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
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095
079
095
127
143
079
111
127
111
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048
063
111
079
079
095
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127
127
127
111
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095
159
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079
111
111
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111
143
127
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238
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111
111
111
111
159
159
143
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111
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19
175
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254
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127
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1397
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079
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238
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143
079
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238
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175
111
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27
048
111
079
9635
6746
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273
2016
119
667
302
079
079
048
10619
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5048
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2111
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333
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063
11524
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4143
3063
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1349
714
365
063
079
063
12365
8079
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319
2349
1413
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397
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048
13048
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5857
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2444
1492
794
397
095
095
032
13603
8825
6111
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3444
2508
1571
825
397
127
127
063
14095
9095
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4841
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1619
857
397
127
111
063
14444
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6556
50
3683
2746
1683
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413
111
095
032
14746
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6714
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381
2794
1746
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413
159
143
048
15048
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6889
5286
3921
2873
181
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444
175
159
063
15349
10016
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40
2968
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10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
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4302
319
2079
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508
127
111
016
16571
10762
7587
5841
4333
3254
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1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
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54
127
079
048
17317
11159
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6032
446
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524
143
079
048
17524
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6016
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143
063
048
17698
11381
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60
4492
3381
2175
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508
143
048
016
17873
1146
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6016
4476
3381
219
1175
54
143
048
016
18048
11492
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6048
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3365
2206
1175
524
127
048
032
18238
11492
7921
6032
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508
111
048
016
18413
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6032
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3381
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524
127
095
016
18619
11476
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6032
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3381
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524
143
159
032
18889
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6032
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175
159
048
19048
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6032
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175
143
032
19032
11476
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222
159
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19016
1146
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6032
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159
127
032
18794
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6032
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175
175
048
18524
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524
143
143
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6032
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492
127
048
016
18159
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111
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17968
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6032
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219
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127
063
032
1781
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1159
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143
048
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17619
11333
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4492
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508
127
032
032
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11206
7952
6032
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143
063
048
17238
11127
7921
6048
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143
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2159
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127
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111
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127
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2095
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143
111
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10556
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427
3175
2048
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508
127
111
016
15921
10429
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3095
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1079
476
127
111
048
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10286
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4127
3048
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1063
444
159
111
063
15492
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1937
1032
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111
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127
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429
19
159
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14635
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127
032
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11175
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238
032
159
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5111
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1349
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 24
Previous Work Humid Air (N2 O2 H2O)
Goal understand sources of OH radical (removes SO2 and NOx from flue gas)
bull Started with a published model- added reactions- edited rate constants amp reaction products- iterated until ldquoself-consistentrdquo (~900 reactions)
bull Ran model- tested againstreintepreted exp results- analyzed sources of OH amp error
Theodore S Dibble SUNY
Kinetic Modeling of Electron Beams
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 25
bull Software Kintecus Chemical ModelingPlug flow reactorhuge number of reactionsAccurate numerical integration
bull Input ParametersDose rate (Joules absorbedkg gas) from IBAInitial species concentrationsSet of reactions and rate constants
bull Outputs Concentrations vs timeSensitivity coefficients
Theodore S Dibble SUNY
Technical Details
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
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063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
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111
111
111
111
159
159
143
127
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127
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111
127
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127
111
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175
19
175
19
111
111
143
143
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127
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206
206
222
206
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238
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46
476
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254
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302
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381
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635
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222
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048
143
079
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46
254
175
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81
54
286
175
159
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143
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063
73
1159
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381
238
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127
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1349
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429
27
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19
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302
159
032
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095
1127
2238
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146
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032
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079
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333
222
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3095
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381
222
048
127
063
2968
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246
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429
238
032
159
048
4333
4063
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2016
1397
825
46
254
048
159
079
5571
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2175
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889
476
238
048
143
079
6587
5127
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3079
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10
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238
032
175
111
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1063
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254
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079
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2603
1873
1095
603
27
048
111
079
9635
6746
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3714
273
2016
119
667
302
079
079
048
10619
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5048
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2111
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698
333
095
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063
11524
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4143
3063
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1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
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079
048
13048
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5857
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2444
1492
794
397
095
095
032
13603
8825
6111
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3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
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6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
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6889
5286
3921
2873
181
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444
175
159
063
15349
10016
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40
2968
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10
46
159
127
048
15587
10206
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4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
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4302
319
2079
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508
127
111
016
16571
10762
7587
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4333
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1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
2175
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54
127
079
048
17317
11159
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6032
446
3365
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524
143
079
048
17524
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6016
4492
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2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
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6016
4476
3381
219
1175
54
143
048
016
18048
11492
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6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
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1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
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524
127
095
016
18619
11476
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6032
446
3381
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524
143
159
032
18889
11476
7968
6032
4492
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524
175
159
048
19048
11444
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6032
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219
1175
524
175
143
032
19032
11476
8016
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2238
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556
222
159
032
19016
1146
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6032
4492
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219
1175
524
159
127
032
18794
11476
7952
6032
4492
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219
1175
54
175
175
048
18524
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7921
6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
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3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
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2175
1159
508
111
048
032
17968
11492
7968
6032
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219
1175
54
127
063
032
1781
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6016
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3365
219
1159
524
143
048
016
17619
11333
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60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
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2175
1175
524
143
079
048
17127
11063
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6032
4444
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2159
1159
556
127
063
048
16984
10952
7778
5937
4429
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2127
1143
54
111
095
048
16714
10841
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4365
3254
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127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
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508
127
111
016
15921
10429
7381
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4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
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1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
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5349
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175
127
048
14937
9746
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2825
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952
429
19
159
063
14635
9508
6651
5095
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1714
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413
143
127
032
14317
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032
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397
127
111
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11175
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10222
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1143
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286
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4365
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27
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143
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1619
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238
032
159
095
5111
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1413
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016
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032
175
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1492
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444
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063
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079
762
127
1349
1238
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27
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159
095
714
1095
1159
1111
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365
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063
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079
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10
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143
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492
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175
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524
683
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127
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444
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667
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397
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143
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381
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635
54
349
159
111
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048
19
063
333
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492
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476
27
143
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222
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429
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079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 26
Technical Approach Discussion
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 27
High Energy Systems for Transforming CO2 to Valuable Products
Sponsor
Funding $799997 DOE ($206000 co-funding) two year effort
Objective Develop a direct electron beam (E-Beam) synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide using carbon dioxide (CO2) captured from a coal-fired power plant and methane (natural gas)
Team Member Rolesbull Overall project integration and managementbull Design construct the E-Beam reactor and the testing unitbull Conceptual design for coal-fired power plants with DEBS
bull Provide guidance in E-Beam reactor design and E-Beam accelerator for testing
bull Develop a kinetic model for the E-Beam reactor
DE-FE0029787
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
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127
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206
206
222
206
143
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111
127
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127
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222
238
238
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238
159
063
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095
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159
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381
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111
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111
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365
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206
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111
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175
063
317
429
46
476
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254
127
127
127
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238
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524
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508
302
159
127
143
048
206
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556
619
667
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381
175
127
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063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
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73
46
254
175
175
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127
095
635
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81
54
286
175
159
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095
063
698
984
1079
1032
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603
333
206
143
079
095
063
73
1159
1238
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683
381
238
159
063
127
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778
1349
1429
1302
1111
73
429
27
175
063
175
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857
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81
476
27
159
048
19
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952
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181
1651
1349
889
556
302
159
032
159
095
1127
2238
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146
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317
19
032
159
079
1397
2651
2317
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1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
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381
222
048
127
063
2968
3556
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246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
5667
4175
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
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6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
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5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
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2952
1841
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46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
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4937
3635
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1651
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111
095
032
13921
8984
627
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841
397
127
111
063
13381
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111
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397
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032
12032
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73
397
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079
048
11175
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30
2175
1333
73
349
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095
063
10222
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2825
2079
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317
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079
063
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1952
1143
635
286
079
079
063
8175
60
4365
3413
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1079
571
27
048
143
079
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546
4032
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254
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19
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6206
4921
3714
30
227
1619
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508
238
032
159
095
5111
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46
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143
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73
413
238
032
143
063
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2905
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119
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365
222
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127
2476
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1048
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032
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1413
952
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016
159
095
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173
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1317
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524
286
143
032
175
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1492
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1413
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444
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063
19
079
762
127
1349
1238
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397
27
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063
159
095
714
1095
1159
1111
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365
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063
111
079
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10
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143
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492
286
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175
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524
683
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127
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444
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667
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397
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143
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143
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381
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635
54
349
159
111
159
048
19
063
333
46
492
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476
27
143
127
127
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222
095
286
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429
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111
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143
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143
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111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 28
Project Objectives
OBJECTIVES
The objective of this project is to develop the Direct E-Beam Synthesis (DEBS) process to produce valuable chemicals such as acetic acid methanol and carbon monoxide at relatively low severity (pressure being near one atmosphere and temperatures of lt150degC) from near-pure CO2 captured from a pulverized coal (PC)-fired power plant and methane imported as natural gas Creating valuable products will offset the cost of carbon capture and storage (CCS) The high energy output from an electron beam (E-Beam) accelerator will be used to break chemical bonds The project comprises two budget periods (BP) of 9 and 15 months each for a total duration of 24 months
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 29
Project ObjectivesBP Objectives
1
bull Complete design and manufacture of testing skid with E-Beam reactor for testing at IBAbull Successful commissioning of DEBS equipment at GTI and IBA
bull Identify at least two catalysts to control the recombination and increase the yields for more valuableproducts
bull Develop preliminary predictive kinetic model to guide BP2 testing
2
bull Determine key operating parameters at various E-Beam energies to maximize the per pass conversion of CO2 to valuable products control selectivities between various products and minimize E-Beam energy requirements
bull Identify operating conditions and catalyst combinations to further control selectivities between products and minimize overall energy requirements
bull Review experimental data to optimize and improve preliminary kinetic model developed in BP1bull Complete data analysis and reporting of the experimental runs
bull Complete economical assessment techno-economic analysis and perform life cycle analysis for the process
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
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079
111
111
111
111
159
159
143
127
238
127
111
111
127
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127
111
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175
19
175
19
111
111
143
143
111
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127
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206
206
222
206
143
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222
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238
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429
46
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254
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302
159
127
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635
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222
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048
143
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46
254
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286
175
159
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143
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238
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127
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302
159
032
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095
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2238
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146
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032
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079
1397
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635
333
222
032
159
079
1937
3095
2587
2238
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381
222
048
127
063
2968
3556
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246
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1302
762
429
238
032
159
048
4333
4063
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2667
2016
1397
825
46
254
048
159
079
5571
4603
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2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
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4175
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
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3714
273
2016
119
667
302
079
079
048
10619
7206
5048
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2111
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698
333
095
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063
11524
7635
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3063
2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
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2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
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6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
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1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
2175
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54
127
079
048
17317
11159
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6032
446
3365
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524
143
079
048
17524
11238
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6016
4492
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2159
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508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
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6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
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508
111
048
016
18413
11476
7905
6032
4429
3381
2175
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524
127
095
016
18619
11476
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6032
446
3381
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524
143
159
032
18889
11476
7968
6032
4492
3381
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524
175
159
048
19048
11444
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6032
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3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
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556
222
159
032
19016
1146
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6032
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219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
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6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
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3381
2175
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508
111
048
032
17968
11492
7968
6032
4476
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219
1175
54
127
063
032
1781
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6016
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3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
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1159
508
143
063
048
17238
11127
7921
6048
4444
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524
143
079
048
17127
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6032
4444
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2159
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556
127
063
048
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10952
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54
111
095
048
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4365
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127
111
048
16492
10698
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4317
3238
2095
1143
508
143
111
016
16222
10556
7492
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427
3175
2048
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508
127
111
016
15921
10429
7381
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4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
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1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
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5349
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1841
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46
175
127
048
14937
9746
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2825
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952
429
19
159
063
14635
9508
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1714
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413
143
127
032
14317
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032
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397
127
111
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11175
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286
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8175
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27
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238
032
159
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5111
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143
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222
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127
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1413
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587
317
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016
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095
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286
143
032
175
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1492
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1413
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444
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063
19
079
762
127
1349
1238
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27
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095
714
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063
111
079
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921
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10
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302
19
143
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492
286
175
175
063
095
079
524
683
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46
254
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048
127
095
444
603
667
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397
19
143
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143
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381
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635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
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127
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222
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254
349
381
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429
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095
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111
063
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048
238
286
317
333
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143
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143
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063
222
254
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27
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 30
Experiments will be conducted in non-catalytic as well as catalytic modes A kinetic model will be developed by SUNY based on the collected data and will be
used to predict the chemical performance of the DEBS process A conceptual design for coupling the DEBS process to a coal-fired power plant will
be developed
This project will expand on the concept of DEBS to Develop a commercially viable process Minimize E-Beam energy requirements Maximize CO2 conversion Selectively control the yield of more valuable products using
catalysts
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
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222
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524
159
127
032
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11476
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6032
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048
18524
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524
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492
127
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016
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508
111
048
032
17968
11492
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6032
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127
063
032
1781
11444
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6016
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219
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524
143
048
016
17619
11333
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60
4492
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2159
1159
508
127
032
032
17444
11206
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6032
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508
143
063
048
17238
11127
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524
143
079
048
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11063
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6032
4444
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2159
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556
127
063
048
16984
10952
7778
5937
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2127
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54
111
095
048
16714
10841
7667
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3254
2127
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508
127
111
048
16492
10698
7571
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4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 31
Current technology for the commercial production of acetic acid methanol and carbon monoxide requires High temperatures and pressures Expensive catalysts in multiple process steps High capital and operating costs
The DEBS process uses high-energy electron beams to break chemical bonds allowing production of the desired chemicals at near-ambient pressure and temperatures and has been demonstrated by other research groups at bench-scale
Successfully combining DEBS technology with CO2 captured from coal-fired power plant flue gas provides a low-cost energy-efficient process to produce valuable chemicals and reduce emissions
Advantages Over Traditional Processes
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
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0
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297
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053
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175
0
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0
366
978
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315
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035
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2008
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4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 32
Electron Beam Deposition into Gas
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 33
Electron Beam Primer
V = Voltage (eV)I = Current (amp)V x I = Power (watt)
1eV = Kinetic energy of an electron accelerated to 1 voltCharge of an electron = 1602 x 10-19 coulombs
1 coulomb = 625 x 1018 electrons
Current = ChargeTime1 amp = 1 coulomb 1 sec
1 eV x 1 amp= 1 watt = 1 Jsec1 eV = 1602 x 10-19 J
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 34
Electron Beam Primer
500keV amp 15mAsqin E-Beam on a 1 sq in areaE-Beam power = 750 watt or 750 Jsec
Each electron will have500000 x 1602 x 10-19 = 8 x 10-14 J of energy
E-Beam will have15 x 10-3 1602 x 10-19 = 93633 x 1015 electrons per second
Each electron has the potential to achieve ~100000 interactions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
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079
111
111
111
111
159
159
143
127
238
127
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111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
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127
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206
206
222
206
143
079
111
127
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127
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222
238
238
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095
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111
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111
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063
317
429
46
476
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254
127
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302
159
127
143
048
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381
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476
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635
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222
159
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048
143
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46
254
175
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127
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81
54
286
175
159
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698
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206
143
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238
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127
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429
27
175
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27
159
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19
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181
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302
159
032
159
095
1127
2238
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146
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19
032
159
079
1397
2651
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1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
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381
222
048
127
063
2968
3556
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246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
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2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
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4175
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
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3714
273
2016
119
667
302
079
079
048
10619
7206
5048
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2889
2111
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698
333
095
079
063
11524
7635
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4143
3063
2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
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2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
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524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
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524
127
095
016
18619
11476
7937
6032
446
3381
2175
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524
143
159
032
18889
11476
7968
6032
4492
3381
2175
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524
175
159
048
19048
11444
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6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
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556
222
159
032
19016
1146
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6032
4492
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219
1175
524
159
127
032
18794
11476
7952
6032
4492
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219
1175
54
175
175
048
18524
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6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
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3381
2175
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508
111
048
032
17968
11492
7968
6032
4476
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219
1175
54
127
063
032
1781
11444
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6016
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3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
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2175
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524
143
079
048
17127
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6032
4444
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2159
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556
127
063
048
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10952
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4429
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54
111
095
048
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10841
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4365
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127
111
048
16492
10698
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4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
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508
127
111
016
15921
10429
7381
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4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
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1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
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5349
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1841
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46
175
127
048
14937
9746
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2825
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429
19
159
063
14635
9508
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413
143
127
032
14317
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032
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397
127
111
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11175
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286
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27
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238
032
159
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5111
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143
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587
317
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016
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032
175
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1492
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1413
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444
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063
19
079
762
127
1349
1238
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27
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095
714
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063
111
079
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10
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302
19
143
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492
286
175
175
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095
079
524
683
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46
254
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048
127
095
444
603
667
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397
19
143
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143
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381
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635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
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444
238
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127
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222
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254
349
381
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429
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095
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111
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048
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317
333
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143
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143
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063
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27
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127
0
0
0
0
0
752
297
454
053
0
0
0
0
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0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
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1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 35
Industrial Accelerator Design (linear)
Typical Numbers in range of interest450 to 1000 keV25 to 250 mA11 - 100 kW1
Efficiency 45 ndash 602
1 Robert W Hamm RampM Technical Enterprises Inc 9th ICFA Seminar ndash October 30 20082 Applied Energetics httpwwwappliedenergeticscomdownloadsproduct-offeringsnested-high-voltage-generatorpdf3 Kim et Al amp NHV Japan amp Bulgaria Power Plant
Source of Electrons
Acceleration Modules
Electron beam
Large Scale Industrial Applications800 keV500 mA400 kW3
Efficiency up to 883
Vacuum
Foil
Target
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
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1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 36
Electron Beam Deposition
Maximum efficiency occurs when electron beam deposition depth is equal to reactor depthDeposition depth depends on these parametersbull Electron beam voltagebull Gas compositionbull Gas pressure (Limited by foil)bull Foil composition and thicknessre
acto
r dep
th=
d
ElectronBeam Voltage ndash Controls how FAR the electrons will go
Current - Controls how MANY electrons will go
Beam Energy
Beam
Dep
th
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
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NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 37
Electron Beam Deposition (continued)
Electron beam inVoltage VinCurrent IExposure time T
Electron beam outVoltage Vout = Vin - ∆VCurrent IExposure time T
Dose = ((Vin-Vout) times I times T) M
Dose = energy deposited per unit massUnit of dose 1 Joulekg = 1 Gray
mass M
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
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079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
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127
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206
206
222
206
143
079
111
127
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222
238
238
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063
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095
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111
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111
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111
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063
317
429
46
476
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254
127
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508
302
159
127
143
048
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381
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476
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73
635
429
222
159
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048
143
079
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46
254
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175
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127
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81
54
286
175
159
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698
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143
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063
73
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381
238
159
063
127
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73
429
27
175
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476
27
159
048
19
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181
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556
302
159
032
159
095
1127
2238
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146
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317
19
032
159
079
1397
2651
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1111
635
333
222
032
159
079
1937
3095
2587
2238
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1222
698
381
222
048
127
063
2968
3556
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246
1873
1302
762
429
238
032
159
048
4333
4063
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2667
2016
1397
825
46
254
048
159
079
5571
4603
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2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
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10
524
238
032
175
111
7556
5667
4175
3286
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
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698
333
095
079
063
11524
7635
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4143
3063
2222
1349
714
365
063
079
063
12365
8079
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
1873
10
46
159
127
048
15587
10206
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5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
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6032
4444
3349
2175
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54
127
079
048
17317
11159
7921
6032
446
3365
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524
143
079
048
17524
11238
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6016
4492
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2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
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524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
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524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
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3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
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219
1175
54
127
063
032
1781
11444
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6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
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2175
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524
143
079
048
17127
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6032
4444
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2159
1159
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127
063
048
16984
10952
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54
111
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048
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10841
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127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
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1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
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5349
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1841
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46
175
127
048
14937
9746
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2825
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429
19
159
063
14635
9508
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1714
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413
143
127
032
14317
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095
032
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397
127
111
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11175
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286
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238
032
159
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5111
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016
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032
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1413
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444
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063
19
079
762
127
1349
1238
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27
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095
714
1095
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365
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063
111
079
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921
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10
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302
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143
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492
286
175
175
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524
683
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46
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048
127
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444
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667
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19
143
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143
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381
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635
54
349
159
111
159
048
19
063
333
46
492
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476
27
143
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127
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222
095
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238
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429
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095
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048
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143
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222
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27
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 38
Deposition into a Gas Flowing in a Reactor
Flow velocity v
Dose = (V (potential) times I (currentarea) times a (window area) v (velocity)) M (mass)
Mass M
ElectronBeam
e-beam window area = a
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
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111
079
238
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333
349
381
159
111
143
111
048
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048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
2175
1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
16714
10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
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222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
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3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
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1362
699
437
349
384
6638
1041
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6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 39
Electron Beam Primer
C-H bond energy ~5eV
One 500keV electron can break approximately 100000 x (5 eV) bonds
Bond Dissociation Energies
Bond ΔHƒ298 (kJmol)
C-C 607
C-H 3372
C-O 10765
C=O 749
CequivO 1075
Dehydrogenation of CHx
ΔH (kJmol)
CH4 rarr CH3∙ + H∙ 405
CH3∙ rarr CH2∙ + H∙ 439
CH2∙ rarr CH∙ + H∙ 488
CH∙ rarr C + H∙ 685
CH4 rarr CH2∙ + 2H∙ 808
CH4 rarr C + 4H∙ 1266
CH2∙ rarr C + 2H∙ 857
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
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2016
119
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302
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048
10619
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11524
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063
12365
8079
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319
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1413
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397
079
079
048
13048
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397
095
095
032
13603
8825
6111
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397
127
127
063
14095
9095
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4841
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1619
857
397
127
111
063
14444
9365
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50
3683
2746
1683
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413
111
095
032
14746
9603
6714
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381
2794
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413
159
143
048
15048
9841
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3921
2873
181
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444
175
159
063
15349
10016
7079
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40
2968
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10
46
159
127
048
15587
10206
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4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
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10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
2175
1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
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524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
3381
219
1175
524
159
127
032
18794
11476
7952
6032
4492
3381
219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
1175
524
143
143
032
18349
11476
7905
6032
4444
3381
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1159
492
127
048
016
18159
11492
7952
6032
4444
3381
2175
1159
508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
4492
3365
219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
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508
143
063
048
17238
11127
7921
6048
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524
143
079
048
17127
11063
7857
6032
4444
3333
2159
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556
127
063
048
16984
10952
7778
5937
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54
111
095
048
16714
10841
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127
111
048
16492
10698
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3238
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508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
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3635
2698
1651
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413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
079
079
063
9222
6556
4651
3635
2683
1952
1143
635
286
079
079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
968
508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
2778
2365
1825
1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
079
079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
159
175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
079
127
079
079
111
143
079
143
127
111
095
063
048
095
079
095
111
143
079
111
127
111
063
063
048
095
079
111
143
127
079
127
127
095
048
063
063
079
079
095
127
111
095
127
111
127
063
048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
1362
699
437
349
384
12733
11213
7965
627
4838
3581
2463
1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 40
Monte Carlo Simulation
Monte Carlo simulations are used to model the probability of different outcomes in a process that cannot easily be predicted due to the intervention of random variables
bull The electron trajectories are simulated by using a Monte Carlo method
bull Each electron enters the reactor with a given energy and its trajectory is followed
until it comes to rest or exits the reactor
bull To simulate a beam the process is repeated for a large number of electrons
bull Secondary electrons are generated and tracked within the fast secondary model
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
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095
111
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063
063
095
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127
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063
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111
127
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111
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111
143
127
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238
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111
111
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111
159
159
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19
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206
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238
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119
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127
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016
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143
111
032
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2127
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110
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111
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127
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17317
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127
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016
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143
159
032
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6032
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175
159
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143
032
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159
127
032
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175
175
048
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524
143
143
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048
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127
063
032
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143
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4492
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508
127
032
032
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143
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048
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143
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111
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3238
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143
111
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3175
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127
111
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
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489
402
14
0
0
0
0
0
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124
803
506
402
262
0
0
0
0
454
1624
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1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
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366
315
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0
3057
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349
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0
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152
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0
193
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0
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0
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0
475
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11
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384
349
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0
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2008
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612
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332
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0
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0
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315
315
0
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0
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0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 41
Initial electrons energy 800 keVEnergy cut-off 1 keVResults from EGS-4 code calculated at JAERI Takasaki
Y crossection of RV X crossection of RV
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
Estimation of Electron Paths in Flue Gas Treatment
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 42
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
079
175
063
317
429
46
476
46
254
127
127
127
079
238
079
365
476
524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
159
063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
714
825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
1159
952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
079
857
1587
1603
1476
1238
81
476
27
159
048
19
079
952
1889
181
1651
1349
889
556
302
159
032
159
095
1127
2238
2048
1841
146
984
603
317
19
032
159
079
1397
2651
2317
2032
1603
1111
635
333
222
032
159
079
1937
3095
2587
2238
1746
1222
698
381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
3286
2492
173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
095
079
063
11524
7635
5349
4143
3063
2222
1349
714
365
063
079
063
12365
8079
5619
4317
319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
6365
4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
937
413
159
143
048
15048
9841
6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
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2175
1159
508
143
048
016
17873
1146
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6016
4476
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219
1175
54
143
048
016
18048
11492
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6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
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2175
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508
111
048
016
18413
11476
7905
6032
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524
127
095
016
18619
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143
159
032
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175
143
032
19032
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8016
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222
159
032
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1146
7968
6032
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219
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159
127
032
18794
11476
7952
6032
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219
1175
54
175
175
048
18524
11476
7921
6032
446
3397
2175
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524
143
143
032
18349
11476
7905
6032
4444
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2175
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492
127
048
016
18159
11492
7952
6032
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2175
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508
111
048
032
17968
11492
7968
6032
4476
3365
219
1175
54
127
063
032
1781
11444
7984
6016
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219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
2159
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508
127
032
032
17444
11206
7952
6032
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508
143
063
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7921
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2159
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127
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127
111
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143
111
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427
3175
2048
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508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
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4048
3016
1937
1032
46
159
111
048
15222
9968
70
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2952
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46
175
127
048
14937
9746
6825
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3873
2825
1794
952
429
19
159
063
14635
9508
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5095
3746
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1714
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413
143
127
032
14317
9254
6476
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1651
905
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111
095
032
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397
127
111
063
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154
81
397
111
111
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349
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095
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317
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1952
1143
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286
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60
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181
1079
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27
048
143
079
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546
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254
048
19
095
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30
227
1619
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238
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159
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5111
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46
238
048
143
079
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444
254
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143
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238
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119
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365
222
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206
032
159
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524
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127
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175
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095
714
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1111
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10
841
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302
19
143
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063
619
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889
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492
286
175
175
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524
683
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46
254
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127
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667
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397
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143
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143
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381
524
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635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
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222
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286
413
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238
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222
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254
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381
397
429
19
095
111
111
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048
238
286
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333
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143
127
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127
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222
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254
27
27
159
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222
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238
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127
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175
19
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127
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206
111
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127
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238
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111
111
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127
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111
206
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127
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063
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143
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127
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111
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032
111
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143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
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1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
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1415
734
402
315
384
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12209
8122
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4803
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2445
1398
752
419
315
366
200
12313
814
6254
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138
716
437
315
366
1951
12191
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472
349
349
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11843
8087
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437
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384
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716
402
332
366
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5991
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241
1327
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384
315
332
0
8594
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384
315
315
0
7685
6533
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4437
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2288
1293
681
384
315
349
0
6864
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524
4262
3232
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646
402
332
366
0
6061
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4087
3126
2079
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612
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332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
700keVY
ampC]
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
079
095
127
143
079
111
127
111
095
048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
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127
063
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246
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1302
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048
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4063
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2667
2016
1397
825
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254
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079
5571
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238
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079
6587
5127
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524
238
032
175
111
7556
5667
4175
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173
1063
571
254
048
175
079
8587
6222
4476
3492
2603
1873
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27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
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2111
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333
095
079
063
11524
7635
5349
4143
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2222
1349
714
365
063
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063
12365
8079
5619
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319
2349
1413
762
397
079
079
048
13048
8508
5857
4508
3302
2444
1492
794
397
095
095
032
13603
8825
6111
4667
3444
2508
1571
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397
127
127
063
14095
9095
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4841
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1619
857
397
127
111
063
14444
9365
6556
50
3683
2746
1683
921
413
111
095
032
14746
9603
6714
5159
381
2794
1746
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413
159
143
048
15048
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6889
5286
3921
2873
181
968
444
175
159
063
15349
10016
7079
5397
40
2968
1873
10
46
159
127
048
15587
10206
7206
5508
4095
3032
1952
1048
46
159
111
048
15778
10349
7317
5635
4159
3048
2016
1079
46
143
111
063
16048
10476
7444
573
4222
3127
2032
1095
492
127
111
032
16349
10619
7524
581
4302
319
2079
1127
508
127
111
016
16571
10762
7587
5841
4333
3254
2095
1143
508
143
111
032
16873
10889
7714
5905
4397
327
2127
1127
524
127
095
048
17048
110
7825
5984
4429
3302
2143
1143
54
111
079
048
17143
11095
7873
6032
4444
3349
2175
1175
54
127
079
048
17317
11159
7921
6032
446
3365
2175
1175
524
143
079
048
17524
11238
7968
6016
4492
3381
2159
1143
508
143
063
048
17698
11381
7984
60
4492
3381
2175
1159
508
143
048
016
17873
1146
7968
6016
4476
3381
219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
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1159
508
111
048
016
18413
11476
7905
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127
095
016
18619
11476
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524
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159
032
18889
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19048
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524
175
143
032
19032
11476
8016
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556
222
159
032
19016
1146
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6032
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219
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524
159
127
032
18794
11476
7952
6032
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219
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54
175
175
048
18524
11476
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3397
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524
143
143
032
18349
11476
7905
6032
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492
127
048
016
18159
11492
7952
6032
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111
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032
17968
11492
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6032
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219
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54
127
063
032
1781
11444
7984
6016
4492
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219
1159
524
143
048
016
17619
11333
7984
60
4492
3381
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508
127
032
032
17444
11206
7952
6032
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508
143
063
048
17238
11127
7921
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143
079
048
17127
11063
7857
6032
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2159
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127
063
048
16984
10952
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5937
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54
111
095
048
16714
10841
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508
127
111
048
16492
10698
7571
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3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
905
413
111
095
032
13921
8984
627
4778
3508
2571
1603
841
397
127
111
063
13381
8714
60
4603
3381
2476
154
81
397
111
111
063
12794
8333
5762
4429
327
2413
146
778
397
079
095
032
12032
7905
5524
4238
3143
2302
1381
73
397
079
079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
4937
3857
2825
2079
1254
698
317
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079
063
9222
6556
4651
3635
2683
1952
1143
635
286
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079
063
8175
60
4365
3413
2556
181
1079
571
27
048
143
079
7159
546
4032
3206
2429
1698
1032
556
254
048
19
095
6206
4921
3714
30
227
1619
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508
238
032
159
095
5111
4381
3397
2794
2095
1492
857
46
238
048
143
079
3778
3873
3079
2587
1952
1349
794
444
254
048
143
063
2492
3365
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2365
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1286
73
413
238
032
143
063
1667
2905
2476
2159
1683
119
667
365
222
032
143
063
127
2476
2222
1952
1556
1048
619
317
206
032
159
095
1032
2095
1952
1762
1413
952
587
317
175
016
159
095
905
1762
173
1587
1317
873
524
286
143
032
175
095
825
1492
154
1413
119
778
444
254
159
063
19
079
762
127
1349
1238
1048
698
397
27
175
063
159
095
714
1095
1159
1111
905
651
365
238
159
063
111
079
683
921
1016
10
841
587
302
19
143
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079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
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778
698
46
254
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175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
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127
127
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222
079
254
349
381
397
429
19
095
111
111
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048
238
286
317
333
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143
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127
063
222
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254
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27
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222
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238
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048
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19
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206
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111
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127
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143
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127
111
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127
111
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111
175
111
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063
032
111
079
063
095
095
143
127
0
0
0
0
0
752
297
454
053
0
0
0
0
0
0
0
0
856
664
454
175
0
0
0
0
0
0
0
366
978
734
489
315
0
0
0
0
0
0
28
874
1118
786
489
402
14
0
0
0
0
0
908
1415
124
803
506
402
262
0
0
0
0
454
1624
1659
1345
856
506
384
402
035
0
0
0
1275
2096
1817
1449
943
559
384
419
14
0
0
0
2131
2323
2008
1572
1031
628
402
402
244
0
0
0
2602
2516
2201
1729
1153
699
454
384
332
0
0
0
2777
2725
2393
1886
1275
768
489
366
315
0
0
0
3057
2986
2585
2026
1398
821
541
384
349
0
0
0
3354
3232
2777
2201
152
891
524
384
349
0
0
193
372
351
2986
2358
1607
925
524
402
332
105
0
1555
4053
379
3232
2533
1712
978
524
437
332
209
0
3109
4454
4104
3423
2673
1799
1031
541
402
332
349
0
475
4856
4402
3634
2795
1886
11
577
384
349
366
0
5484
5293
4681
3825
2935
2008
1153
612
366
332
366
0
6288
5729
4961
4018
3057
2114
1205
664
384
297
349
0
7126
6166
5222
4209
3179
2201
1223
681
402
315
315
0
7965
6567
5484
4384
3301
227
1258
664
402
315
332
0
8821
69
5729
4506
3388
2305
1258
681
437
332
332
1817
9729
7231
5939
4628
3476
2358
1327
681
437
332
349
7091
10672
7581
6096
4716
351
2376
1362
699
437
349
349
13205
11441
7878
6201
4803
351
241
1398
716
402
332
366
17973
11965
8052
6254
4821
3528
241
1415
734
402
315
384
19475
12209
8122
6254
4803
3528
2445
1398
752
419
315
366
200
12313
814
6254
4803
3581
2463
138
716
437
315
366
1951
12191
8157
6288
4803
3598
2463
1362
699
472
349
349
18148
11843
8087
6305
4838
3616
2463
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699
437
349
384
12733
11213
7965
627
4838
3581
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1362
699
437
349
384
6638
1041
772
6148
4803
3545
2445
1327
716
402
332
366
1187
9502
7406
5991
4734
3494
241
1327
699
384
315
332
0
8594
6935
5764
4594
3423
2358
1327
716
384
315
315
0
7685
6533
552
4437
3319
2288
1293
681
384
315
349
0
6864
6061
524
4262
3232
2218
1258
646
402
332
366
0
6061
5624
4961
4087
3126
2079
1187
612
419
332
402
0
524
5153
4681
3895
2969
1957
1136
612
419
349
402
0
3773
4699
4366
372
2795
1834
1083
612
419
349
402
0
2008
4315
4069
3494
2638
1764
1048
594
402
332
402
0
541
3913
3773
3266
248
1659
1013
577
402
332
297
0
0
3563
3476
3022
2341
1572
943
541
384
315
175
0
0
3248
3197
2813
2183
1449
874
506
349
332
035
0
0
3057
2917
2602
2043
1327
803
489
366
366
0
0
0
1992
2707
241
1886
1223
734
472
332
366
0
0
0
996
2498
2236
1729
1136
699
454
349
366
0
0
0
018
2288
2079
1589
1048
664
402
366
297
0
0
0
0
1974
1921
1433
978
628
384
454
175
0
0
0
0
1205
1817
1309
891
594
384
524
053
0
0
0
0
524
1293
1205
839
559
419
366
0
0
0
0
0
0
716
11
768
541
454
193
0
0
0
0
0
0
122
1048
734
524
472
0
0
0
0
0
0
0
0
891
681
437
437
0
0
0
700keV_X
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
175
159
143
079
016
143
016
048
095
127
159
159
143
079
063
063
032
095
095
079
095
079
127
127
095
063
048
063
048
079
095
095
111
095
143
111
095
048
063
063
095
079
095
143
127
095
143
127
111
063
063
048
095
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095
127
143
079
111
127
111
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048
063
111
079
079
095
143
079
127
127
127
111
063
095
159
079
079
111
111
095
143
111
143
127
095
111
238
111
095
079
111
111
111
111
159
159
143
127
238
127
111
111
127
127
127
111
159
175
19
175
19
111
111
143
143
111
127
127
19
206
206
222
206
143
079
111
127
063
127
095
222
238
238
238
238
159
063
143
159
063
095
095
238
254
27
286
302
143
079
159
143
063
111
079
238
302
333
349
381
159
111
143
111
048
159
048
254
365
413
413
444
206
111
111
111
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175
063
317
429
46
476
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254
127
127
127
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238
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365
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524
571
508
302
159
127
143
048
206
079
413
556
619
667
571
381
175
127
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063
143
063
476
635
714
73
635
429
222
159
19
048
143
079
556
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825
825
73
46
254
175
175
048
127
095
635
825
952
937
81
54
286
175
159
079
095
063
698
984
1079
1032
873
603
333
206
143
079
095
063
73
1159
1238
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952
683
381
238
159
063
127
079
778
1349
1429
1302
1111
73
429
27
175
063
175
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857
1587
1603
1476
1238
81
476
27
159
048
19
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952
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181
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556
302
159
032
159
095
1127
2238
2048
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146
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317
19
032
159
079
1397
2651
2317
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1111
635
333
222
032
159
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1937
3095
2587
2238
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381
222
048
127
063
2968
3556
2889
246
1873
1302
762
429
238
032
159
048
4333
4063
3206
2667
2016
1397
825
46
254
048
159
079
5571
4603
3508
2873
2175
1556
889
476
238
048
143
079
6587
5127
3841
3079
2333
1667
10
524
238
032
175
111
7556
5667
4175
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173
1063
571
254
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175
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8587
6222
4476
3492
2603
1873
1095
603
27
048
111
079
9635
6746
4762
3714
273
2016
119
667
302
079
079
048
10619
7206
5048
3937
2889
2111
1286
698
333
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063
11524
7635
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3063
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1349
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365
063
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063
12365
8079
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319
2349
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397
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079
048
13048
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4508
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2444
1492
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397
095
095
032
13603
8825
6111
4667
3444
2508
1571
825
397
127
127
063
14095
9095
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4841
3556
2635
1619
857
397
127
111
063
14444
9365
6556
50
3683
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032
14746
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381
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143
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15048
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10016
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1079
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143
111
063
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573
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127
111
032
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143
111
032
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327
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110
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54
111
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048
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6032
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54
127
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048
17317
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446
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143
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143
063
048
17698
11381
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60
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2175
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508
143
048
016
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1146
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6016
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219
1175
54
143
048
016
18048
11492
7968
6048
446
3365
2206
1175
524
127
048
032
18238
11492
7921
6032
4444
3381
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1159
508
111
048
016
18413
11476
7905
6032
4429
3381
2175
1175
524
127
095
016
18619
11476
7937
6032
446
3381
2175
1175
524
143
159
032
18889
11476
7968
6032
4492
3381
2175
1175
524
175
159
048
19048
11444
7968
6032
4492
3381
219
1175
524
175
143
032
19032
11476
8016
5984
4476
3381
2238
1175
556
222
159
032
19016
1146
7968
6032
4492
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219
1175
524
159
127
032
18794
11476
7952
6032
4492
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219
1175
54
175
175
048
18524
11476
7921
6032
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3397
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524
143
143
032
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11476
7905
6032
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492
127
048
016
18159
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7952
6032
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508
111
048
032
17968
11492
7968
6032
4476
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219
1175
54
127
063
032
1781
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1159
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143
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016
17619
11333
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60
4492
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2159
1159
508
127
032
032
17444
11206
7952
6032
4476
3381
2175
1159
508
143
063
048
17238
11127
7921
6048
4444
3365
2175
1175
524
143
079
048
17127
11063
7857
6032
4444
3333
2159
1159
556
127
063
048
16984
10952
7778
5937
4429
3286
2127
1143
54
111
095
048
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10841
7667
5873
4365
3254
2127
1143
508
127
111
048
16492
10698
7571
5841
4317
3238
2095
1143
508
143
111
016
16222
10556
7492
5778
427
3175
2048
1111
508
127
111
016
15921
10429
7381
5698
4206
3095
2016
1079
476
127
111
048
15698
10286
7286
5587
4127
3048
1984
1063
444
159
111
063
15492
10127
7159
5476
4048
3016
1937
1032
46
159
111
048
15222
9968
70
5349
3968
2952
1841
984
46
175
127
048
14937
9746
6825
5222
3873
2825
1794
952
429
19
159
063
14635
9508
6651
5095
3746
2778
1714
937
413
143
127
032
14317
9254
6476
4937
3635
2698
1651
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413
111
095
032
13921
8984
627
4778
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2571
1603
841
397
127
111
063
13381
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60
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3381
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154
81
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111
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12794
8333
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397
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095
032
12032
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4238
3143
2302
1381
73
397
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079
048
11175
746
5238
4063
30
2175
1333
73
349
079
095
063
10222
7016
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2079
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317
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286
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8175
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1032
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19
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6206
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3714
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1619
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508
238
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159
095
5111
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857
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143
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1349
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286
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175
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1492
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1413
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444
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063
19
079
762
127
1349
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27
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095
714
1095
1159
1111
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651
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063
111
079
683
921
1016
10
841
587
302
19
143
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079
063
619
778
889
889
794
492
286
175
175
063
095
079
524
683
778
778
698
46
254
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175
048
127
095
444
603
667
698
603
397
19
143
175
048
143
079
381
524
571
635
54
349
159
111
159
048
19
063
333
46
492
524
476
27
143
127
127
079
222
095
286
413
444
444
444
238
127
127
127
079
222
079
254
349
381
397
429
19
095
111
111
063
175
048
238
286
317
333
349
143
095
143
127
048
127
063
222
254
254
27
27
159
079
159
159
063
111
079
206
222
222
238
238
159
048
127
143
063
095
095
175
19
19
206
206
127
095
111
127
079
127
111
159
159
175
159
206
111
127
127
127
111
127
127
159
143
127
111
238
127
111
111
127
127
111
111
143
127
079
111
206
111
079
079
095
111
127
111
111
111
063
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127
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079
111
143
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143
127
111
095
063
048
095
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095
111
143
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111
127
111
063
063
048
095
079
111
143
127
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127
127
095
048
063
063
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079
095
127
111
095
127
111
127
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048
063
048
079
095
079
111
079
127
111
175
111
079
063
032
111
079
063
095
095
143
127
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 43
The luminance of air nitrogen within Radiation Field areaPicture taken at Accno 2 JAERI TRCRE
500keV
800keV
Dose Distribution Visualization
Ref Presentation by Sylwester Bułka et al International Atomic Energy Agency Meeting on Electron Beam Flue Gas Treatment Warsaw Poland 14 ndash 18 May 2007
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 44
Determination of Reactor Depth in Flue Gas Treatment
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Ref Mao Benjiang ldquoFlue Gas Desulphuration and Denitration with Electron Beam Irradiation and Ammonia reagentrdquo 2005
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 45
Technology Technical approach
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 46
Key Experimental Parameters
bull E-Beam dose (kJgm)bull Gas residence time in beam and off beam (ms)bull E-Beam energy 300-500 keVbull Use of a promoter such as carbon monoxidebull Use of catalyst(s)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 47
bull E-Beam Energy Consumption kJgm of Methane
bull Estimate based on the heat of reaction for a model reaction (direct production of liquid fuels from methane)
Example Reaction
gt 8 CH4 = C8 H18 (Isooctane) + 7 H2
(Endothermic Heat of Reaction = 293 kJgm methane)
H2 yield ~110 wt of feed methane
Target Range of E-Beam Dose
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 48
Target Range of E-Beam Dose (continued) gt Experimental Data indicate ~ 4-7 kJgm methane (as electrical energy) for E-
Beam based pure methane conversion to H2 C2-C4 gases amp C5+ liquid fuels
Ref Vinokurov et al Chemistry amp Technology of Fuels and Oils V-41 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 49
gt For a mixture with 50 mol CH4 and 50 mol CO2
based on the endothermic heat of reaction for
CO2 + CH4 = CO + CH3OHthe theoretical energy need would be about 77 KJgm of methane
gt Assuming 30 E-Beam losses in the reactor this would be ~11 KJgm methanegt Initially we can use a target value of ~15 KJgm methane feed
Target Range of E-Beam Dose (continued)
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 50
E-Beam Plasma-based Chemical Reactions are Ultra-fast
gt ldquoDue to very high concentrations of ions radicals ion-radicals and other reactive particles in E-Beam plasma chemical reactions take place at extremely high rates of ~001-10 millisecondsrdquo
Ref Vinokurov et al ldquoPlasma-Chemical Processing of Natural Gasrdquo Chem amp Tech of Fuels and Oils Vol 41 No 2 2005
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 51
Electron Beam Flue Gas Treatment
Schematic diagram of the EBFGT technologyRef Kim et al ldquoElectron-beam Flue-gas Treatment Plant for Thermal Power Station ldquoSvilozardquo AD in Bulgariardquo J of the Korean Physical Society Vol 59 No 6 December 2011 pp 34943498
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 52
Data for H2 from Methane Residence Time ~2 ms
Ref ldquoH2 Production from Methane in E-Beam Plasmardquo Sharafutdinov et al Technical Physics Letter Vol 31 2005
For E-Beam based H2production from methane literature data indicates average gas residence time of about 2 milliseconds
Target Range of Gas Residence Time
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 53
Target Range of Gas Residence Time (continued)
Gas feed rate std litersmin 1 6
H2 yield (wt methane) 235 67
C2-C4 (wt CH4) 85 377
C5+ liquids (wt CH4) none 556
Carbon (wt CH4) 68 none
Yield of liquids is favored at lower Gas Residence Times (vs H2)
Ref Vinokurov et al data Chemistry and Technology of Fuels amp Oils V-41 2 2005
For maximum liquid productions from methane gas residence time should be about 02-10 milliseconds
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 54
gt Literature data for typical gas residence times (or gas velocities) for E-Beam based removal of SOXNOX from power plant flue gas show
For pilot plant studies Williams et al have reported E-Beam reactor gas velocities of about 13-26 meterssecond
gt For an experimental E-Beam reactor with a cross-flow interaction of feed gas amp E-beam over 3 cc volume amp an effective area of 15 sqcm for gas flow we would need a gas flow of 100 std litersmin to allow ~2 ms gas residence time
The Gas velocity would be ~11 meterssecond
Target Range of Gas Residence Time (continued)
Ref K Williams et al ldquoExpts For Very High Power E-Beam Systems for Utility Stack Gas Treatmentrdquo Rad Phys Chem V-31 1-3 pp 29-44 1988
Arunabha Basu Consultant
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 55
Target Range of Gas Residence Time (continued)
Vinokurov et Al had tested CO2CH4 (11 molar ratio) conversion with Corona-discharge and barrier-discharge type plasma
bull ~43 per pass methane conversion with Corona discharge (vs~15 with Barrier discharge)
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
bull Design of Experimentbull Data Analysisbull Economics
GTIMr Vann Bush
Managing DirectorInternal consultant
SUNYDr Theodore Dibble
bull Reaction Kinetics Consultation
bull Model development
IBAMr Rick Galloway
bull E-Beam Consultationbull Management of IBA
activities
GTIMr Howard Meyerbull Project Overviewbull Project
Managementbull Project QAQC
GTIMr Timothy Tamale
System Integration and Testing
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 60
Project Structure ndash Task Description
Budget Period 1 and 2
Task 10 ndash Project Management and Planningbull GTI will coordinate and plan the project activities with Team Members at IBA and SUNY GTI will
report technical progress and financial status to DOENETL throughout the duration of the project
bull GTI shall coordinate activities in order to effectively accomplish the work and ensure that project
plans results and decisions are appropriately documented and project reporting and briefing
requirements are satisfied
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized
without the specific written authorization of the Contracting Officerbull Successful completion of all work proposed in Budget Period 1bull Satisfactory achievement of applicable success criteria as identified in the PMPbull Submission and approval of a Continuation Application in accordance with the terms and conditions
of the award
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
Innovation non-equilibrium process that breaks bonds directly unlike conventional chemistry that requires heating the entire molecule
Advantages Over Traditional Processes
Electron Beam Deposition into Gas
Electron Beam Primer
Electron Beam Primer
Industrial Accelerator Design (linear)
Electron Beam Deposition
Electron Beam Deposition (continued)
Deposition into a Gas Flowing in a Reactor
Electron Beam Primer
Monte Carlo Simulation
Estimation of Electron Paths in Flue Gas Treatment
Dose Maps for Crossections of a Reaction Vessel
Dose Distribution Visualization
Determination of Reactor Depth in Flue Gas Treatment
Technology Technical approach
Key Experimental Parameters
Target Range of E-Beam Dose
Target Range of E-Beam Dose (continued)
Target Range of E-Beam Dose (continued)
E-Beam Plasma-based Chemical Reactions are Ultra-fast
Electron Beam Flue Gas Treatment
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target Range of Gas Residence Time (continued)
Target for Promoters
Limitations of Experimental Approach
Administrative Efforts
Planned Project Team
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Structure ndash Task Description
Project Schedule ndash Budget Period 1
Project Schedule ndash Budget Period 2
Budget ndash Project Funding Profile
Turning Raw Technology into Practical Solutions
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 61
Project Structure ndash Task DescriptionBudget Period 1
Task 20 ndashDesign and Construction of Experimental System
Subtask 21 ndash Reactor Design and Construction
Subtask 22 ndash Test Unit Design and Construction
Subtask 23 ndash Catalyst Selection
Task 30 ndash Start-Up and System Checks at GTI
Task 40 ndashSystem Commissioning at IBA
Task 71 - Develop Preliminary Kinetic Model
GoNo Go Decision Point ndash Budget Period 2 work under this agreement shall not be authorized without the specific written authorization of the Contracting Officer
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 62
Project Structure ndash Task Description
Budget Period 2
Task 50 - Conduct Parametric Testing
Subtask 51 Initial scoping experiments
Subtask 52 Co-current flow testing
Subtask 53 Parametric testing
Task 60 - Conduct Parametric Testing with Catalyst
Task 72 - Develop Kinetic Model
Task 80 - Data Analysis Life Cycle Analysis and Economics
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 63
Project Schedule ndash Budget Period 1
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 64
Project Schedule ndash Budget Period 2
NETL Project Kickoff Meeting DE-FE0029787 - High Energy Systems for Transforming CO2 to Valuable Products 65
Budget ndash Project Funding Profile
Budget Period 1 Budget Period 2 Total Project
05012017-01312018 02012018-04302019Government
ShareCost Share Government
ShareCost Share Government
ShareCost Share
Gas Technology Institute $150763 $0 $221811 $0 $372574 $0
