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Radiation Physics and Chemistry 76 (2007) 14801484

Industrial applications of electron beam flue gas treatmentFrom

laboratory to the practice

Andrzej G. Chmielewskia,b,

aInstitute of Nuclear Chemistry and Technology, Warsaw, PolandbFaculty of Chemical and Process Engineering, Warsaw University of Technology, Warsaw, Poland

Abstract

The electron beam technology for flue gas treatment (EBFGT) has been developed in Japan in the early 1980s. Later on, this process

was investigated in pilot scale in the USA, Germany, Japan, Poland, Bulgaria and China. The new engineering and process solutions

have been developed during the past two decades. Finally industrial plants have been constructed in Poland and China. The high

efficiency of SOx

and NOx

removal was achieved (up to 95% for SOx

and up to 70% for NOx

) and by-product is a high quality fertilizer.

Since the power of accelerators applied in industrial installation is over 1 MW and requested operational availability of the plant is equal

to 8500 h in year, it is a new challenge for radiation processing applications.

r 2007 Elsevier Ltd. All rights reserved.

Keywords: Electron accelerator; Flue gas treatment; Sulfur dioxide; Nitrogen oxides; VOC

1. Introduction

The municipal and industrial activities of the man lead to

environment degradation. The pollutants are emitted to the

atmosphere with off-gases from industry, power stations,

residential heating systems and vehicles. Fossil fuels, which

include coal, natural gas, petroleum, shale oil and bitumen

are the main source of heat and electrical energy. All these

fuels contain beside major constituents (carbon, hydrogen,

oxygen) other materials as metal, sulfur and nitrogen

compounds. During the combustion process different

pollutants as fly ash, sulfur oxides (SO2and SO3), nitrogen

oxides (NOx NO2+NO) and volatile organic com-

pounds are emitted. Fly ash contains different traceelements (heavy metals). Gross emission of pollutants is

tremendous all over the world. These pollutants are present

in the atmosphere in such conditions that they can affect

man and his environment. Air pollution caused by

particulate matter and other pollutants not only acts

directly on environment but by contamination of water and

soil leads to their degradation. Wet and dry deposition of

inorganic pollutants leads to acidification of environment.

These phenomena affect health of the people, increase

corrosion of metal structures, historical buildings and

monuments. Widespread forest damage has been reported

in Europe and North America regions. Many cultivated

plants are not resistant to these pollutants either especially

in the early period of vegetation. The mechanisms of

pollutants transformation in atmosphere are described by

environmental chemistry. Photochemistry plays an impor-

tant role in these transformations. SO2 and NOx are

oxidized and sulfuric and nitric acids are formed in

presence of water vapor, fog and droplets. Other discussed

problem connected with human activities is emission ofvolatile organic compounds to the atmosphere. These

emissions cause stratospheric ozone layer depletion, ground

level photochemical ozone formation, toxic or carcinogenic

human health effects, enhancing the global greenhouse

effect, accumulation and persistence in environment

(Chmielewski, 2002). Waters in the open and underground

reservoirs are being polluted, as well as cultivated soil and

forests. Most of the plants, especially coniferous trees are

not resistant to sulfur oxides. In recent years, investigation

has shown that emission to the atmosphere of volatile

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0969-806X/$ - see front matterr 2007 Elsevier Ltd. All rights reserved.

doi:10.1016/j.radphyschem.2007.02.056

Fax: +48 22 8111532.

E-mail addresses: A.Chmielewski@ichtj.waw.pl,

A.Chmielewski@ichip.pw.edu.pl (A.G. Chmielewski).

http://www.elsevier.com/locate/radphyschemhttp://localhost/var/www/apps/conversion/tmp/scratch_8/dx.doi.org/10.1016/j.radphyschem.2007.02.056mailto:A.Chmielewski@ichtj.waw.pl,mailto:A.Chmielewski@ichtj.waw.pl,mailto:A.Chmielewski@ichip.pw.edu.plmailto:A.Chmielewski@ichip.pw.edu.plmailto:A.Chmielewski@ichip.pw.edu.plmailto:A.Chmielewski@ichtj.waw.pl,http://localhost/var/www/apps/conversion/tmp/scratch_8/dx.doi.org/10.1016/j.radphyschem.2007.02.056http://www.elsevier.com/locate/radphyschem

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organic compounds (VOC) can cause stratospheric

ozone layer depletion, ground level photochemical

ozone formation, and toxic or carcinogenic human health

effects.

They contribute to the global greenhouse effect adding a

new dimension to the environmental degradation as a

result of burning of fossil fuels. Chlorinated organicpollutants which are emitted from fossil fuel power plants,

municipal waste incinerators, chemical industry are very

harmful to the environment and human being. Recent

studies reported that chlorinated benzenes or phenols are

suspected as precursors for dioxins emissions. Dioxins are

relatively chemical inert and demonstrate long lifetime in

environment, therefore they are called persistent organic

pollutants (POPs). They are transported by air and are

deposited on the surfaces of the soil, water and plants.

Then they may enter human food chain. Consequently, the

problems associated with air pollutants emission are no

longer just local or regional, but have become continental

in scope. The situation regarding environment contamina-

tion is becoming critical (EOLSS, 2001, 2002). Therefore

the economically and technically feasible technologies for

pollution control are searched for. The radiation offers

advanced solutions to the selected problems as well

(Chmielewski, 2005; Cooper et al., 1998; SNU, 2003;

IAEA, 2005).

2. Process theory

Wet flue gas desulfurization (FGD) and selective

catalytic reduction (SCR) can be applied for flue gas

treatment and SO2 and NOx emission control. VOCs areusually adsorbed on carbon, but this process is rarely used

for lean hydrocarbon concentrations up to now. All these

technologies are complex chemical processes and waste,

like wastewater, gypsum and used catalyst are generated

(Srivastava et al., 2001).

Electron beam technology is among the most promising

advanced technologies of new generation. This is a dry-

scrubbing process of simultaneous SO2and NOx removal,

where no waste except the by-products are generated.

Studies show that irradiation of flue gases with an electron

beam can bring about chemical changes that make removal

of sulfur and nitrogen oxides easier. The main components

of flue gases are N2, O2, H2O, and CO2, with much lower

concentration of SOx

and NOx

. NH3may be present as an

additive to aid removal of the sulfur and nitrogen oxides.

Radiation energy is absorbed by gas components in

proportion to their mass fraction in the mixture. The fast

electrons slow down and secondary electrons are formed

which play important role in overall energy transfer. After

irradiation, fast electrons interact with gas creating various

ions and radicals, the primary species formed include e,

N2+, N+, O2

+, O+, H2O+, OH+, H+, CO2

+, CO+, N2*,

O2*, N, O, H, OH, and CO. In the case of high water vapor

concentration the oxidizing radicals OHd and HO2d and

excited ions as O(3P) are the most important products.

These species take part in a variety of ionmolecule

reactions, neutralization reactions, dimerization (Person

and Ham, 1988). The SO2, NO, NO2, and NH3 present

cannot compete with the reactions because of very low

concentrations, but react with N, O, OH, and HO2radicals. After humidification and lowering its tempera-

ture, flue gases are guided to reaction chamber, whereirradiation by electron beam takes place. Ammonia is

injected upstream the irradiation chamber. There are

known several pathways of NO oxidation. In the case of

electron beam treatment the most important are as follows

(Ma tzing and Paur, 1992):

NO O3P M ! NO2 M;

O3P O2 M ! O3 M;

NO O3 M ! NO2 O2 M;

NO HO2d

M ! NO2 d

OH M:

After the oxidation NO2 is converted to nitric acid in the

reaction with OHd according to the reaction:

NO2 dOH M ! HNO3 M:

HNO3 aerosol reacts with NH3 giving ammonium nitrate

that can be written

HNO3 NH3 ! NH4NO3:

Partly NO is reduced to atmospheric nitrogen.

There can be also several pathways of SO2 oxidation

depending on the conditions. In the electron beam

treatment the most important are radio-thermal andthermal reactions (Tokunaga and Suzuki, 1984).

Radio-thermal reactions proceed through radical oxida-

tion of SO2 in the reaction:

SO2 dOH M ! HSO3 M

then HSO3 creates ammonium sulfate in the following

steps:

HSO3 O2 ! SO3 HO2;

SO3 H2O ! H2SO4;

H2SO4 2NH3 ! NH42SO4:

The thermal reaction is based on the following process:

SO2 2NH3 ! NH32SO2;

NH32SO2 !O2;H2O

NH42SO4.

The total yield of SO2 removal consists of the yield of

thermal and radio-thermal reactions that can be written

(Chmielewski, 1995;Ma tzing et al., 1993):

ZSO2 Z1f; T Z2D; aNH3 ; T.

The yield of the thermal reaction depends on the

temperature and humidity and decreases with the temperature

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increase. The yield of the radio-thermal reaction depends

on the dose, temperature and ammonia stoichiometry. The

main parameter in NOx

removal is the dose. The rest of

parameters play minor role in the process. Nevertheless in

real, industrial process, dose distribution and gas flow

conditions are important from the technological point of

view (Chmielewski et al., 1998). The similar chemistryof the process is observed in corona discharge process

(Shang et al., 2006), however energy consumption and

more complicated reactor design seems to be limitations of

the process.

3. Pilot plants

Japanese scientists demonstrated in 19701971 the

removal of SO2 using an electron beam from a linear

accelerator (212 MeV, 1.2 kW). A dose of 50kGy at

100 1C led the conversion of SO2 to an aerosol of sulfuric

acid droplets, which were easily removed (Machi, 1983).

Ebara Co. used an electron accelerator (0.75 MeV,

45kW) to convert SO2 and NOx into a dry product

containing (NH4)2SO4 and NH4NO3 which could be used

as a fertilizer.

Using the Ebara process, two larger scale plants were

constructed in Indianapolis, USA (Frank, 1995) and

Karlsruhe, Germany (Wittig et al., 1988). The Indianapolis

plant was equipped with two electron beam accelerators

(0.8MeV, 160kW) and had a capacity of 1.63.2

10,000 m3/h with gas containing 1000ppm SO2 and

400 ppm NOx

. In Badenwerk, Karlsruhe, two electron

accelerators (0.3 MeV, total power 180 kW) were used to

treat 1210,000 m3

/h flue gas containing 50500 pm SO2and 300500 ppm NO

x. The first pilot system in China,

using the same principle to remove SO2 and NOx in flue

gas, was built at the Thermal Power Plant of Science City

in Mianyang, Sichuan. Its designed flow volume is

300012,000 Nm3/h, SO2 removal rate is not o90% and

NOx

, not o70% (Mao et al., 2000;Yonghua et al., 2002).

However the final engineering design technology for

industrial applications was achieved at the pilot plants

being operated in Nagoya, Japan (Namba et al., 1995) and

Kaweczyn, Poland (Chmielewski et al., 1995). In the case

of the latter a new engineering solutions were applied;

doublelongitudinal gas irradiation, air curtain separating

secondary window from corrosive flue gases and modifica-

tions of humidification/ammonia system (high enthalpy

water or steam injection, ammonia water injection) and

others. The obtained results have confirmed the earlier

discussed physico-chemistry of the process. The high dose

is required for NOx

removal, while SOx

is removed at

proper conditions, at low-energy consumption.

The new solutions are tested for low-grade fuels like

lignite. The pilot plant for treatment of flue gases from low-

grade lignite (high ash, high sulfur and high water content

has been constructed in Bulgaria (Doutzkinov, 2005). The

flow capacity is 10,000 Nm3/h and the accelerator from

Nagoya pilot plant was used.

4. Industrial plants

These new solutions led to the economical and technical

feasibility improvement and final industrial-scale plant

construction.

Ebara Corporation constructed full-scale plant in

Chengdu, China mostly for SOx removal, therefore thepower of accelerators applied is 320 kW for treatment of

270,000 Nm3/h of the flue gas. Reported efficiency is 80%

for SOx

and 20% for NOx

(Doi et al., 2000).

The flue gas treatment industrial installation is located in

EPS Pomorzany in Szczecin in the north of Poland

(Chmielewski et al., 2004). The installation purifies flue

gases from two Benson boilers of 65 MWe and 100MWtheach. The maximum flow rate of the gases is 270,000 Nm3/h

and the total beam power exceeds 1 MW. A flue gas

treatment plant was installed in EPS Pomorzany in

Szczecin, Poland. There are two reaction chambers with

nominal flow gas rate of 135,000 Nm3/h. Each chamber is

irradiated by two accelerators (260 kW, 700 keV) installed

in series. The applied dose is in the range of 712 kGy.

The removal of SO2 approaches 8090% in this dose

range, and that of NOx

is 5060%. The by-product is

collected by the electrostatic precipitator and is shipped to

the fertilizer plant.

The installation consists of four main parts:

flue gas conditioning unit; ammonia storage and dosage unit; reaction chambers; and by-product collecting and storage unit.

As it was previously mentioned the removal efficiency

depends strongly on the process conditions. The highest

obtained efficiency for SO2 reaches 95%, while for NOx it

reaches 70%. The data obtained during the operation of

the installation confirmed the previously considered

assumption on the impact of the process parameters on

the removal effectiveness. In the case of NOx

removal the

most important parameter is the dose. The inlet concen-

tration of NOx

is the second parameter, that impact on this

pollutant removal was observed. The correlation is linear

and total removal (taken in mg/Nm3) increases with the

inlet concentration of NOx

, while the relative removal

(in %) decreases with the parameter increase. The

ammonia stoichiometry factor has a very little impact on

the NOx

removal.

In the case of SO2 removal there are more parameters

that affect this pollutant removal efficiency. The most

important among them is temperature of the gas after

humidification due to the thermal reactions contribution.

Afterwards the dose should be mentioned. Although the

humidity seems to have the major impact on the process

efficiency, it is hard to prove it with no doubt because

of the strong correlation between the humidity and

the temperature of the process (dew point temperature is

a factor of both parameters; humidity and temperature).

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The temperature decreases during the water evaporation

process and humidity increases. Unexpectedly high influ-

ence of ammonia stoichiometry ratio on the SO2 removal

efficiency has been observed. The other factors as flue gas

flow rate and inlet concentration have much less impact on

the removal efficiency. During the experiments one more

parameter having impact on the whole process has beendetected: the ammonia injection mode. It was observed,

that the injection of part of ammonia water directly to

humidification tower increases the SO2 removal efficiency.

The new industrial plant is under construction in China

in Beijing, Jingfeng Power Plant, the flow capacity will be

equal to 630,000 Nm3/h. Three accelerators will be

installed; 2 1000kV/500 mA and 1 1000 kV/300 mA.

The plant will be operational in 2007 (Mao, 2005).

The critical point in the technology are accelerators. These

machines should be operated continuously 8500h per year

and the period between maintenance services should be at

least 3000 h. The cable connections between high power

supply and accelerator should be avoided and good cooling

systems for the cathode and primary window provided. The

improved foil materials have to be applied. The results of the

work done by some centers demonstrated that such

improvements in the titanium foil can be achieved by Pd

surface alloying (Bonilla et al., 2006, 2006a).

5. New prospects of technologyradiation-induced VOC

removal from off gases

In the case of VOCs decomposition the process itself is

based on the similar principles as primary reactions

concerning SO2 and NOx removal i.e. free radicals attackon organic compounds chains or rings causing VOCs

decomposition (Chmielewski et al., 2002).

For chlorinated aliphatic hydrocarbons decomposition (e.g.

chloroethylene), Cl dissociated secondary electron-attachment

and Cl, OH radicals reaction with VOCs play very important

roles for VOCs decomposition (Sun et al., 2006).

For aromatic hydrocarbons, VOCs decomposition will

mainly go through:

1. Positive ions charge transfer reactions

M RH RH VOC; e:g: Benzene or PAHs

M RH:

Because RH has lower ionization energy (IE)

(Benzene: IE 9.24 eV; PAHs: IEo10 eV) than most

primary positive ions (IE411 eV) formed above, part of

VOC will be decomposed by rapid charge transfer

reactions.

2. Radicalneutral particles reactionsdOH radical plays very important role for VOC

decomposition, especially when water concentration is

10%. dOH radicals react with VOC in two ways:dOH radical addition to the aromatic ring (e.g. toluene)

d

OH C6H5CH3 R1d

and H atom abstraction (for the alkyl-substituted

aromatic compounds) or H atom elimination (for

benzene, naphthalene and the higher polycyclic aro-

matic hydrocarbons).

C6H5CH3+dOH R2

d+H2O (H atom abstraction),

C6H6+dOH C6H5OH+H (H atom elimination).

Radicals (R1d, R2

d) formed above go though very complex

reactions: O2 addition, O atom release, aromatic CHO

(-dehydes), OH (-ol) compounds formed or ring cleavage

products:

Rd R1d

; R2d O2 RO2

d;

2RO2d 2ROd O2;

RO2d NO ROd NO2;

ROd O2 HO2d products aromatic 2CHO; 2O;

ROd ! aliphatic products:

The possibility of the process application for the dioxins

removal form flue gases has been studied (Hirota et al.,

1995; Paur et al., 1998) and recent pilot studies demon-

strated that process is technically and economically feasible

(Hirota et al., 2003).

6. Conclusions

1. Electron beam flue gas treatment technology has been

applied in the full industrial scale.

2. The advantages of the technology i.e. high SO2and NOxremoval efficiencies were achieved.

3. No wastewater or solid wastes are generated and

byproduct is a high-grade fertilizer component.

4. The laboratory and pilot scale test have demonstrated

that the process can be applied for VOC removal as well.

Therefore three pollutants can be treated simulta-

neously. There is no other technology with such

capabilities.

5. The critical point in the technology implementation is

reliability of accelerators in continuous machine opera-

tion. The longer periods between servicing and good

corrosion/mechanical-stress resistance of the primaryand secondary window foils should be a target for future

developments. The results of the tests performed in the

industrial harsh conditions should be analyzed and

adopted by accelerator manufacturers, in both phases of

machine design and its manufacturing.

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