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Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
J.M. Alarcón*, J.R. Fernández, J.C. Abanadesj.alarcon@incar.csic.es
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a
fuel gas in a fixed-bed reactor
6th IEAGHG High Temperature Solid Looping Cycles Network Meeting, September 1-2, 2015, Milan
INSTITUTO NACIONAL DEL CARBÓN (INCAR-CSIC)
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Introduction 1
2
3
4
5
6
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Outline
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions7
Conclusions
Reduction/calcination tests
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
The Ca/Cu Looping Process(Abanades & Murillo, CSIC, EP09382169.2, 16th Sep 2009)
(Abanades et al., Env. Sci. Tech., 44, 6901-6904, 2010)
Endothermic/exothermic reactionscoupled in the same bed matrix
efficiency
Equipment cost
Based on the “unmixed reformingconcept” (Kumar et al., 2000)
Chemical Looping+
Chemical Looping Combustion
CaO for CO2 capture in thereformer (higher H2 yield)
Steam reforming + CaO carbonation
Cu oxidation
CuO reduction+ CaCO3 calcination
CO2 rich product gas suitablefor transport and storage
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
FEED GASES
PREHEATING
GASES
FIXED-BED
REACTOR
IR & TC
ANALYZERS
Experimental set up
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Material: Inconel
Internal diameter: 0.038 m
External diameter: 0.042 m
Height: 1 m
Solids mass: around 1 kg
Multipoint type K thermocouple (15
points)
Insulating material: quartz wool
FIXED-BED REACTOR
Experimental set up
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Material: Inconel
Internal diameter: 0.038 m
External diameter: 0.042 m
Height: 1 m
Solids mass: around 1 kg
Multipoint type K thermocouple (15
points)
Insulating material: quartz wool
FIXED-BED REACTOR
Experimental set up
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Material: Inconel
Internal diameter: 0.038 m
External diameter: 0.042 m
Height: 1 m
Solids mass: around 1 kg
Multipoint type K thermocouple (15
points)
Insulating material: quartz wool
FIXED-BED REACTOR
Experimental set up
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Pseudo-homogeneous model
Mass and thermal dispersion in axial direction
Ideal gas behaviour
Negligible intraparticle mass and temperature gradients
Constant bed void fraction
Uniform particle size
Perfect mixing of the solids
Negligible carbon deposition
ASSUMPTIONS
Model description
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Mass balance
Energy balance
/ ;
Kinetics of CuO reduction
Kinetics of CaCO3 calcination
/
Axial pressure distribution
(García Labiano et al., 2004)
(Martínez et al., 2012)
Model description
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
PARAMETERS VALUES
Feed gas temperature, Tgin 475 ºC
Initial solids temperature, Ts0 26 ºC
Pressure, P 1 atm
Inlet flow velocity 40 LN/min
Particle size, dp 0.003 m
Reactor length, L 0,92 m
Reactor diameter, D 0,038 m
Bed porosity, ε 0.5
Bed density, ρs 1920 kg/m3
Operating conditions
U= 5 W/m2K
HEATING OF THE PACKED BED
Heat transfer tests
Axial temperature profiles
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
PARAMETERS VALUES
Feed gas temperature, Tgin 475 ºC
Initial solids temperature, Ts0 26 ºC
Pressure, P 1 atm
Inlet flow velocity 40 LN/min
Particle size, dp 0.003 m
Reactor length, L 0,92 m
Reactor diameter, D 0,038 m
Bed porosity, ε 0.5
Bed density, ρs 1920 kg/m3
Operating conditions
U= 5 W/m2K
HEATING OF THE PACKED BED
Heat transfer tests
Outlet gas temperatures
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Operating conditions
PARAMETERS VALUES
Feed gas temperature, Tgin 400 ºC
Initial solids temperature, Ts0 600 ºC
Pressure, P 1 atm
Inlet flow velocity 15 LN/min
Particle size, dp 0.003 m
Reactor length, L 0,92 m
Reactor diameter, D 0,038 m
Bed porosity, ε 0.5
CuO density, ρCuO 380 kg/m3
Bed density, ρs 1840 kg/m3
Reduction tests
CO2 H2 as fuel gas
CO2
CuO-based particles: 60% active
Ca-based particles: 12% active
CaO as inert material underthese conditions
CO2 20% of CuO
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Reduction tests
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Breakthrough between 6 and 9 minutes
Validation of the model
R
High reactivity of H2 with CuO
HR
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Operating conditions
PARAMETERS VALUES
Feed gas temperature, Tgin 400 ºC
Initial solids temperature, Ts0 680 ºC
Pressure, P 1 atm
Inlet flow velocity 15 LN/min
Particle size, dp 0.002 m
Reactor length, L 0,92 m
Reactor diameter, D 0,038 m
Bed porosity, ε 0.5
CuO density, ρCuO 380 kg/m3
CaCO3 density, ρCuO 249 kg/m3
Bed density, ρs 1840 kg/m3
CO2H2 as fuel gas
CO2
CuO-based particles: 60% active
Ca-based particles: 12% active
Cu/Ca molar ratio=1,8
CO2
Temperature of solids bedvarying from 415 ºC (bottom) to 720 ºC (top)
Effect of starting temperature on reduction/calcinationoperation
Reduction/calcination tests
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
RHC
C
High reactivity of H2 with CuO even at low temperatures (400ºC)
Calcination of CaCO3 is negligible below 800 ºC
At 870ºC (t>5min) calcination is highly favoured
flow gas rate by calcination: heat exchange front advances faster
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
t=2 mint=5 min t=7 min
CaCO3 conversiont<2 min, Rapid and total reduction of the CuO
t<5 min, T=870ºC Reduction and calcination fronts advance together
Leaving behind the second part of the reactor totally converted.
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Conclusions
CO2
Experimentally demonstrated that the reduction of CuO with a fuelgas can supply the energy required to carry out the calcination ofCaCO3 in a same fixed-bed reactor.
The dynamic model gives a good description under the operatingconditions considered.
CO2
CO2
A balanced Cu/Ca molar ratio in the bed makes both reduction andcalcination fronts advance together with moderate maximumtemperatures (870 ºC), leaving behind solids totally converted.
CO2
CO2
Temperatures lower than 800 ºC allow a rapid reduction of CuO withH2, but not the calcination and part of the bed can be left uncalcined.
Future work: study of the key design parameters: Cu/Ca molar ratio,temperature and composition of the fuel gas, alternative fuel gases(CH4, CO) and other materials for the Ca/Cu looping process, and thestudy of the oxidation step with different N2 dilutions.
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a
fuel gas in a fixed-bed reactor
6th IEAGHG High Temperature Solid Looping Cycles Network Meeting, september 1-2, 2015, Milan
INSTITUTO NACIONAL DEL CARBÓN (INCAR-CSIC)
Thank you for your attention!
Investigation of the calcination of CaCO3 by the simultaneous reduction of CuO with a fuel gas in a fixed-bed reactor
J.M. Alarcón, J. R. Fernández , J. C. Abanades
Axial mass dispersion coefficient
Effective axial heat dispersion
Gas-to-particle heat transfer coefficient
(Edwards and Richardson, 1968)
(Vortmeyer and Berninger, 1982)
(Krupiczka, 1967)
(Gunn and Misbah, 1993)
(Gunn, 1987)
Model description
Introduction
Experimental set up
Model description
Heat transfer tests
Reduction tests
Reduction/Calcination
tests
Conclusions
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