Two Stage-CLC: a novel reactor configuration for packed bed CLC with syngas
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1 Two Stage-CLC: a novel reactor configuration for packed bed CLC with syngas Paul Hamers, Fausto Gallucci, Erin Kimball, Paul Cobden, Martin van Sint Annaland Chemical Process Intensification Multiphase Reactors Department of Chemical Engineering and Chemistry TU/e, The Netherlands September 2, 2013
2 Process scope Goal: Air at T=1200 C p=20 bar / Chemical Engineering & Chemistry PAGE 1
3 Reactor configurations Main goal: combined cycle to reach high efficiency T ex = 1200 C, p = 20 bar Fluidized beds Packed beds Pro Continuous process No solid/gas separation necessary High pressures could be more easily applied Con Gas/solids separation at desired operating conditions High temperature valve is required / Chemical Engineering & Chemistry PAGE 2
4 Packed bed CLC process N 2 /O 2 Temperature [K] Axial position [m] Temperature at x=l [K] Oxidation cycle Time [s] Air Heated gasses are fed to a gas turbine / Chemical Engineering & Chemistry PAGE 3
5 Oxygen carrier selection Air obtained at 450 C after adiabatic compression from atmospheric conditions Temperature rise of 750 C has to be achieved with CLC Possible oxygen carriers: Lowest melting point ( C) Selectivity γ CO at 800 C Selectivity γ H2 at 800 C Active weight material required for 750 C T rise Costs [ /ton] NiO/Ni % >20,000 CuO/Cu % >3000 Fe 2 O 3 /Fe 3 O >100% >1000 Fe 3 O 4 /FeO *** >1000 Mn 3 O 4 /MnO % >1000 / Chemical Engineering & Chemistry PAGE 4
6 Alternative: Two stage CLC Smaller temperature changes in one reactor Lower active weight content and T melting no issue Different combinations of oxygen carriers are possible More information: Int. J. Greenhouse Gas Control, 16 (2013), pp / Chemical Engineering & Chemistry PAGE 5
7 Two-stage CLC: principle heat removal heat removal T g,out Main criteria for oxygen carrier selection: Temperature ( C) T g,in heat removal 2. oxidation 1. reduction 1 st oxygen carrier 2. oxidation 1. reduction 2 nd oxygen carrier 1 st carrier: High reactivity at T low copper 2 nd carrier Stable at T high manganese axial position (m) / Chemical Engineering & Chemistry PAGE 6
8 Theoretical demonstration TS-CLC demonstrated theoretically by 1D packed bed reactor model Two reactors considered as 1 reactor Simulation parameters Length bed 1 3 meter Criteria for operating parameters: - Pressure drop <5% - Prevent fuel slip - Similar cycle time for oxidation/heat removal and reduction Oxygen carrier bed wt% CuO/Al 2 O 3 Length bed 2 3 meter Oxygen carrier bed 2 30wt% Mn 3 O 4 /Al 2 O 3 Feed oxidation/heat removal Air, 4 kg/(m 2 s) at 450 C, 20 bar Feed reduction Syngas, CO/H 2 =1, 0.15 kg/(m 2 s) at 450 C, 20 bar / Chemical Engineering & Chemistry PAGE 7
9 TS-CLC: axial profiles reduction CuO/Al 2 O 3 Mn 3 O 4 /Al 2 O CuO/Al 2 O 3 Mn 3 O 4 /Al 2 O Temperature [ C] w act in oxidized form axial position [m] axial position [m] red, initial red, tau=1/3 red, tau=2/3 red, end purge, end / Chemical Engineering & Chemistry PAGE 8
10 TS-CLC: Axial profiles oxidation and heat removal Temperature [ C] CuO/Al 2 O 3 Mn 3 O 4 /Al 2 O CuO/Al 2 O 3 Mn 3 O 4 /Al 2 O 3 w,act in oxidized form [-] axial position [m] axial position [m] ox, initial ox, tau=1/3 ox, tau=2/3 HR HR, end purge, end / Chemical Engineering & Chemistry PAGE 9
11 TS-CLC demonstrated theoretically Gas temperature at outlet ( C) reduction oxidation/ heat removal TS-CLC possible: flow at high temperature and pressure is produced for the gas turbine time (s) PAGE 10
12 Comparison between TS-CLC and single stage Outlet temperature [ C] Reduction Oxidation/heat removal time [s] Two-stage CLC: Outlet temperature profiles more dispersed CO 2 and H 2 O are produced at higher temperature Temperature changes at the outlet are much less dramatic According to energy balance, flow send to the gas turbine expander is only 4% less NiO/Al2O3 CuO Mn3O4 / Chemical Engineering & Chemistry PAGE 11
13 Conclusions CLC is also possible in two stages More different oxygen carriers could be used for packed bed CLC Smaller temperature changes per reactor (max. ΔT=400 C) The temperature changes are much less dramatic at the outlet of the bed Effects on electrical efficiency: CO 2 and H 2 O produced at higher temperature Smaller air flow to gas turbine: HT HP feed produced for the GT cycle is only 4% less / Chemical Engineering & Chemistry PAGE 12
14 Outlook Demonstrate the TS-CLC configuration experimentally Compare the electrical efficiency with the conventional single stage PB-CLC (in collaboration with Politecnico di Milano) / Chemical Engineering & Chemistry PAGE 13
15 Acknowledgement This research project is carried out within the CATO2 program (Dutch National Program on CCS) Partners: / Chemical Engineering & Chemistry PAGE 14
16 Questions? / Chemical Engineering & Chemistry PAGE 15
17 Model description 1D adiabatic packed bed reactor, assumed: No radial temperature and concentration gradients Pseudo-homogeneous model No heat losses through the reactor wall Reactor products: only H 2 O and CO 2 No carbon deposition More information: Noorman et al, Packed Bed Technology for Chemical-Looping Combustion. Ind. Eng. Chem. Res. 2007, 46, / Chemical Engineering & Chemistry PAGE 16
18 Model description Component mass balance for gas phase ig, ig, ig, g g gv g gd ax grm i i t x x x Component mass balance for solid phase 0 s, j s s act grm j j t Energy balance T T T C C v C r H t x x x g g p, g s s p, s s g p, g eff g i R, i Reaction rate r k C C n 0 i eff g, i s, j More information: Noorman et al, Packed Bed Technology for Chemical-Looping Combustion. Ind. Eng. Chem. Res. 2007, 46, / Chemical Engineering & Chemistry PAGE 17
19 Theoretical demonstration TS-CLC demonstrated theoretically by 1D packed bed reactor model Criteria for operating parameters: - Pressure drop <5% - Prevent fuel slip - Similar cycle time for oxidation/heat removal and reduction 30wt% Mn 3 O 4 BED 1 BED 2 Oxygen carrier 12.5wt% CuO on Al 2 O 3 on Al 2 O 3 Particle diameter [mm] 3 3 Solids bulk density in oxidized state, ε s ρ s [kg/m 3 ] Gas porosity [m 3 gas/m 3 reactor] Reactor length [m] Oxidation/ Reduction Purge Heat removal Gas inlet flowrate [kg/(m 2 s)] Gas inlet [mol fraction] O 2 : 0.21 H 2 : 0.5 N 2 : 1 N 2 : 0.79 CO: 0.5 Gas inlet temperature [ C] Gas inlet pressure [bar] Reaction rate, r i [mol/(m 3 s)] 50c O2 25c H2-25c CO Cycle time [s] / Chemical Engineering & Chemistry PAGE 18
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