MATERIALS THERMODYNAMICS KINETICS SUMMARY INTRODUCTION
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2 Introduction H 2 production & chemical looping Materials iron oxide & iron containing perovskite Thermodynamics equilibrium models & reaction front velocities Kinetics concept, results & link to thermodynamics Summary
3 ammonia production fuel cells H 2 vehicle fuel hydrogenation of oils energy vector fuel cells ammonia vehicle production fuel rocket fuel H 2 hydrogenation of oils Natural Gas Reforming Renewable Electrolysis Nuclear Electrolysis energy vector Thermo-Chemical Electrolysis rocket fuel Gasification
4 850 o C CO Oxidised OCM H 2 CO 2 Reduced OCM H 2 O OCM = Oxygen Carrier Material
5 IRON OXIDE Fe 2 O 3 Fe 3 O 4 FeO Fe Cheap Large oxygen capacity Unstable over 40+ cycles Thermal sintering? Phase changes? A. Murugan, A. Thursfield and I. S. Metcalfe, Energy Environ. Sci., 2011, 4, 4639 Different support materials? Substitute for completely different material? MATERIALS THERMODYNAMICS KINETICS SUMMARY
6 PEROVSKITE La0.7 Sr0.3 Fe O3-δ Expensive Lower oxygen capacity Stable operation Regeneration No phase changes LaFeO3 A site B site O site La Fe O A. Murugan, A. Thursfield and I. S. Metcalfe, Energy Environ. Sci., 2011, 4, 4639 MATERIALS THERMODYNAMICS KINETICS SUMMARY
7 PEROVSKITE La0.7 Sr0.3 Fe O3-δ Expensive Lower oxygen capacity Stable operation Regeneration La0.7Sr0.3FeO3-δ (LSF731) No phase changes A site A. Murugan, A. Thursfield and I. S. Metcalfe, Energy Environ. Sci., 2011, 4, 4639 MATERIALS La/Sr THERMODYNAMICS B site O site Fe O KINETICS O vacancy δ SUMMARY
8 CO CO 2 Fe 3 O 4 Fe/FeO H 2 H 2 O Fe 2 O 3 Fe 3 O 4 FeO Fe Thermodynamics well known for iron oxide Bauer Glaessner Diagram M.F. Bleeker, S.R.A. Kersten and H.J. Veringa, Catal. Today, 2007, 127, 278
9 Non-stoichiometry po 2 90% CO/10% CO 2 model LSF731 x = % CO/50% CO 2 10% CO/90% CO 2 Adaptable model CO/CO 2 ratio δ 9: : : x x po 2 (atm) K Fe x 2 po2 K 1 1 OX KOX xpo2
10 IRON OXIDE Step-wise reaction fronts Assuming infinitely fast kinetics Need to visualise bed as infinite elements Gas Flow (u gas ) Fe 2 O 3 Fe 3 O 4 FeO Fe P. Heidebrecht, K. Sundmacher, Chem. Eng. Sci., 2009, 64, 5057
11 LSF731 front 1 Multiple fronts can move at u 1 u gas solid gas d dy any time u front (m/s) Each δ has a velocity u front H 2 /H 2 O u front CO/CO 2 δ change in order: propagation limited by u gas = 0.1 m/s ph 2 O/pH 2 pco/pco 2
12 LSF731 OXIDATION 1 st cycle H 2 /H 2 O Inlet (u gas ) DELTA
13 LSF731 REDUCTION 2 nd cycle etc. CO/CO Inlet (u gas ) DELTA
14 CO 2 CO 2 CO 2 CO 2 CO 2 CO CO CO CO CO CO CO:CO 2 1:0 CO:CO 2 3:1 CO:CO 2 1:1 CO:CO 2 1:3 CO:CO 2 0:1 Fe FeO Fe 3 O 4 Fe 2 O 3 MATERIALS THERMODYNAMICS KINETICS SUMMARY
15 Molar Flow for Production of CO 2 (mol/s) CO/(CO+CO 2 ) (%) Time (minutes) % Fe 2 O 3 /40% Al 2 O o C 100% CO 1 10% CO 2 50% CO 2 90% CO 2 100% CO 2 10 CO 2 feed Reduction extent 0% 56% FeO Fe 10% 44% FeO Fe 50% 47% Fe 3 O 4 FeO 90% 2% Fe 3 O 4 FeO 100% 10% Fe 2 O 3 Fe 3 O Fe Fe 3 O 4 FeO T ( o C) 1000 MATERIALS THERMODYNAMICS KINETICS SUMMARY
16 Hydrogen is essential : now and in the future Perovskites could be a potential replacement to Fe 2 O 3 Equilibrium model was made for LSF731 packed bed Bed behaviour was studied : infinitely fast kinetics Preliminary kinetic studies & thermodynamic predictions agree
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