Elementary Reaction Kinetics of the CO ∕ CO2 ∕ Ni ∕ YSZ Electrode
2011
Results of combined experimental and theoretical investigations of elementary chemical reaction processes of COA¢Â�Â�CO2 gas
mixtures at nickel/yttria-stabilized zirconia (Ni/YSZ) solid oxide fuel cell (SOFC) model anode systems are presented. Temperature-programmed desorption and reaction measurements were performed in order to determine adsorption/desorption kinetic data as well as thermodynamic parameters for the CO/CO2/Ni and CO/CO2/yttria-stabilized zirconia (YSZ) heterogeneous reaction systems. From these data, an elementary kinetic reaction mechanism of the electrochemical CO oxidation at Ni/YSZ anodes was developed. Numerical simulations were performed for three different spillover mechanisms. Steady-state polarization curves and electrochemical impedance spectra were calculated, allowing for a direct comparison with experiments performed by
Lauvstad et al. [J. Electrochem. Soc., 149, E506 (2002)]. Best agreement with the experimental data was obtained when assuming two consecutive charge-transfer steps from YSZA¢Â�Â�O2A¢Â�Â� via YSZA¢Â�Â�OA¢Â�Â� to NiA¢Â�Â�O, the second step being accompanied by oxygen spillover over the three-phase boundary.
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