Abstract

Results of combined experimental and theoretical investigations of elementary chemical reaction processes of 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 and /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 via to Ni–O, the second step being accompanied by oxygen spillover over the three-phase boundary.

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