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Micro-patterned metal/ceramic model thin film electrodes were used to investigate the hydrogen oxidation mechanism on various metal/ion conductor combinations such as Ni/yttria-stabilized zirconia (YSZ), Pt/YSZ, Ni/scandia-stabilized zirconia, Ni/titania/YSZ. For all electrode types besides those with a continuous titania interlayer a triple phase boundary (TPB) and an area pathway could be separated. Moreover, activation energies as well as hydrogen and water reaction orders were determined for both pathways and compared with previously published data on Ni/YSZ. It was found that when varying the electronically conducting phases on YSZ the activation energy of the TPB path remains virtually the same. However, changing the ion conductor significantly influenced the activation energy, indicating a rate-limiting step on the electrolyte. However, the stark difference in water reaction order of Ni/YSZ and Pt/YSZ electrodes shows that the metal phase is also actively participating in the reaction chain. It is suggested that the electrolyte surface is responsible for the rate-limiting electrochemical redox reaction while the metal interacts with the gas phase molecules and thus supplies the reactants. For samples with a thin mixed conducting titania layer on YSZ, the electrochemical behavior drastically changed, which can be explained by an extension of the reaction zone away from the TPB.

Comparison of electrochemical hydrogen oxidation on different metal/ceramic model anodes and mechanistic implications