Abstract
LnFeO3-δ (Ln = La, Pr and Gd) as cathodes for CO2 electroreduction are investigated in solid oxide electrolysis cells at 800 °C. Their surface properties, oxygen desorption behaviour, CO2 adsorption capacity, structure stability under working conditions, activation mechanism and CO2 electroreduction kinetics processes are studied by various characterization methods, such as O2 or CO2 temperature programmed desorption, in situ X-ray diffraction, near ambient pressure X-ray photoelectron spectroscopy, quasi situ infrared spectroscopy and distribution of relaxation time analysis. Similar CO2 electrochemical performances are measured for these Fe-based perovskite cathodes due to their similar physicochemical properties. Although their perovskite structure is stable, cathode surfaces are reconstructed under electroreduction conditions. The produced oxygen vacancies and Fe nanoparticles under the CO2 electroreduction conditions enhance the ability of CO2 adsorption and conversion. Carbonate species are considered as the transition species for CO2 electroreduction based on these characterizations. At last, a mechanism of CO2 electroreduction on these Fe-based perovskite cathodes is proposed.
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