Abstract

Designing a highly efficient fuel electrode for CO2/H2O co-electrolysis with controllable CO/H2 ratios is fundamentally challenging due to the significant influence of water-gas shift (WGS) reaction. Perovskite oxide La0.6Sr0.4Fe0.8Mn0.2O3 (LSFM) has been identified as a promising alternative to conventional Ni-based cermet electrodes, offering inherent redox stability. In this study, LSFM exhibits efficient electrocatalytic activity and remarkable syngas control, with ratios directly controlled by adjusting the CO2/H2O feed. In-situ/ex-situ catalytic analyses reveal LSFM’s efficacy in controlling syngas, attributed to substantial CO2 adsorption on its surface. The carbonated surface interacting with H2O leads to the formation of bicarbonate species, acting potential active intermediates that facilitate CO2 electroreduction to CO while suppressing the WGS reaction. Stable syngas control is confirmed by long-term reversible operations at various applied currents with nearly 100 % Faradaic efficiency. This study highlights the great potential of LSFM perovskite for efficient and steady syngas production in co-electrolysis, providing insights into advanced fuel electrode design.

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