Abstract

Electrocatalytic reduction of carbon dioxide (CO2) with high selectivity to generate value-added chemical products and fuels, utilizing renewable electricity sources, offers an effective approach to address the continued increase in atmospheric CO2. Here, we report cerium (Ce)-doped indium oxide (In2O3) electrocatalyst generated in situ on carbon paper (Ce-In2O3/CP), and its application in the electrochemical reduction of CO2 (CO2RR) to formate formation with high Faradaic efficiency (FE) (reaching 97.6% at −1.7 V vs. Ag/AgCl) and excellent stability. Experimental analysis and density functional theory (DFT) calculations indicate that doping Ce onto the (222) plane of In2O3 induces lattice distortion, which promotes electron transfer from Ce to In while adjusting the local electronic structure of the In atoms around Ce, making them more favorable for the adsorption of *OOCH intermediates and effectively lowering the energy barrier of the rate-determining step. Furthermore, Ce doping lowers the overpotential required for formate production and suppresses the hydrogen evolution reaction (HER), effectively enhancing the selectivity of formate.

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