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The design of efficient copper(Cu)‐based catalysts is critical for CO2 electroreduction into multiple carbon products. However, most Cu‐based catalysts are favorable for ethylene production while selective production of ethanol with high Faradaic efficiency and current density still remains a great challenge. Herein, we design a carbon‐coated CuOx (CuOx@C) catalyst through one‐pot pyrolysis of Cu‐based metal‐organic framework (MOF), which exhibits high selectivity for CO2 electroreduction to ethanol with Faradaic efficiency of 46 %. Impressively, the partial current density of ethanol reaches 166 mA cm−2, which is higher than that of most reported catalysts. Operando Raman spectra indicate that the carbon coating can efficiently stabilize Cu+ species under CO2 electroreduction conditions, which promotes the C−C coupling step. Density functional theory (DFT) calculations reveal that the carbon layer can tune the key intermediate *HOCCH goes the hydrogenation pathway toward ethanol production. [ABSTRACT FROM AUTHOR]

The electrochemical CO2 reduction reaction (CO2RR) over Cu‐based catalysts shows great potential for converting CO2 into multicarbon (C2+) fuels and chemicals. Herein, we introduce an A2M2O7 structure into a Cu‐based catalyst through a solid‐state reaction synthesis method. The Cu2P2O7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO2RR conditions. The reconstructed Cu2P2O7 catalyst achieves a Faradaic efficiency of 73.6 % for C2+ products at an applied current density of 350 mA cm−2, remarkably higher than the CuO counterparts. The reconstructed Cu2P2O7 catalyst has a high electrochemically active surface area, abundant defects, and low‐coordinated sites. In situ Raman spectroscopy and density functional theory calculations reveal that CO adsorption with bridge and atop configurations is largely improved on Cu with defects and low‐coordinated sites, which decreased the energy barrier of the C−C coupling reaction for C2+ products. [ABSTRACT FROM AUTHOR]