Selective CO2Electroreduction to Ethanol over a Carbon‐Coated CuOxCatalyst

Abstract The design of efficient copper(Cu)‐based catalysts is critical for CO2electroreduction 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 CO2electroreduction 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 CO2electroreduction 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.