Zang Yipeng, Liu Tianfu, Wei Pengfei, Li Hefei, Wang Qi, Wang Guoxiong, Bao Xinhe
State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, China.
Angew Chem Int Ed Engl. 2022 Oct 4;61(40):e202209629. doi: 10.1002/anie.202209629. Epub 2022 Aug 23.
The design of efficient copper(Cu)-based catalysts is critical for CO 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 CuO (CuO @C) catalyst through one-pot pyrolysis of Cu-based metal-organic framework (MOF), which exhibits high selectivity for CO electroreduction to ethanol with Faradaic efficiency of 46 %. Impressively, the partial current density of ethanol reaches 166 mA cm , which is higher than that of most reported catalysts. Operando Raman spectra indicate that the carbon coating can efficiently stabilize Cu species under CO 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.
设计高效的铜(Cu)基催化剂对于将CO电还原为多种碳产物至关重要。然而,大多数Cu基催化剂有利于乙烯的生成,而以高法拉第效率和电流密度选择性生产乙醇仍然是一个巨大的挑战。在此,我们通过对铜基金属有机框架(MOF)进行一锅热解来设计一种碳包覆的CuO(CuO@C)催化剂,该催化剂对CO电还原为乙醇表现出高选择性,法拉第效率为46%。令人印象深刻的是,乙醇的分电流密度达到166 mA cm ,高于大多数已报道的催化剂。原位拉曼光谱表明,碳涂层可以在CO电还原条件下有效地稳定Cu物种,从而促进C-C偶联步骤。密度泛函理论(DFT)计算表明,碳层可以调节关键中间体*HOCCH沿着加氢途径生成乙醇。