Adjacent Copper Single Atoms Promote C-C Coupling in Electrochemical CO2 Reduction for the Efficient Conversion of Ethanol

作者：Xia, Wei; Xie, Yijun; Jia, Shuaiqiang; Han, Shitao; Qi, Ruijuan; Chen, Tao; Xing, Xueqing; Yao, Ting; Zhou, Dawei; Dong, Xue; Zhai, Jianxin; Li, Jingjing; He, Jianping; Jiang, Dong; Yamauchi, Yusuke; He, Mingyuan; Wu, Haihong^*; Han, Buxing^*

来源：Journal of the American Chemical Society, 2023, 145(31): 17253-17264.

DOI：10.1021/jacs.3c04612

• ELECTROREDUCTION
• CATALYSTS
• ELECTROCATALYSIS
• PRODUCTS
• ETHYLENE
• SITES

The electrochemical CO2 reduction reaction(CO2RR) using renewable electricity is one of the mostpromising strategiesfor reaching the goal of carbon neutrality. Multicarbonous (C2+) products have broad applications, and ethanol is a valuablechemical and fuel. Many Cu-based catalysts have been reported to beefficient for the electrocatalytic CO2RR to C2+ products, but they generally offer limited selectivity and currentdensity toward ethanol. Herein, we proposed a silica-mediated hydrogen-bondedorganic framework (HOF)-templated approach to preparing ultrahigh-densityCu single-atom catalysts (SACs) on thin-walled N-doped carbon nanotubes(TWN). The content of Cu in the catalysts prepared by this methodcould be up to 13.35 wt %. It was found that the catalysts showedoutstanding performance for the electrochemical CO2RR toethanol, and the Faradaic efficiency (FE) of ethanol increased withthe increase in Cu-N-3 site density. The FE of ethanolover the catalysts with 13.35 wt % Cu could reach & SIM;81.9% witha partial current density of 35.6 mA cm(-2) usingan H-type cell, which is the best result for electrochemical CO2RR to ethanol to date. In addition, the catalyst could bestably used for more than 25 h. Experimental and density functionaltheory (DFT) studies revealed that the adjacent Cu-N-3 active sites (one Cu atom coordinates with three N) were the activesites for the reaction, and their high density was crucial for thehigh FE of ethanol because the adjacent Cu-N-3 siteswith a short distance could promote the C-C coupling synergistically.

• 单位
  南京航空航天大学; 中国科学院