文献类型：期刊文献

英文题名：Cu Single-Atom Catalysts for High-Selectivity Electrocatalytic Acetylene Semihydrogenation

作者：Jiang, Xiaoli[1];Tang, Lei[1];Dong, Lei[1];Sheng, Xuedi[1];Zhang, Wenfei[1];Liu, Zhen[1];Shen, Jianhua[2];Jiang, Hongliang[1];Li, Chunzhong[1]

机构：[1]East China Univ Sci & Technol, Minist Educ, Sch Chem Engn, Key Lab Ultrafine Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Minist Educ,Key Lab Ultrafine Mat, Shanghai 200237, Peoples R China

年份：2023

卷号：62

期号：33

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20232814367155);WOS:【SCI-EXPANDED(收录号:WOS:001029002400001)】；

基金：Acknowledgments This work was supported by the National Natural Science Foundation of China (22222804 and U22B20143), the National Key R&D program (2022YFB3808400), the Science and Technology Commission of Shanghai Municipality (22dz1205900), and the Shanghai Municipal Science and Technology Major Project. The authors thank the Shanghai Synchrotron Radiation Facility (14W1, SSRF).

语种：英文

外文关键词：Acetylene Semihydrogenation; C-C Coupling; Overhydrogenation; Selectivity; Single Atom

摘要：The site isolation strategy has been employed in thermal catalytic acetylene semihydrogenation to inhibit overhydrogenation and C-C coupling. However, there is a dearth of analogous investigations in electrocatalytic systems. In this work, density functional theory (DFT) simulations demonstrate that isolated Cu metal sites have higher energy barriers on overhydrogenation and C-C coupling. Following this result, we develop Cu single-atom catalysts highly dispersed on nitrogen-doped carbon matrix, which exhibit high ethylene selectivity (>80 % Faradaic efficiency for ethylene, <1 % Faradaic efficiency for C-4, and no ethane) at high concentrations of acetylene. The superior performance observed in the electrocatalytic selective hydrogenation of acetylene can be attributed to the weak adsorption of ethylene intermediates and highly energy barriers on C-C coupling at isolated sites, as confirmed by both DFT calculations and experimental results. This study provides a comprehensive understanding of the isolated sites inhibiting the side reactions of electrocatalytic acetylene semihydrogenation.