文献类型：期刊文献

英文题名：Highly Ethylene-Selective Electrocatalytic CO2 Reduction Enabled by Isolated Cu-S Motifs in Metal-Organic Framework Based Precatalysts

作者：Wen, Chun Fang[1];Zhou, Min[2];Liu, Peng Fei[1];Liu, Yuanwei[1];Wu, Xuefeng[1];Mao, Fangxin[1];Dai, Sheng[3,4];Xu, Beibei[5,6];Wang, Xue Lu[5,6];Jiang, Zheng[7];Hu, P.[2,8];Yang, Shuang[1];Wang, Hai Feng[2];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Sch Mat Sci & Engn, Minist Educ, Key Lab Ultrafine Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[4]East China Univ Sci & Technol, Sch Chem & Mol Engn, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]East China Normal Univ, Sch Phys & Mat Sci, Phys Dept, 3663 North Zhongshan Rd, Shanghai 200062, Peoples R China;[6]East China Normal Univ, Sch Phys & Mat Sci, Shanghai Key Lab Magnet Resonance, 3663 North Zhongshan Rd, Shanghai 200062, Peoples R China;[7]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[8]Queens Univ Belfast, Sch Chem & Chem Engn, Belfast BT9 SAG, Antrim, North Ireland

年份：2022

卷号：61

期号：2

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20214911273176);WOS:【SCI-EXPANDED(收录号:WOS:000740934200015)】；

基金：This work was financially supported by the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003), the National Natural Science Funds for Distinguished Young Scholars (51725201), the Innovation Program of Shanghai Municipal Education Commission (E00014), the National Natural Science Foundation of China (51902105, 21873028, 22072045), the Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400) and the Shanghai Sailing Program (19YF1411600). The authors acknowledge the support by Shanghai Rising-star and Shuguang Programs (20QA1402400, 17SG30). The authors acknowledge the Fundamental Research Funds for the Central Universities (JKD01211519, JKVJ1211022). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center. The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry. The authors also thank the crew of the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility (SSRF) and the 1W1B beamline of Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analyses.

语种：英文

外文关键词：CO2 reduction reaction; electrocatalysis; Cu-S species; metal-organic frameworks; operando XAFS

摘要：Copper-based materials are efficient electrocatalysts for the conversion of CO2 to C2+ products, and most these materials are reconstructed in situ to regenerate active species. It is a challenge to precisely design precatalysts to obtain active sites for the CO2 reduction reaction (CO2RR). Herein, we develop a strategy based on local sulfur doping of a Cu-based metal-organic framework precatalyst, in which the stable Cu-S motif is dispersed in the framework of HKUST-1 (S-HKUST1). The precatalyst exhibits a high ethylene selectivity in an H-type cell with a maximum faradaic efficiency (FE) of 60.0%, and delivers a current density of 400 mA cm(-2) with an ethylene FE up to 57.2% in a flow cell. Operando X-ray absorption results demonstrate that Cu delta+ species stabilized by the Cu-S motif exist in S-HKUST-1 during CO2RR. Density functional theory calculations indicate the partially oxidized Cu delta+ at the Cu/CuxSy interface is favorable for coupling of the *CO intermediate due to the modest distance between coupling sites and optimized adsorption energy.