文献类型：期刊文献

英文题名：A copper coordination polymer precatalyst with asymmetric building units for selective CO2-to-C2H4 electrolysis

作者：Wen, Chun Fang[1];Zhou, Min[2];Wu, Xuefeng[1];Liu, Yuanwei[1];Mao, Fangxin[1];Fu, Huai Qin[3];Shi, Yingli[1];Dai, Sheng[4];Zhu, Minghui[5];Yang, Shuang[1];Wang, Hai Feng[2];Liu, Peng Fei[1];Yang, Hua Gui[1]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Key Lab Ultrafine Mat,Minist Educ, 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]Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Gold Coast, Qld 4222, Australia;[4]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[5]East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2023

卷号：11

期号：23

起止页码：12121

外文期刊名：JOURNAL OF MATERIALS CHEMISTRY A

收录：;EI(收录号：20232414218395);WOS:【SCI-EXPANDED(收录号:WOS:000994129700001)】；

基金：This work was financially supported by the National Key R&D Program of China (2021YFA1500700), the Science and Technology Commission of Shanghai Municipality (21DZ1207101, 22ZR1416400), the Key Program of National Natural Science Foundation of China (22239001), 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 National Natural Science Foundation of China (22202069), the Innovation Program of Shanghai Municipal Education Commission (E00014), and the Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400). Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center. The authors 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 the Beijing Synchrotron Radiation Facility (BSRF) for their constructive assistance with the XAFS measurements and data analysis.

语种：英文

外文关键词：Carbon dioxide - Catalysts - Coordination reactions - Copper compounds - Density functional theory - Efficiency - Electrolytic reduction - Etching - X ray absorption

摘要：The electrochemical reduction of carbon dioxide (CO2) to value-added multi-carbon products provides a feasible way to achieve carbon neutrality. However, enhancing the faradaic efficiency for a specific multi-carbon product like ethylene at high current densities is still a challenge. Herein, we report a Cu(ii)-benzene-1,3,5-tricarboxylate coordination polymer (Cu-BTC-CP) with asymmetric building units, synthesized by a water etching strategy, for highly selective electrochemical CO2-to-C2H4 conversion. The Cu-BTC-CP catalyst achieves an ethylene faradaic efficiency as large as 65.2 +/- 3% at a high current density of 350 mA cm(-2) in a flow cell. Operando X-ray absorption fine structure analysis uncovers that the Cu-BTC-CP catalyst reconstructs to low-coordinated copper under reaction conditions. Density functional theory calculations further indicate that the low-coordinated Cu sites on metallic Cu surfaces are favorable for *CO intermediate coupling and promote CO2 conversion to ethylene.