文献类型：期刊文献

英文题名：Altering the CO2 Electroreduction Pathways Towards C1 or C2+ Products via Engineering the Strength of Interfacial Cu-O Bond

作者：Zhang, Yu[1];Li, Yicheng[1];Gao, Nana[2];Delmo, Ernest Pahuyo[3];Hou, Guoyu[1];Luo, Ali[2];Wang, Dongyang[5];Chen, Ke[5];Antonietti, Markus[4];Liu, Tianxi[6];Tian, Zhihong[2]

机构：[1]East China Univ Sci & Technol, Sch Mech & Power Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Henan Univ, Engn Res Ctr Nanomat, Kaifeng 475004, Peoples R China;[3]Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Kowloon, Clear Water Bay, Hong Kong, Peoples R China;[4]Max Planck Inst Colloids & Interfaces, Dept Colloid Chem, Muhlenberg 1, D-14476 Potsdam, Germany;[5]Henan Univ, Ctr Phys Low Dimens Mat, Sch Phys & Elect, Sch Future Technol, Kaifeng 475004, Peoples R China;[6]Jiangnan Univ, Sch Chem & Mat Engn, Key Lab Synthet & Biol Colloids, Minist Educ, Wuxi 214122, Peoples R China

年份：2024

卷号：63

期号：36

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20243116802301);WOS:【SCI-EXPANDED(收录号:WOS:001281926400001)】；

基金：This work was supported by the National Natural Science Foundation of China (No. 22109044, No. 52373205, No. 52003251), Natural Science Foundation of Shanghai, China (No. 22ZR1418500), start-up funds from the East China University of Science and Technology, Henan Center for Outstanding Overseas Scientists (GZS2022014), and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Electrocatalysis; CO2 Reduction; Cu-Based Catalyst; Coordination polymers; Reaction pathways

摘要：Copper (Cu)-based catalysts have established their unique capability for yielding wide value-added products from CO2. Herein, we demonstrate that the pathways of the electrocatalytic CO2 reduction reaction (CO2RR) can be rationally altered toward C-1 or C2+ products by simply optimizing the coordination of Cu with O-containing organic species (squaric acid (H2C4O4) and cyclohexanehexaone (C6O6)). It is revealed that the strength of Cu-O bonds can significantly affect the morphologies and electronic structures of derived Cu catalysts, resulting in the distinct behaviors during CO2RR. Specifically, the C6O6-Cu catalysts made up from organized nanodomains shows a dominant C-1 pathway with a total Faradaic efficiency (FE) of 63.7 % at -0.6 V (versus reversible hydrogen electrode, RHE). In comparison, the C4O4-Cu with an about perfect crystalline structure results in uniformly dispersed Cu-atoms, showing a notable FE of 65.8 % for C2+ products with enhanced capability of C-C coupling. The latter system also shows stable operation over at least 10 h with a high current density of 205.1 mA cm(-2) at -1.0 V-RHE, i.e., is already at the boarder of practical relevance. This study sheds light on the rational design of Cu-based catalysts for directing the CO2RR reaction pathway.