Cu single-atom electrocatalyst on nitrogen-containing graphdiyne for CO_(2)electroreduction to CH4

作     者：Hao Dai Tao Song Xian Yue Shuting Wei Fuzhi Li Yanchao Xu Siyan Shu Ziang Cui Cheng Wang Jun Gu Lele Duan 戴昊;宋涛;乐弦;李福智;魏淑婷;徐延超;舒偲妍;崔子昂;王成;顾均;段乐乐

作者机构：Department of ChemistrySouthern University of Science and TechnologyShenzhen 518055GuangdongChina Center of Artificial Photosynthesis for Solar Fuels and Department of ChemistrySchool of ScienceWestlake UniversityHangzhou 310030ZhejiangChina Department of ChemistryTsinghua UniversityBeijing 100084China Division of Solar Energy Conversion and Catalysis at Westlake UniversityZhejiang Baima Lake Laboratory Co.LtdHangzhou 310000ZhejiangChina Institute of Natural SciencesWestlake Institute for Advanced StudyHangzhou 310024ZhejiangChina 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2024年第64卷第9期

页      面：123-132页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 

基　　金：国家自然科学基金(22179057) 西湖大学科研启动项目 

主　　题：Carbon dioxide reduction Electrocatalysis Cu single-atom catalyst N-containing graphdiyne Methane 

摘      要：Developing Cu single-atom catalysts(SACs)with well-defined active sites is highly desirable for producing CH4 in the electrochemical CO_(2)reduction reaction and understanding the structure-property ***,a new graphdiyne analogue with uniformly distributed N2-bidentate(note that N2-bidentate site=N^N-bidentate site;N2¹dinitrogen gas in this work)sites are *** to the strong interaction between Cu and the N2-bidentate site,a Cu SAC with isolated undercoordinated Cu-N2 sites(Cu1.0/N2-GDY)is obtained,with the Cu loading of 1.0 wt%.Cu1.0/N2-GDY exhibits the highest Faradaic efficiency(FE)of 80.6%for CH4 in electrocatalytic reduction of CO_(2)at-0.96 V ***,and the partial current density of CH4 is 160 mA cm^(-2).The selectivity for CH4 is maintained above 70%when the total current density is 100 to 300 mA cm^(-2).More remarkably,the Cu1.0/N2-GDY achieves a mass activity of 53.2 A/mgCu toward CH4 under-1.18 V *** situ electrochemical spectroscopic studies reveal that undercoordinated Cu-N2 sites are more favorable in generating key*COOH and*CHO intermediate than Cu nanoparticle *** work provides an effective pathway to produce SACs with undercoordinated Metal-N2 sites toward efficient electrocatalysis.