In-situ electrochemical interface of Cu@Ag/C towards the ethylene electrosynthesis with adequate ^(*)CO supply  

作　　者：Haotian Duan Wenyang Li Lixiu Ran Fulong Zhu Tianxiang Li Ming Miao Wen-Jin Yin Xin Wang Yongzhu Fu 

机构地区：[1]College of Chemistry,Zhengzhou University,Zhengzhou 450001,Henan,China [2]School of Physics and Electronic Science,Hunan University of Science and Technology,Xiangtan 411201,Hunan,China [3]Department of Chemistry,Biochemistry and Pharmaceutical Sciences,University of Bern,Bern 3012,Switzerland

出　　处：《Journal of Energy Chemistry》2024年第12期292-299,共8页能源化学（英文版）

基　　金：financially supported by the National Natural Science Foundation of China (22303087);the Joint Fund of the Technical R&D Program of Henan Province (232301420049);the Natural Science Foundation of Henan province (212300410281)。

摘　　要：The conversion of carbon dioxide to ethylene by electrochemical reduction (CO_(2)RR) provides a new strategy for achieving carbon dioxide conversion.However,copper-based catalysts have the disadvantages of unsatisfactory selectivity and low current density,which limit the potential CO_(2)RR industrial expansion.Researches have verified that the real reaction sites at the catalyst surface often undergo reconstruction during the reaction,therefore,understanding and utilizing this phenomenon is crucial for improving catalytic performance.In this work,we introduced additional Ag component into Cu@Ag/C tandem catalyst by in-situ electrochemical reconstruction of Cu_(2)CO_(3)(OH)_(2)/AgCl/C precursor.This electro-reduced catalyst exhibits a C_(2)H_(4)Faradaic efficiency of 50.41%in H-cell,and 58.03%in the flow cell,surpassing the counterparts of pure Cu and Ag,as well as the Cu-Ag homolog with separated interface.Moreover,it also provides a long-term stability of 21 h with the ethylene Faraday efficiency (FE) over 50%.The appropriate amount of Ag dopant into the Cu catalyst changes the electronic structure of Cu surface by the electron transfer from Cu to Ag,which distinctly enhances the binding energy of CO_(2) on the catalyst.Meanwhile,in-situ Raman results and theoretical calculation reveal that the introduction of silver increases the number of active sites and improves the coverage of*CO intermediate,thereby accelerating the kinetics of C–C coupling and reducing its energy barrier.The combination of cascade catalytic strategy and in-situ electroreduction interface provides potential applications for future artificial carbon balance.

关 键 词：Basic copper carbonate SILVER Tandem catalyst CO_(2)reduction reaction ETHYLENE 

分 类 号：TQ426[化学工程] TQ221.211