Modified Cu active sites by alloying for efficient electrocatalytic reduction CO_(2) to CO  

作　　者：Yan Wang Ruikuan Xie Naixuan Ci Zhiyuan Zhu Chaoyi Li Guoliang Chai Hua-Jun Qiu Yinghe Zhang 

机构地区：[1]Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application,Harbin Institute of Technology,Shenzhen 518055,Guangdong,China [2]School of Science,Harbin Institute of Technology,Shenzhen 518055,Guangdong,China [3]School of Materials Science and Engineering,Harbin Institute of Technology,Shenzhen 518055,Guangdong,China [4]State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou 350002,Fujian,China

出　　处：《Journal of Energy Chemistry》2024年第12期450-457,共8页能源化学（英文版）

基　　金：supported by Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application(No.ZDSYS20220527171407017)。

摘　　要：Transition metals like Au,Ag,and Cu have been reported to be quite active for CO_(2) reduction.In this study,we use density functional theory(DFT)calculation to investigate the electronic structure and catalytic performance of Au,Ag,Cu and their alloys for CO_(2) reduction reaction(CO_(2)RR).Theoretical calculations identified the combination of Ag,Cu,and Au in a face-centered cubic(fcc)alloy as an outstanding electrocatalyst for CO_(2) reduction to CO,with Cu as the active site.The d-orbital projected density of state(PDOS)profile suggests that alloying alters the electronic structure of the Cu site,thereby affecting the Gibbs free energy change for the formation of*COOH intermediate(ΔG_(*COOH)).To demonstrate the theoretical prediction experimentally,we employ a top-down dealloying approach to synthesize a nanoporous structured AgCuAu alloy(NP-Ag_(5)Cu_(5)Au_(5)).Electrochemical experiments validate that the ternary alloy catalyst is clearly better than unary and binary catalysts,showing a Faradaic efficiency(FE)for CO over 90%across a broad potential range of 0.6 V,with a peak of approximately 96%at-0.573 V vs.RHE.This study underscores the potential of multi-component alloys in CO_(2)RR and establishes a theoretical basis for designing efficient catalysts for CO_(2) utilization.

关 键 词：CO_(2)reduction CO Multi-component alloy Nano-porous ELECTROCATALYST 

分 类 号：TQ127.12[化学工程—无机化工] TQ426