Computational design of bimetallic Tm_(2)@g-C_(9)N_(4)electrocatalysts for enhanced CO reduction toward C_(2)products  

作　　者：Jiajun Wang Guolin Yi Shengling Guo Jianing Wang Shujuan Li Ke Xu Weiyi Wang Shulai Lei 

机构地区：[1]Tianjin Key Laboratory of Structure and Performance for Functional Molecules,College of Chemistry,Tianjin Normal University,Tianjin 300387,China [2]Department of Chemical Physics&Hefei National Laboratory for Physical Sciences at Microscale,University of Science and Technology of China,Hefei 230026,China [3]Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices,Hubei University of Arts and Science,Xiangyang 441053,China [4]Hubei Longzhong Laboratory,Xiangyang 441053,China

出　　处：《Chinese Chemical Letters》2024年第7期484-490,共7页中国化学快报（英文版）

基　　金：supported by the Science and Technology Research Project of Hubei Provincial Department of Education(No.D20212603);Hubei University of Arts and Science(No.2020kypytd002);National Natural Science Foundation of China(No.22303098);Natural Science Foundation of Hubei Province(No.2022CFC030)。

摘　　要：Electrochemical CO reduction(ECOR)as a potential strategy for producing valuable chemicals and fuels has captured substantial attention.However,the currently available electrocatalysts suffer from poor selectivity and low Faradaic efficiency,limiting their industrial application.Herein,we systematically investigate the potential of homonuclear bimetallic electrocatalysts,Tm_(2)@C_(9)N_(4)(TM=Fe,Co,Ni,and Cu),for the ECOR through extensive density functional theory calculations.Our findings suggest that all four proposed monolayers exhibit exceptional stability,making them highly suitable for experimental synthesis and practical applications.Interestingly,these transition-metal dual atoms anchored on C_(9)N_(4)monolayers show great potential in facilitating the production of high-value C_(2)products,such as C_(2)H_(5)OH and C_(2)H_(4),due to the significantly low limiting potentials(-0.06~-0.46 V)and small kinetic energy barriers(0.54–1.08 eV)for the CO coupling process.Moreover,with the exception of Ni_(2)@C_(9)N_(4),these bimetallic catalysts demonstrate the impressive suppression of the competitive hydrogen evolution reaction(HER),leading to a high selectivity for C_(2)products in ECOR.Our predictions would accelerate the development of high-performance C_(9)N_(4)-based dual-atom catalysts for the ECOR.

关 键 词：C_(9)N_(4)monolayer Double-atom catalysts CO electroreduction Multi-carbon products Density functional theory 

分 类 号：O643.36[理学—物理化学] TQ207[理学—化学] X701[化学工程—有机化工]