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 Jiajun Wang;Guolin Yi;Shengling Guo;Jianing Wang;Shujuan Li;Ke Xu;Weiyi Wang;Shulai Lei

作者机构：Tianjin Key Laboratory of Structure and Performance for Functional MoleculesCollege of ChemistryTianjin Normal UniversityTianjin 300387China Department of Chemical Physics&Hefei National Laboratory for Physical Sciences at MicroscaleUniversity of Science and Technology of ChinaHefei 230026China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and DevicesHubei University of Arts and ScienceXiangyang 441053China Hubei Longzhong LaboratoryXiangyang 441053China 

出 版 物：《Chinese Chemical Letters》 (中国化学快报（英文版）)

年 卷 期：2024年第35卷第7期

页      面：484-490页

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

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) 

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

摘      要：Electrochemical CO reduction(ECOR)as a potential strategy for producing valuable chemicals and fuels has captured substantial ***,the currently available electrocatalysts suffer from poor selectivity and low Faradaic efficiency,limiting their industrial ***,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 *** findings suggest that all four proposed monolayers exhibit exceptional stability,making them highly suitable for experimental synthesis and practical ***,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 ***,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 *** predictions would accelerate the development of high-performance C_(9)N_(4)-based dual-atom catalysts for the ECOR.