How water molecules occupying the active site of a single-atom catalyst affect the electrochemical reduction of carbon dioxide

作     者：Jia Zhao Di Liu Fenfei Wei Weng Fai Ip Hui Pan Sen Lin Jia Zhao;Di Liu;Fenfei Wei;Weng Fai Ip;Hui Pan;Sen Lin

作者机构：State Key Laboratory of Photocatalysis on Energy and EnvironmentCollege of ChemistryFuzhou UniversityFuzhou 350002China Institute of Applied Physics and Materials EngineeringUniversity of MacaoTaipa 999078MacaoChina Department of Physics and ChemistryFaculty of Science and TechnologyUniversity of MacaoTaipa 999078MacaoChina 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2023年第16卷第7期

页      面：9091-9098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：We thank the National Natural Science Foundation of China(No.21973013) the National Natural Science Foundation of Fujian Province,China(No.2020J02025) the“Chuying Program”for the Top Young Talents of Fujian Province 

主　　题：electrocatalytic CO_(2)reduction solvent effect single-atom catalysis density functional theory ab initio molecular dynamics 

摘      要：In single-atom catalysts(SACs),the single atoms are often exposed as protrusions above the *** solvent molecules in the electrocatalytic environment can interact or even bind to these coordination-unsaturated single atoms and thus influence the reaction process,but this has not been studied in *** this work,we systematically investigate the thermodynamics of CO_(2)reduction reaction(CO_(2)RR)to CO over MoS_(2)-supported single metal atom catalysts(TM@MoS_(2),TM=transition metal)under vacuum and explicit solvent environments using density functional *** addition,the ab initio molecular dynamics results show that explicit H_(2)O molecules can coordinate to the TM site and undergo competitive adsorption with the CO_(2)RR intermediates,which significantly affects the energy and conformation of the CO_(2)RR *** structure analysis reveals that the occupying H_(2)O molecules change the electronic state of single atom and further influence the adsorption strength of different CO_(2)RR *** work shows that water molecules can not only act as ligands to influence the electronic state of TM,but also affect the energy and conformation of CO_(2)RR intermediates,which highlights the important role of occupying H_(2)O molecules at the single-atom sites in CO_(2)RR and provides useful insights for the design of SACs for efficient CO_(2)RR.