Carbon-supported CoS_(4)-C single-atom nanozyme for dramatic improvement in CO_(2)electroreduction to HCOOH:A DFT study combined with hybrid solvation model  

作　　者：Hao Sun Jingyao Liu 

机构地区：[1]Institute of Theoretical Chemistry,College of Chemistry,Jilin University,Changchun 130023,China

出　　处：《Chinese Chemical Letters》2023年第8期449-453,共5页中国化学快报（英文版）

基　　金：supported by the National Key Research and Development Program of China(No.2021YFA1500403);the National Natural Science Foundation of China(No.21773083).

摘　　要：Single-atom nanozymes(SANs)have attracted extensive attention due to their characteristics of both single-atom catalysts(SACs)and enzymes.Using spin-polarized density functional theory(DFT)calculations combined with the hybrid solvation model,this work designed a series of carbon-supported Group VIII transition metals TMS_(4)-C SANs,similar to the TMS_(4)active center of formate dehydrogenase(FADH),aiming to develop highly efficient SANs for CO_(2)electroreduction.DFT calculations show that compared with TMN4-C,TMS_(4)-C have FADH-like feature,which can selectively reduce CO_(2)to formic acid.Particularly,CoS4-C is the most promising SAN for CO_(2)reduction,with a low limiting potential of-0.07 V,which exceeds most reported catalysts.Two descriptors of TMX4-C(X=N,S)based on intrinsic and electronic structure properties were proposed to shed light on the origin activity of candidates.The findings presented here will provide new insights into the design of novel enzyme-like catalysts for electrochemical CO_(2)reduction.

关 键 词：Single-atom catalysts Nanozymes ELECTROCATALYSIS CO_(2)reduction Density functional theory 

分 类 号：X701[环境科学与工程—环境工程] TQ225.121[化学工程—有机化工] TQ426