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ResearchArticles

Angewanie

ElectrocatalysisVeryImportantPaperHowtocite:Angew.Chem.Int.Ed.2023,62,e202310740

Electrocatalysis

VeryImportantPaper

SulfurChangestheElectrochemicalCO2ReductionPathwayoverCuElectrocatalysts

ShuyuLiang+,JiewenXiao+,TianyuZhang,*YueZheng,QiangWang,*andBinLiu*

Abstract:ElectrochemicalCO2reductiontovalue-added

chemicalsorfuelsoffersapromisingapproachtoreducecarbonemissionsandalleviateenergyshortage.Cu-basedelectrocatalystshavebeenwidelyreportedascapableofreducingCO2toproduceavarietyofmulti-carbonproducts(e.g.,ethyleneandethanol).Inthiswork,wedevelopsulfur-dopedCu2Oelectrocatalysts,whichinsteadcanelectrochemicallyreduceCO2toalmostexclusivelyformate.WeshowthatadynamicequilibriumofSexistsattheCu2O-electrolyteinterface,andS-dopedCu2Oundergoesinsitusurfacereconstruc-tiontogenerateactiveS-adsorbedmetallicCusitesduringtheCO2reductionreaction(CO2RR).Densityfunctionaltheory(DFT)calculationstogetherwithinsituinfraredabsorptionspectroscopymeasurementsshowthattheS-adsorbedmetallicCusurfacecannotonlypromotetheformationofthe*OCHOintermediatebutalsogreatlysuppress*Hand*COOHadsorption,thusfacilitatingCO2-to-formateconversionduringtheelectrochemicalCO2RR.

Introduction

TransformingCO2tovalue-addedchemicalsorfuelspoweredbyrenewableenergyprovidesanattractive

[*]S.Liang,+J.Xiao,+T.Zhang,Y.Zheng,Q.Wang

BeijingKeyLabforSourceControlTechnologyofWaterPollution,CollegeofEnvironmentalScienceandEngineering,BeijingForestryUniversity

Beijing100083(P.R.China)and

EngineeringResearchCenterforWaterPollutionSourceControlEco-remediation,CollegeofEnvironmentalScienceandEngineer-

ing,BeijingForestryUniversityBeijing100083(P.R.China)