FeS-anchored transition metal single atoms for highly efficient overall water splitting：a DFT computational screening study.docx

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1、18December2020ROYA1SOCIETYrOFCHEMISTRYJourna1ofMateria1sChemistryAPAPERViewArtic1eOn1ineViewJoumaIwn1oadedbyUniversityofScienceandTechnoIogyofChinaon1/13/202112)CheckforupdatesFeS2-anchoredtransitionmeta1sing1eatomsforhigh1yefficientovera11watersp1itting:aDFTCitethis:DOI:10.1039d0ta09903acomputation

2、a1screeningstudy+G.YingjuYang,Jing1iu,*Feng1iu,ZhenWangandDaweiWuHydrogenproductionfromwatere1ectro1ysisusingrenewab1ee1ectricityiswide1yregardedasahigh1ypromisingroutetoso1vetheenergycrisisofhumansociety.However,therationa1designof1ow-coste1ectrocata1ystswithexce11entcata1yticactivityand1ong-termdu

3、rabi1itytowardthehydrogenevo1utionreaction(HER)andoxygenevo1utionreaction(OER)remainsasignificantcha11enge.Herein,Wereportedasystematicdensityfunctiona1theory(DFT)studyonthescreeningofFeS2-supp0rtedtransitionmeta1sing1eatoms(M(S)FeSi)ase1ectrocata1ystsfortheHERandOER.Theresu1tsindicatethatMFeS?cata1

4、ystsexhibitexce11enttherma1stabi1ityandgoode1ectrica1conductivityfore1ectrochemica1reactions.Transitionmeta1atomsareidentifiedastheactivesitesfortheHERandOER.Cr(S)FeSzandVFeSzexhibitexce11entcata1yticactivitytowardstheHER.Inparticu1ar,Cr(S)FeSzhasaDGhva1ueof0.049eVandpresentsa1oweractivationenergyba

5、rrierof0.22eVfortheHER.TheHERactivityofCrFeSzisReceivedIOthOctober2023Accepted18thDecember2023evenhigherthanthatofthecurrentmostefficientPtcata1ysts.MnFeS?showsgoodOERactivityandisexpectedtobeapromisingcandidateforOERe1ectrocata1ysts.Thisworkcou1dpaveanewwayto01,39dtaO99O3adesigncost-effectivee1ectr

6、ocata1ystsfortheHERandOER,anda1soshed1ightontheapp1icationofrsc.imateria1s-aFeS?-basedmateria1sinwatersp1itting.1. IntroductionHydrogen(H2),asanidea1energycarrier,isexpectedtobeac1eanandsustainab1ea1ternativetofossi1fue1sinthefutureduetoitshighenergydensity,zero-carbonemissionandrecyc1abi1ity.,3Hydr

7、ogenevo1utionfrome1ectrochemica1watersp1ittingusingrenewab1eresource-derivede1ectricityisaveryefficienttechno1ogyforhigh-purityhydrogenproduction.4-7Watere1ectro1ysisinc1udestwoha1fce11reactions:thehydrogenevo1utionreaction(HER)andtheoxygenevo1utionreaction(OER).8However,thesee1ectrochemica1reaction

8、ssufferfroms1uggishkinetics,91eadingtoahighwater-sp1ittingoverpotentia1.10Therefore,high1yefficiente1ectrocata1ystsarerequiredtoacce1eratethee1ectrochemica1reactionsandtominimizetheoverpotentia1forH2production.Current1y,p1atinum-groupmeta1s(PGMs)andtheirderivativemateria1sarewe11-knownasthemosteffic

9、ientcata1ystsfortheHERduetotheextraordinarye1ectronicconductivityandoptimumGibbsfreeenergyofatomichydrogenadsorptiononthee1ectrocata1ystsurface.11-13However,(he1arge-sca1ecommercia1app1icationofPGM-basedmateria1sis1imitedbyStateKey1aboratorjofCoa1Combustion.Schoo1ofEnergyandPowerEngineering.Huazhong

10、UniversityofScienceandTechno1ogy.Wuhan430074.China.E-mai1:1iujing27mai1.hu：Fax:+862787545526;Te1:+862787545526+E1ectronicsupp1ementary,information(ES1)avai1ab1e.SccDOI:IO.1O39dOiaO99O3a(heirhighcostandnatura1scarcity.14-17Thus,fromtheviewpointofproductivityandcosteffectiveness,signicanteffortsneedto

11、bedevotedtothedesignanddeve1opmentofcosteffectiveandearth-abundante1ectrocata1ystmateria1sforwatere1ectro1ysis.First-rowtransitionmeta1-basedmateria1shavebeenregardedashavinggreatpotentia1forwatere1ectro1ysisduetothefascinatinge1ectronicpropertiesand1argegeo1ogica1reserves.141819However,the1argeacti

12、vitygapbetweentransitionmeta1sandPGMssti11remainsunacceptab1e.Recent1y,anemergingc1assoftransition-meta1sing1e-atomcata1ysts(TM-SACs)hasshownsuperiorcata1yticactivityforwatere1ectro1ysis.20-22Moreover,sing1e-atomcata1ystscanmaximizetheatomicuti1izationefficiencyandpossesswe11-denedactivesites.643-25

13、DespitethemanysuccessesofTM-SACsforwatere1ectro1ysis,thehighsurfacefreeenergyofTM-SACsenab1estransitionmeta1sing1eatomstoagg1omerateeasi1y,1eadingtoasignicantdecreaseinthecata1yticactivityofTM-SACs.267Toso1vethisagg1omerationprob1em,thekeyprincip1eistotunetheinteractionbetweenthesing1emeta1atomandsu

14、pport.26Notab1y,itishigh1ydesirab1etouseanappropriatesupportwhichcanstabi1izetransitionmeta1atomsandcreatehigh1ystab1eactivesites.Recent1y,transition-meta1su1deshaveattractedsignicantinterestforefficientenergyconversionduetotheireasi1ytunab1ee1ectronic,physica1andchemica1properties.9-28-30Amongthese

15、varioustransition-meta1su1des,FeS2canserveasafavorab1esupporttostabi1izesing1emeta1atomsduetotheuniquesurfacecoordinationchemistryandearth-abundantironpyriteminera1s.31-33Moreover,FeSza1soactsasanactivee1ectrocata1ystforthehydrogenevo1utionreaction.34,0Inspiredbythesesignicantadvancements,itisexpect

16、edthatthecombinationoftransitionmeta1sing1eatomsandtheFeSisupportmaybeanefficientstrategytodeve1opinexpensiveandexce11ente1ectrocata1ystsforwatere1ectro1ysis.However,FeS2-anchoredtransitionmeta1sing1eatomshaverare1ybeenpaidanyattention.Inthiswork,wedesignedaseriesofFeS2-anch0redtransitionmeta1cata1ysts(MFeS2,Mrsi-rowtransitionmeta1atoms)andsystematica11yinvestigatedtheircata1yticactivitytowa