Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO2‐to‐CH4 PhotoreductionWord下载.docx

Revealing the Sudden Alternation in Pt@h‐BN Nanoreactors for Nearly 100% CO2‐to‐CH4 PhotoreductionWord下载.docx

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Howtodevelopanefficientphotocatalystwithhighactivityandhighselectivityisthebiggestchallengelimitingtheapplicationofphotocatalysis.Areasonabledesignofthenanoreactormodelisaneffectivestrategy.Herein,aseriesofPtnanoparticlescoatedwithhexagonalboronnitride（Pt@h-BN）nanoreactorshighlydispersedonaphotochemicallyinertcarrier,Al2O3substrate,aresynthesized.Theresultsshowthatasthenumberofh-BNcoatinglayersincreases,theselectivityofphotocatalysisisalteredfromnearly100%CO2-to-COtonearly100%CO2-to-CH4,andtheoptimizedspace-timeyieldofCH4isupto184.7pmolg（Pt）-1h-1withthree-layercoating.TheinsitucharacterizationsrevealthecleavageoftheCOonPttobetheratedeterminingstepandtheexistenceofthekeyintermediateCO2~speciesonthesurfaceofPt@h-BNfacilitatesCH4formation.Notably,combinedwithdetailedsimulationcalculations,thisworkrevealsthattheconfinementeffectinPt@h-BNattributestheelectronsmobilitybehaviorandalleviatetheinteractionofCO—Pt.Whatismore,thechangeofthereactionsiteistheessenceforthesuddenalternation.Thisworkwillbringanewinsighttotheselectivecatalysisofnoblemetalsinthegas-solidphase.

1. Introduction

Duetothehugefossilenergyconsumptioninthepast100years,theCO2concentrationintheeath'

satmospherehascontinuedtorise,andnowithasexceeded410ppmJ1,2]Knowingthatthegreenhouseeffectisdestructivetohumansociety,agroupoftopscientistsproposedsomeconceptsofuliquidsun-light"

【3-5】"

artificialphotosynthesis”,"

-，and'

'

futuristicsolarrefineryActually,theseconceptsessentiallyfollowthisformula:

CO2+water+sunlight=greenfuel+oxygen.Sinceitcantrulyachievezerocarbonemissions,solarenergyhasgraduallyattractedpeople'

sattentionasanidealenergysourceforproducinghighvalue-addedchemicals.Throughtheprocessofartificialphotosynthesis,CO2gascanbeeasilyfixed,asastrategyofkillingtwobirdswithonestonetoproducechemicals

Dr.W.Bi,Prof.Y.Hu,Prof.H.Jiang,Prof.L.Zhang,Prof.C.LiShanghaiEngineeringResearchCenterofHierarchicalNanomaterialsKeyLaboratoryforUltrafineMaterialsofMinistryofEducationSchoolofMaterialsScienceandEngineeringEastChinaUniversityofScience&

TechnologyShanghai200237,China

E-mail:

huyanjie@;

czli@

TheORCIDidentificationnumber（s）fortheauthor（s）ofthisarticlecanbefoundunderhttps:

//doi.org/10.1002/adfm,202010780.

DOI:

10.1002/adfm.202010780fbrhumanactivities.However,torealizetheabovevision,thebiggestchallengeliesinthedevelopmentandutilizationofphotocatalystswithhighactivityandhighselectivity.

Forthedevelopmentofefficientphotocatalysts,scientistshavedonealotofmeaningfulwork」”—”]Jiangetal.2]reportedthatbyaccuratelyanchoringTiO2intwodiflferentmolecularcompartmentsofMIL-101,aquantumefficiencyofupto11.3%wasachieved,provingthattheprecisepositioningofTiO2inthemetal-organicframework（MOF）systemcaneffectivelyimprovethematerialperformance.LietalJ16^reportedthatthroughatop-downdirectmetalatomizationmethodtopreparesingleatomsandtheuseofC=Ospeciestoadjustthecoordinationenvironment,ahighturnovernumberof1493.5couldbeachievedinCO2photoreductionprocess.Wangetal.阿reportedaphotocatalyticsystemthatcouplesdirectandindirectZ-schemeheterostructurestorealizethestoichiometricphotocatalyticreactionofCO2andH2O.Thehigherreductionpotentialcombinedwiththespatialseparationefficiencyeffectivelypreventsthereversereactionoftheproduct.JiangetalJ18lconstructeda2D/2Dultra-thinZ-schemeheterojunctionthroughasimpleself-assemblymethod.UnderAM1.5Girradiation,theyieldofthetotalmixedproductofthetargetedmaterialwas-153.1jimolg-1in6h,whichis12.2timeshigherthanthatofthecontrolsample.Thisworkprovidesanewinsightfbrtherapidseparationandtransferofelectrons.

However,duringthereactionprocess,selectivityoptimizationinphotocatalyticCO2reduction（CO2PR）applicationsisoftenmorechallengingthanactivityimprovement.BieetalJ19]reportedasingle-layernitrogen-dopedgraphene-coatedCdShollowsphere.Throughreasonableadjustmentofthecontactinterfacebetweenthephotocatalystandtheco-catalyst,theperformancewasfinallyimprovedbyfourtofivetimes.However,theselectivityofCH4asthemainproductisonlycloseto33.8%.Inordertoimproveselectivity,theusualstrategyistochangethehighlyexposedactivesurfaceofthematerial,ortoaddasacrificialagenttothereactionsystem.LietalP。

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