磷原子摻雜氫氧化物的制備和氧析出性能研究摘要預催化劑的結(jié)構調(diào)整將不可避免地引發(fā)材料內(nèi)部屬性的改變，進而引起催化反應能壘及動力學改變。由于大多數(shù)預催化劑經(jīng)過重構后活性有所提高，且重構物種提供了真實的催化位點和較高的催化活性，因此深化重構程度，開發(fā)完全重構的催化劑具有重要的價值。由于在電解水中OER過程存在較高的能量勢壘且化學動力學過程緩慢，要求催化劑具有高效的催化反應活性。當前，工業(yè)電解水制氫中所使用的催化劑大多為貴金屬OER催化劑(IrO2或RuO2)，存在價格昂貴、資源稀缺等缺點，這對于氫能的大規(guī)模生產(chǎn)和應用是不利的。因此，研發(fā)既高效又穩(wěn)定，且成本相對較低的非貴金屬催化劑變得尤為關鍵。鎳鐵氫氧化物是最具發(fā)展?jié)摿Φ膲A性OER電催化劑，在摻雜雜原子后，催化劑在活性位點數(shù)量增加、電子結(jié)構優(yōu)化以及吸附性能改善等因素綜合作用下，能夠有效提高水電解性能。本論文中制備了磷摻雜的鎳鐵基雙氫氧化物電催化劑，并探索其在堿性條件下的OER催化性能。代表性樣品NF/NiFeP-15在堿性電解液當中具有較好的穩(wěn)定性和較低的Tafel斜率(49.8mVdec-1)，說明其較快的OER反應動力學。關鍵詞：重構現(xiàn)象、電解水、析氧反應、雜原子摻雜、鎳鐵氫氧化物

AbstractThereconstructionoftheprecatalystwillinevitablyleadtochangesintheintrinsicpropertiesofthematerial,resultinginchangesintheenergybarrierandkineticsofthecatalyticreaction.Duetotheimprovedactivityofmostprecatalystsafterreconstruction,andthefactthatthereconstructedspeciesproviderealcatalyticsitesandhighcatalyticactivity,itisofgreatvaluetodeepenthedegreeofreconstructionanddevelopfullyreconstructedcatalysts.DuetothehighenergybarrierandslowchemicalkineticsintheOERprocessofelectrolyzingwater,itisrequiredthatthecatalysthasefficientcatalyticreactionactivity.Currently,mostofthecatalystsusedinindustrialelectrolysisofwaterforhydrogenproductionarepreciousmetalOERcatalysts(IrO2orRuO2),whichhavedisadvantagessuchashighcostandscarceresources,whicharenotconducivetothelarge-scalepreparationanduseofhydrogenenergy.Therefore,developingefficient,stable,andcost-effectivenon-preciousmetalcatalystsisparticularlyimportant.NickelironhydroxideisthemostpromisingalkalineOERelectrocatalyst.Afterdopingwithheteroatoms,thecatalystcaneffectivelyimproveitswaterelectrolysisperformancebyincreasingthenumberofactivesites,optimizingitselectronicstructure,andimprovingitsadsorptionperformance.Inthispaper,phosphorusdopednickelirondoublehydroxideelectrocatalystswerepreparedandtheirOERcatalyticperformanceunderalkalineconditionswasexplored.TherepresentativesampleNF/NiFeP-15exhibitsgoodstabilityandalowTafelslope(49.8mVdec-1)inalkalineelectrolyte,indicatingitsfastOERreactionkinetics.Keywords:reconstructionphenomenon,electrolysisofwater,oxygenevolutionreaction,heteroatomdoping,nickelironhydroxide

目錄1.緒論 51.1前言 51.2析氧反應（OER）機理 61.3金屬基析氧催化劑研究進展簡介 61.3.1金屬氧化物/氫氧化物電催化劑 61.3.2硫化物/氮化物/磷化物電催化劑 82.本文研究的意義與主要內(nèi)容 92.1研究內(nèi)容 92.2實驗儀器 92.3實驗材料 102.4實驗部分 102.5電化學測試 112.5.1循環(huán)伏安法(CV) 112.5.2線性掃描伏安法(LSV) 112.5.3電化學交流阻抗(EIS) 113.結(jié)果與討論 124.結(jié)論 18參考文獻 19

1.緒論1.1前言預催化劑重構必然會引起物質(zhì)內(nèi)在性質(zhì)改變，進而引起催化反應能量勢壘及動力學改變。所以研究重構產(chǎn)生的根源對認識重構化學非常關鍵。研究者們發(fā)現(xiàn)催化劑重構現(xiàn)象在OER、HER和CO2還原中普遍存在，從而推動了學者對催化重構的科學認識ADDINZOTERO_ITEMCSL_CITATION{"citationID":"DXUoew1x","properties":{"formattedCitation":"\\super1\\uc0\\u8211{}4\\nosupersub{}","plainCitation":"1–4","noteIndex":0},"citationItems":[{"id":556,"uris":["/users/10605487/items/PB7VYVDL"],"itemData":{"id":556,"type":"article-journal","abstract":"Abstract\nEvaluatingthedynamicstructuralreconstructionprocessesoftransitionmetal‐basedoxygenevolutionreaction(OER)catalystsatindustrialcurrentdensitiesinamembraneelectrodeassembly(MEA)configurationofananionexchangemembrane(AEM)electrolyzerisrequiredforthepracticalapplicationofOERelectrodesinAEM‐typenext‐generationelectrolyzers.ThisstudyunveilsthedeepreconstructionphenomenonofaMo‐containingOERcatalystanodeduringelectrolysisathighcurrentdensities.AcompletereconstructionofthecatalystduetoselectiveMo‐leachingisinevitableduringhighcurrentoperationandtherebynewcatalyticsurfacesoftheMo‐containingNi‐basedelectrodesforsustainablewaterelectrolysisareexposed.Thereconstructionwasconfirmedbyexsituandin?situsurfacecharacterizationtechniques.Ascalablerouteforelectrodefabricationdemonstratedanditisshownthatthereconstructionmechanismofthecatalystleadstoamoresustainableoperationoftheelectrolyzerathighcurrentdensities.","container-title":"ChemCatChem","DOI":"10.1002/cctc.202301023","ISSN":"1867-3880,1867-3899","issue":"2","journalAbbreviation":"ChemCatChem","language":"en","page":"e202301023","source":"DOI.org(Crossref)","title":"DeepReconstructionofMo‐basedOERPre‐CatalystsinWaterElectrolysisatHighCurrentDensities","volume":"16","author":[{"family":"Antony","given":"RajiniP."},{"family":"Cechanaviciute","given":"IevaA."},{"family":"Quast","given":"Thomas"},{"family":"Zerdoumi","given":"Ridha"},{"family":"Saddeler","given":"Sascha"},{"family":"Junqueira","given":"Jo?oR.C."},{"family":"Schuhmann","given":"Wolfgang"}],"issued":{"date-parts":[["2024",1,22]]}},"label":"page"},{"id":552,"uris":["/users/10605487/items/RBC8BHE6"],"itemData":{"id":552,"type":"article-journal","abstract":"Transitionmetalnitrides(TMNs)electrocatalystsexperiencerapidperformancedegradationduringoxygenevolutionreaction(OER)duetosevereandirreversibleelectrochemicalreconstruction,impedingtheirpracticalapplicationinelectrochemicalwatersplitting.Toaddressthisissue,ternarymetal(Ni,Fe,Cr)nitridenanoparticlesonspongynitrogen‐dopeddisorderedcarbonskeletonelectrocatalyst(NFCN/C)issynthesizedusinganovelone‐potpyrolysisofeutecticmixturemethod.Theionomer‐freeNFCN/Celectrode,whichundergoesmoderateelectrochemicalreconstruction,demonstrateshighOERperformanceinbothalkalinefreshwaterandseawatersolutions,achievingacurrentdensityof250?mA?cm\n?2\nwithlowoverpotentialsof349and364?mV,respectively.TheNFCN/CanodewithPt/Ccathodedelivers10?mA?cm\n?2\natalowcellvoltageof1.49?Vandexhibitslong‐termdurabilityof450?hat500?mA?cm\n?2\n.In?situRamanspectroscopyandultravioletphotoelectronspectroscopy(UPS),alongwithpre‐andpost‐characterizations,elucidatethatbothhighelectrocatalyticactivityandrobustnessofNFCN/CforOERstemfromtheproposedintrinsicstrategyintegratingphysicalandelectronicstructures.ThisworkpavesthewayfordesigninghighlyefficientandrobustTMNselectrocatalystswithmoderateelectrochemicalreconstructionforindustrialfreshwaterandseawaterelectrolysis.","container-title":"SmallStructures","DOI":"10.1002/sstr.202400031","ISSN":"2688-4062,2688-4062","issue":"8","journalAbbreviation":"SmallStructures","language":"en","license":"/licenses/by/4.0/","page":"2400031","source":"DOI.org(Crossref)","title":"ModeratelyReconstructedTernaryMetalNitrideNanoparticlesforHighlyEfficientandRobustFreshwaterandSeawaterOxidationunderIndustrialCurrentDensity","volume":"5","author":[{"family":"Wang","given":"Shihao"},{"family":"Pan","given":"Hongfei"},{"family":"Wang","given":"Yadong"},{"family":"Tang","given":"Haolin"},{"family":"Zhang","given":"Haining"}],"issued":{"date-parts":[["2024",8]]}},"label":"page"},{"id":551,"uris":["/users/10605487/items/HHP63A5I"],"itemData":{"id":551,"type":"article-journal","abstract":"Theinvestigationoftransitionmetalphosphides(TMPs)asefficientelectrocatalystsforwatersplittinghasgarneredsignificantattentioninacademicresearch.Nevertheless,limitedresearchhasbeenconductedonthealterationofthestructuralandmorphologicalpropertiesofTMPsresultingfromtheunavoidablesurfacereconstructionduringtheoxygenevolutionreaction(OER).Thisstudyintroducesanewlydevelopedcatalyst,namelynickel–cobaltphosphidenanowires(NiCoP),whichfacilitatesthein-situgrowthofnickel–cobaltoxide(NiCo2O4)throughsurfacereconstructionduringanodicpotentialcyclinginalkalineelectrolytes.Thecatalyst’sextensivemodificationcanbeobservedthroughex-situcharacterizationtechniques.Thecatalystundergoesasignificanttransformationthatultimatelyyieldsaphosphidescaffold,leadingtotheformationofaspineloxidesurface.ThistransformationenhancesthecatalyticenvironmentfortheOER,makingithighlyefficientandpotent.ThetransformedcatalystdemonstratescomparablecatalyticperformancetothepreciousRuO2catalystacrossvariouscurrentdensities.Importantly,itexhibitsremarkablelong-termstability,asdemonstratedbyitsabilitytosustaincontinuousoperationfor72hatacurrentdensityof50mAwhilemaintainingstablecatalyticperformance.","container-title":"JournalofElectroanalyticalChemistry","DOI":"10.1016/j.jelechem.2023.117928","ISSN":"15726657","journalAbbreviation":"JournalofElectroanalyticalChemistry","language":"en","page":"117928","source":"DOI.org(Crossref)","title":"Nickel-cobaltphosphidenanowiresasprecatalystsforsurfacereconstructiontopreparedurableandefficientOERcatalysts","volume":"952","author":[{"family":"Cao","given":"Qingbin"},{"family":"Su","given":"Wenxiao"},{"family":"Liu","given":"Haorui"},{"family":"Feng","given":"Chenchen"},{"family":"Zhou","given":"Qi"}],"issued":{"date-parts":[["2024",1]]}},"label":"page"},{"id":555,"uris":["/users/10605487/items/N5UEZJ7N"],"itemData":{"id":555,"type":"article-journal","abstract":"Iron(Fe)promotesthesurfacereconstructionofNiPS\n3\nevenatlowerpotentialfortheNi\n\nx\n\nFe\n\n1?\nx\n\nPS\n3\nOERelectrocatalyst.ThesurfacereconstructedamorphouslayerscanefficientlyactasrealcatalyticactivesitesfortheOER.\n\n,\n\nSurfaceself-reconstructionofoxygenevolutionreaction(OER)electrocatalystsgenerallyoccursduringtheelectrochemicalactivationprocess.Herein,westudythesurfaceself-reconstructionofa2DlayeredFe-dopedNi-thiophosphate(Ni\n\nx\n\nFe\n\n1?\nx\n\nPS\n3\n)nanosheet.TheroleofFeinthesurfaceself-reconstructionofNiPS\n3\nduringtheOERisinvestigatedbyusingan\ninsitu\nRamananalysis.Formationofamorphousmetal/non-metaloxidelayersonthesurfaceofNi\n\nx\n\nFe\n\n1?\nx\n\nPS\n3\ncanefficientlyactastheultimatecatalyticcenterfortheOER.","container-title":"ChemicalCommunications","DOI":"10.1039/D3CC01510F","ISSN":"1359-7345,1364-548X","issue":"60","journalAbbreviation":"Chem.Commun.","language":"en","page":"9247-9250","source":"DOI.org(Crossref)","title":"Unravelingthesurfaceself-reconstructionofFe-dopedNi-thiophosphateforefficientoxygenevolutionreaction","volume":"59","author":[{"family":"Kirubasankar","given":"Balakrishnan"},{"family":"Won","given":"YoSeob"},{"family":"Choi","given":"SooHo"},{"family":"Kim","given":"JaeWoo"},{"family":"Adofo","given":"LaudAnim"},{"family":"Kim","given":"SooMin"},{"family":"Kim","given":"KiKang"}],"issued":{"date-parts":[["2023"]]}},"label":"page"}],"schema":"/citation-style-language/schema/raw/master/csl-citation.json"}1–4。大因素可引起預催化劑重構，一是催化過程電壓變化，二是測試條件變化ADDINZOTERO_ITEMCSL_CITATION{"citationID":"i45wfktX","properties":{"formattedCitation":"\\super5\\nosupersub{}","plainCitation":"5","noteIndex":0},"citationItems":[{"id":542,"uris":["/users/10605487/items/WZJ8QHXF"],"itemData":{"id":542,"type":"article-journal","abstract":"Abstract\nReconstructioninducedbyexternalenvironment(suchasappliedvoltagebiasandtestelectrolytes)changescatalystcomponentandcatalyticbehaviors.Investigationsofcompletereconstructioninenergyconversionrecentlyreceiveintensiveattention,whichpromotethetargeteddesignoftop‐performancematerialswithmaximumcomponentutilizationandgoodstability.However,theadvantagesofcompletereconstruction,itsdesignstrategies,andextensiveapplicationshavenotachievedtheprofoundunderstandingsandsummariesitdeserves.Here,thisreviewsystematicallysummarizesseveralimportantadvancesincompletereconstructionforthefirsttime,whichincludes1)fundamentalunderstandingsofcompletereconstruction,thecharacteristicsandadvantagesofcompletelyreconstructedcatalysts,andtheirdesignprinciples,2)typesofreconstruction‐involvedprecatalystsforoxygenevolutionreactioncatalysisinwidepHsolution,andoriginsoflimitedreconstructiondegreeaswellasdesignstrategies/principlestowardcompletereconstruction,3)completereconstructionfornovelmaterialsynthesisandotherelectrocatalysisfields,and4)advancedinsitu/operandoormultiangle/levelcharacterizationtechniquestocapturethedynamicreconstructionprocessesandrealcatalyticcontributors.Finally,theexistingmajorchallengesandunexplored/unsolvedissuesonstudyingthereconstructionchemistryaresummarized,andanoutlookforthefurtherdevelopmentofcompletereconstructionisbrieflyproposed.Thisreviewwillarousetheattentiononcompletereconstructionmaterialsandtheirapplicationsindiversefields.","container-title":"AdvancedMaterials","DOI":"10.1002/adma.202007344","ISSN":"0935-9648,1521-4095","issue":"32","journalAbbreviation":"AdvancedMaterials","language":"en","page":"2007344","source":"DOI.org(Crossref)","title":"ComprehensiveUnderstandingsintoCompleteReconstructionofPrecatalysts:Synthesis,Applications,andCharacterizations","title-short":"ComprehensiveUnderstandingsintoCompleteReconstructionofPrecatalysts","volume":"33","author":[{"family":"Liu","given":"Xiong"},{"family":"Meng","given":"Jiashen"},{"family":"Zhu","given":"Jiexin"},{"family":"Huang","given":"Meng"},{"family":"Wen","given":"Bo"},{"family":"Guo","given":"Ruiting"},{"family":"Mai","given":"Liqiang"}],"issued":{"date-parts":[["2021",8]]}}}],"schema":"/citation-style-language/schema/raw/master/csl-citation.json"}5。這里我們主要研究電壓的改變，通過CV測量實現(xiàn)電化學活化和重建。催化劑經(jīng)過活化后進行表面重構，表面不可避免地會形成含氧中間體。在原始催化劑的表面上原位生成無定形或者低結(jié)晶活性的催化物種通常被用作真實催化物質(zhì)所對應的氧化物或者氫氧化物ADDINZOTERO_ITEMCSL_CITATION{"citationID":"X4g8WmX8","properties":{"formattedCitation":"\\super6\\nosupersub{}","plainCitation":"6","noteIndex":0},"citationItems":[{"id":562,"uris":["/users/10605487/items/TWVP9DFP"],"itemData":{"id":562,"type":"article-journal","abstract":"NiFe(oxy)hydroxide(NiFeOOH)isrecognizedasahighlyactivenon-preciousmetalcatalystinalkalinewaterelectrolysisduetoitsexceptionalcatalyticproperties.Inthiswork,highvalencemolybdenum(Mo)isintroducedtoimprovetheelectronicstructureandenhancetheelectricalconductivityofNiFeOOHforoxygenevolutionreaction(OER).TheintroductionofMoresultsinaMo-dopedNiFeOOHcatalystwithasignificantlyreducedoverpotentialof205mVat10mA/cm2andaTafelslopeof31.7mV/dec,enablingstableoperationforupto170h.Bothempiricalexperimentandtheorysimulationsareemployedtogaininsightintothe3d-electroninteractionsbetweenmolybdenumandnickel(Ni),iron(Fe)inMo-dopedNiFeOOH.TheresultsindicatethatMo-dopingenhancesthevalencestatesofNiandFe,leadingtoashiftinthed-bandcenterofthebimetallicactivesites.ThismodificationaffectsthetransformationofMo-dopedNiFeOOHintotheγ-NiFeOOHactivephase.ThispotentcombinationlendscredencetoitspotentialsuitabilityandutilityinOERapplications.","container-title":"FrontiersinEnergy","DOI":"10.1007/s11708-024-0960-6","ISSN":"2095-1701,2095-1698","issue":"6","journalAbbreviation":"Front.Energy","language":"en","page":"850-862","source":"DOI.org(Crossref)","title":"ImpactofbimetallicsynergiesonMo-dopingNiFeOOH:InsightsintoenhancedOERactivityandreconstructedelectronicstructure","title-short":"ImpactofbimetallicsynergiesonMo-dopingNiFeOOH","volume":"18","author":[{"family":"Qu","given":"Jingkuo"},{"family":"Dong","given":"Yuchen"},{"family":"Zhang","given":"Tuo"},{"family":"Zhao","given":"Chang"},{"family":"Wei","given":"Liting"},{"family":"Guan","given":"Xiangjiu"}],"issued":{"date-parts":[["2024",12]]}}}],"schema":"/citation-style-language/schema/raw/master/csl-citation.json"}6。重構后所得催化劑催化性能有所改變，例如反應中活性位點和催化位點數(shù)目。在實際應用中，重建物種是否穩(wěn)定同樣可以帶動重建進行并對結(jié)果產(chǎn)生影響。在熱力學穩(wěn)定性方面，對應氧化物，氫氧化物或者氫氧化物在氧化條件下以最為穩(wěn)定。因活性物種生成較多而重構程度較深的催化劑一般會呈現(xiàn)強化催化性能目前，在工業(yè)電解水制氫的過程中，主要使用的催化劑是貴金屬OER催化劑（如IrO2或RuO2），這種催化劑存在著價格高昂和資源有限的問題，這對氫能的大規(guī)模生產(chǎn)和應用構成了障礙ADDINZOTERO_ITEMCSL_CITATION{"citationID":"jZ8hDmB3","properties":{"formattedCitation":"\\super7,8\\nosupersub{}","plainCitation":"7,8","noteIndex":0},"citationItems":[{"id":570,"uris":["/users/10605487/items/CY98KJSG"],"itemData":{"id":570,"type":"article-journal","abstract":"Intheprocessofoxygenevolutionreaction(OER)onperovskite,itisofgreatsignificancetoacceleratethehinderedlatticeoxygenoxidationprocesstopromotetheslowkineticsofwateroxidation.Inthispaper,afacilesurfacemodificationstrategyofnanometer-scaleironoxyhydroxide(FeOOH)clustersdepositingonthesurfaceofLaNiO\n3\n(LNO)perovskiteisreported,anditcanobviouslypromotehydroxyladsorptionandweakenNi-ObondofLNO.TheaboverelevantevidencesarewelldemonstratedbytheexperimentalresultsandDFTcalculations.TheexcellenthydroxyladsorptionabilityofFeOOH-LaNiO\n3\n(Fe-LNO)canobviouslyoptimizeOH\n-\nfillingbarrierstopromotelatticeoxygen-participatedOER(LOER),andtheweakenedNi-ObondofLNOperovskitecanobviouslyreducethereactionbarrierofthelatticeoxygenparticipationmechanism(LOM).Basedontheabovesynergisticcatalysiseffect,theFe-LNOcatalystexhibitsamaximumfactorof5catalyticactivityincreasesforOERrelativetothepristineperovskiteanddemonstratesthefastreactionkinetics(lowTafelslopeof42?mV?dec\n-1\n)andsuperiorintrinsicactivity(TOFsof~40O\n2\nS\n-1\nat1.60?Vvs.RHE).","container-title":"Research","DOI":"10.34133/2020/6961578","ISSN":"2639-5274","journalAbbreviation":"Research","language":"en","license":"/licenses/by/4.0/","page":"2020/6961578","source":"DOI.org(Crossref)","title":"BoostingLatticeOxygenOxidationofPerovskitetoEfficientlyCatalyzeOxygenEvolutionReactionbyFeOOHDecoration","volume":"2020","author":[{"family":"Zhao","given":"Jia-Wei"},{"family":"Li","given":"Cheng-Fei"},{"family":"Shi","given":"Zi-Xiao"},{"family":"Guan","given":"Jie-Lun"},{"family":"Li","given":"Gao-Ren"}],"issued":{"date-parts":[["2020",1]]}},"label":"page"},{"id":568,"uris":["/users/10605487/items/365A2RAN"],"itemData":{"id":568,"type":"article-journal","abstract":"Oxygenreductionreaction(ORR)andoxygenevolutioncreaction(OER)areimportantchemicalreactionsforarechargeablelithium–oxygenbattery(LOB).Recently,high-entropyalloysandoxideshaveattractedmuchattentionbecausetheyshowedgoodelectrocatalyticperformanceforoxygenevolutionreaction(OER)and/oroxygenreductionreaction(ORR).Inthisstudy,weaimedtosynthesizeandcharacterizeCoSn(OH)6andtwotypesofhigh-entropyperovskitehydroxides,thatis,(Co0.2Cu0.2Fe0.2Mn0.2Mg0.2)Sn(OH)6(CCFMMSOH)and(Co0.2Cu0.2Fe0.2Mn0.2Ni0.2)Sn(OH)6(CCFMNSOH).TEMobservationandXRDmeasurementsrevealedthatthehigh-entropyhydroxidesCCFMMSOHandCCFMNSOHhadcubiccrystalswithsidesofapproximately150–200nmandcrystalstructuressimilartothoseofperovskite-typeCSOH.LSVmeasurementresultsshowedthatthehigh-entropyhydroxidesCCFMMSOHandCCFMNSOHshowedbifunctionalcatalyticfunctionsfortheORRandOER.CCFMNSOHshowedbettercatalyticperformancethanCCFMMSOH.","container-title":"Materials","DOI":"10.3390/ma17122963","ISSN":"1996-1944","issue":"12","journalAbbreviation":"Materials","language":"en","license":"/licenses/by/4.0/","page":"2963","source":"DOI.org(Crossref)","title":"SynthesisofHigh-EntropyPerovskiteHydroxidesasBifunctionalElectrocatalystsforOxygenEvolutionReactionandOxygenReductionReaction","volume":"17","author":[{"family":"Chae","given":"Sangwoo"},{"family":"Shio","given":"Akihito"},{"family":"Kishida","given":"Tomoya"},{"family":"Furutono","given":"Kosuke"},{"family":"Kojima","given":"Yumi"},{"family":"Panomsuwan","given":"Gasidit"},{"family":"Ishizaki","given":"Takahiro"}],"issued":{"date-parts":[["2024",6,17]]}},"label":"page"}],"schema":"/citation-style-language/schema/raw/master/csl-citation.json"}7,8。因此，研發(fā)既高效又穩(wěn)定，且成本相對較低的非貴金屬催化劑變得尤為關鍵。鎳鐵氫氧化物是最具發(fā)展?jié)摿Φ膲A性OER電催化劑，然而由于原始鎳鐵氫氧化物的高活化能壘和有序電子構型，導致其電化學重構過程緩慢，重構產(chǎn)物數(shù)量有限且本征活性較低ADDINZOTERO_ITEMCSL_CITATION{"citationID":"ZjI8rDJp","properties":{"formattedCitation":"\\super9,10\\nosupersub{}","plainCitation":"9,10","noteIndex":0},"citationItems":[{"id":548,"uris":["/users/10605487/items/YA9ABSGG"],"itemData":{"id":548,"type":"article-journal","abstract":"NiFe-layereddoublehydroxides(NiFe-LDHs),aspromisingelectrocatalysts,havereceivedsignificantresearchattentionforhydrogenandoxygengenerationthroughwatersplitting.However,theslowoxidationkineticsofNiFe-LDH,duetothelimitednumberofactivesitesandthelowconductivity,hinderstheimprovementofthewater-splittingefficiency.Therefore,toovercometheobstacles,two-dimensional(2D)SnSwasfirstexploredtotailorthepreparedNiFe-LDHviathehydrothermalmethod.ANiFe-LDH/SnSheterojunctionisbuilt,whichisobservedfromthemicrostructuralinvestigations.SnSincorporationcouldgreatlyimprovetheconductivityoftheNiFe-LDHsheets,whichwasreflectedbythereducedchargetransferresistance.Moreover,SnSlayersmodulatedtheelectronicenvironmentaroundtheactivesites,favoringtheadsorptionofintermediatesduringtheoxygenevolutionreaction(OER)process,whichwasverifiedbydensityfunctionaltheorycalculations.AsynergisticeffectinducedbytheNiFe-LDH/SnSheterostructurepromotedtheOERactivitiesinelectrical,electronic,andenergeticaspects.Consequently,theas-preparedNiFe-LDH/SnSelectrocatalystgreatlyimprovedtheelectrocatalyticperformance,exhibiting20%and27%reductionsintheoverpotentialandTafelslopecomparedwiththoseofpristineNiFe-LDH,respectively.TheresultsprovideastrategyforregulatingNiFe-basedelectrocatalystsbyusingemerging2Dmaterialstoenhancewater-splittingefficiency.","container-title":"ACSAppliedMaterials&Interfaces","DOI":"10.1021/acsami.3c18458","ISSN":"1944-8244,1944-8252","issue":"18","journalAbbreviation":"ACSAppl.Mater.Interfaces","language":"en","license":"/licenses/by-nc-nd/4.0/","page":"23054-23060","source":"DOI.org(Crossref)","title":"Two-DimensionalSnSMediatesNiFe-LDH-LayeredElectrocatalysttowardBoostingOERActivityforWaterSplitting","volume":"16","author":[{"family":"Sun","given":"Yaxun"},{"family":"Cai","given":"Qingguo"},{"family":"Wang","given":"Ze"},{"family":"Li","given":"Zhichun"},{"family":"Zhou","given":"Qianyu"},{"family":"Li","given":"Xin"},{"family":"Zhao","given":"Dongye"},{"family":"Lu","given":"Jianfeng"},{"family":"Tian","given":"Shouqin"},{"family":"Li","given":"Yong"},{"family":"Wang","given":"Shifeng"}],"issued":{"date-parts":[["2024",5,8]]}},"label":"page"},{"id":546,"uris":["/users/10605487/items/WXS5F9M9"],"itemData":{"id":546,"type":"article-journal","abstract":"Theoxygenevolutionreaction(OER),whichinvolvesafour-electrontransferandslowkinetics,requiresanefficientcatalysttoovercomethehighenergybarrierforhigh-performancewaterelectrolysis.Inthispaper,anovelNi3S2@V-NiFe(III)LDH/NFcatalystwaspreparedviaafaciletwo-stephydrothermalmethod.TheconstructedheterostructureofNi3S2@V-NiFe(III)LDHincreasesthespecificsurfaceareaandregulatestheelectronicstructure.Furthermore,theintroductionoftheVelementformsanelectrontransportchainofNi-O-Fe-O-V-O-Ni,whichoptimizesthebindingenergybetweenmetalactivesitesandoxygenevolutionreactionintermediates,accelerateselectrontransfer,andimprovesself-reconstruction.Withthisdualregulationstrategy,Ni3S2@V-NiFe(III)LDH/NFexhibitsexceptionalOERperformancewithanoverpotentialof280mVat100mA/cm2andaTafelslopeof45.4mV/dec.Thisworkdevelopsadualregulationstrategycombiningheterostructureformationandthedopingeffect,whicharebeneficialinthedesignofefficientOERcatalysts.","container-title":"Molecules","DOI":"10.3390/molecules29246018","ISSN":"1420-3049","issue":"24","journalAbbreviation":"Molecules","language":"en","license":"/licenses/by/4.0/","page":"6018","source":"DOI.org(Crossref)","title":"ConstructionofHeterostructuredNi3S2@V-NiFe(III)LDHforEnhancedOERPerformance","volume":"29","auth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