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1、ResearchArticlewww.acsami.orgSpectrum-DependentSpiro-OMeTADOxidizationMechanisminPerovskiteSolarCells†‡,†ShenWang,WenYuan,andYingShirleyMeng*†DepartmentofNanoEngineering,UniversityofCaliforniaSanDiego,9500GilmanDrive,LaJolla,California92093,UnitedStates‡DepartmentofChemistry,MichiganStateU
2、niversity,EastLansing,Michigan48824,UnitedStates*SSupportingInformationABSTRACT:Weproposeaspectrum-dependentmechanismfortheoxidationof2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9′-spirobifluorene(Spiro-OMeTAD)withbis-(trifluoromethane)sulfonimidelithiumsalt(LiTFSI),whichiscommonlyuse
3、dinperovskitesolarcellsastheholetransportlayer.TheperovskitelayerplaysdifferentrolesintheSpiro-OMeTADoxidizationforvariousspectralranges.TheeffectofoxidizedSpiro-OMeTADonthesolarcellperformancewasobservedandcharacterized.Withtheinitiallong-wavelengthillumination(>450nm),thechargerecombinatio
4、nattheTiO2/Spiro-OMeTADinterfacewasincreasedduetothehigheramountoftheoxidizedSpiro-OMeTAD.Ontheotherhand,theincreasedconductivityoftheSpiro-OMeTADlayerandenhancedchargetransferattheAu/Spiro-OMeTADinterfacefacilitatedthesolarcellperformance.KEYWORDS:chargerecombination,perovskitesolarcells,
5、solidstate,p-doping,spectrum,impedancespectroscopy1.INTRODUCTIONtheliquid-basedelectrolyte,whichcandissolvetheperovskitelayer,thesmallorganicmoleculeSpiro-OMeTAD,showninHybridorganic−inorganicperovskitesolarcells(PSCs)haveFigure1a,isnonreactivetoperovskiteandislessvolatile.Thegainedincreas
6、ingattentionasintriguingcandidatesfornext-1matchedbandgapwithperovskite,amorphousnature,goodgenerationphotovoltaicdevicessince2010.Recently,20.1%conductivitywithdopants,andhighmeltingpointforSpiro-powerconversionefficiencyhasbeenachievedthrough2OMeTADmakeitoneofthemostadaptableHTMsinintramol
7、ecularexchangereaction.Inadditiontohigh14−17PSCs.Recentresearchdemonstratesthata>400nmefficiencies,PSCsareall-solid-statedeviceswithlowcost,athicknessofSpiro-OMeTADHTMlayercanguaranteeatunablebandgap,andascalablefabricationprocess,indicating3−8higheropen-circuit