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1、oACSAutfittCHceCHEMISTRYOFMATERIALSArticlepubs.acs.org/cmThisisanopenaccessarticlepublishedunderanACSAuthorChoiceLicense,whichpermitscopyingandredistributionofthearticleoranyadaptationsfornon-commercialpurposes.InterfaceStabilityinSolid-StateBatteriesWilliamD.Richards/LincolnJ.Miara/YanWang/JaeChuiK
2、im/andGerbrandCeder*的DepartmentofMaterialsScienceandEngineering,MassachusettsInstituteofTechnology,Cambridge,Massachusetts02139,UnitedStatestSamsungAdvancedInstituteofTechnology-USA,255MainStreet,Suite702,Cambridge,Massachusetts02142,UnitedStatesnDepartmentofMaterialsScienceandEngineering,University
3、ofCalifornia,Berkeley,California94720,UnitedStatesMaterialsSciencesDivision,LawrenceBerkeleyNationalLaboratory,Berkeley,California94720,UnitedStates*SupportingInformationABSTRACT:Developmentofhighconductivitysolid-state(lectrolytesforrecentyears,butincorporatingthesenewmaterialsintohighfrfonkingbatt
4、isnowthelimitingfactorinmanysystems,buttheexactm(ghaidLmspartbecauseexperimentalevaluationoftheinterfacecanImethodologytoexaminethethermodynamicsofformationcresistiveformationiswellcorrelatedwithexperimentalinterfacialthiophosphateelectrolyteshaveespeciallyhighreactivitywitlwindow.Wealsofindthatanum
5、berofknownelectrolytesaformpassivatingbutionicallyconductingbarrierlayers.AsexpecteddecompositionproductsfbrawiderangeofelectnABSTRACT:Developmentofhighconductivitysolid-state(lectrolytesforrecentyears,butincorporatingthesenewmaterialsintohighfrfonkingbattisnowthelimitingfactorinmanysystems,buttheex
6、actm(ghaidLmspartbecauseexperimentalevaluationoftheinterfacecanImethodologytoexaminethethermodynamicsofformationcresistiveformationiswellcorrelatedwithexperimentalinterfacialthiophosphateelectrolyteshaveespeciallyhighreactivitywitlwindow.Wealsofindthatanumberofknownelectrolytesaformpassivatingbution
7、icallyconductingbarrierlayers.Asexpecteddecompositionproductsfbrawiderangeofelectn11ionbatterieshasproceededrapidlyinasprfvendifficult.InterfacialresistanceedinjgnalasepqhisHesistenifictavenotbeenIllgllVOlTc3notinhereferenceficiilt.liVtlyintprfacialp涵冒dhitlystableice顽experim55，右,5Uworlascs.er;inTher
8、firalambutnact:its,mtali争hilly-ex)acom1intcrfac,wedevelo)predicteoweiecttxinsituwiththeele晦wetabulaethestaljffiyand)detoXThigh-performingcombinationsthathavenotyetbeenattemptedexperimentally.soo-eepoqs=qnd8eqsA-3elu=-5i)。一2Moqcosuo=doSO.SOP3曾u-ceqsaO.SOB.Sqndsd=q8S(am)快0w6一角Z一oqoaou。06一一0一.ZJ.SO【.2A
9、popeoeMOCI2015AmericanChemicalSociety0INTRODUCTIONSolid-stateelectrolyteshavethepotentialtodramaticallyimprove-sa花ty-artd-perfdrmanee-。仁state。但the-aitbattery一technology.Thehighenergydensityandlongcyclelifeoflithium-ionbatterieshasledtotheiradoptioninallmanneroftechnologies,butserioussafetyconcernsst
10、illexistduetotheiruseofflammableorganicsolventelectrolytes.Thisisespeciallyproblematicfbrgrid-scalestorageandtransportapplicationsincludingaircraftandautomobiles.Solid-stateionicelectrolytematerialsareaviablenonflammablealternative,wouldenablenoveldevicegeometriestoimprovepackingefficiencyofthecells
11、,andhavethepotentialtoimprovecyclelifeandenablehighervoltagecathodes.1Bysuppressingdendriteformation,solidelectrolytesmayalsoallowtheuseofmetalanodeswhichwouldincreaseenergydensityconsiderably.DevelopmentofLi-ionsolidelectrolyteshasproceededrapidlyinrecentyears,withtheconductivityofsomesystemsevenap
12、proachingandsurpassingthatofliquidelectrolytes.Roomtemperatureconductivitiesofaround1mScm-1havebeenshowninNASICON-typeoxides2-4andlithiumgarnets.Thesesystemstypicallyrequirehighsynthesistemperatures8andcosinteringtoobtaingoodcontactbetweentheelectrodeandelectrolyte,9whichisimportantforbatteryperform
13、ance.10,11NewthiophosphatematerialsbasedonLiaPS/haverecentlyemergedasanovelclassofsuperionicconductingmaterialswithevenhigherconductivitiesandwhosemechanicalACSPublicationspropertiesallowbetterphysicalcontactwithelectrodes.TheseincludeLiioGeP2S12(LGPS),withaconductivityof12mScm-1atroomtemperature,13
14、andU7P3S11,aglass-ceramicwitharoomtemperatureconductivityof27mScm_1.14LessexpensiveversionsofLGPSwhereGeisreplacedbySnor1516-19havealsobeenpredictedandsynthesized.Despitethisprogressinachievinghighbulkconductivity,theratecapabilityofmostall-solid-statecells,particularlythoseemployinghigh-voltageoxid
15、ecathodes,remainspoor.-0,21Thisistypicallyascribedtohighinternalresistanceattheinterfaces,buttheexactmechanismsbywhichthisresistancebuildshavebeendifficulttoascertainexperimentally.Chemicalincompatibility,electrochemicalreaction,andmechanicalissuesmayallplayaroleindegradingbatteryperformance.Coating
16、theelectrodeswithanoxidebarrierlayerhasbeennecessarytosuppressdevelopmentofextremeinterfacialresistanceandenablehigh-ratecycling,13,16,22,23butmanyofthesecellsstillseesignificantdegradationafterrelativelyfewcycles.Thefutureofsolid-statebatteriesdependsonengineeringbetterinterfacestoallowhighratecapabilityandextendedcyclelifeinthisnewgenerationofbatteries.Theexperimentalinvestigat
