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US 9,905,856 B1 12 odepreparedviatheconventionalmethodwithoutdelami activematerials(thoseresponsibleforstoringNaorLiions) nationandcrackingandthosebythepresentlyinvented withoutincreasingtheamountsofalnon-activematerials method. DESCRIPTIONOFTHEPREFERRED EMBODIMENTS (e.g.curentcolectorsandseparator)inordertoobtain a minimum overheadweightandamaximum sodium storage 5 capabilityand,hence,amaximizedenergydensity(Wk/kg orWh/Lofcel). Inalescommonlyusedcelconfiguration,asilustrated Thisinventionisdirectedataflexibleandshape-con- inFIG.1(A),eithertheanodeactivematerial(e.g.NaTi, formablerope-likealkalimetal-sulfurbateryexhibitingan (PO2),orNafilm)orthecathodeactivematerial(e.g. exceptionalyhighvolumetricenergydensityandhighgra-10lithium transitionmetaloxideinaLi-ioncelorsulfur/ vimetricenergydensity.Thisdoesnotincludetheso-caled carbonmixtureinaLi-Scel)isdepositedinathinfilm high-temperatureNa-Scelthatmustoperateatatempera- formdirectlyontoacurentcolector,suchasashetof turehigherthanthemeltingpointoftheelectrolyte(typi- copperfoilorAlfoilusingsputering.However,suchathin caly>350°C.)andhigherthanthemeltingpointofsulfur. filmstructurewithanextremelysmalthicknes-direction Theinventedalkalimetal-sulfurbaterycanbeaprimary15dimension(typicalymuch smallerthan50nm,often batery,butispreferablyasecondarybateryselectedfrom necesarilythinerthan10nm)impliesthatonlyasmall analkalimetal-ionbatery(e.g.usingaLiorNaintercala- amountofactivematerialcanbeincorporatedinanelec tioncompound,suchashardcarbonparticles)oranalkali trode(giventhesameelectrodeorcurrentcollectorsurface metal-sulfursecondarybatery(e.g.usingNaorLimetalfoil area),providingalowtotalNaorListoragecapacityperunit as an anode active material). The battery is based on an 20 electrode surface area.Such a thin film must have a thick aqueouselectrolyte,anon-aqueousororganicelectrolyte,a nesslesthan100nmtobemoreresistanttocycling gelelectrolyte,anionicliquidelectrolyte,oramixtureof inducedcracking(fortheanode)ortofacilitateaful organicandionicliquid.Apolymercanbeadedtothese utilizationofthecathodeactivematerial.Suchaconstraint electrolytestoformagel.Theelectrolytedoesnotinclude furtherdiminishesthetotalNaorListoragecapacityandthe thesolid-stateelectrolyte. 25 sodium orlithium storagecapacityperunitelectrodesurface AsilustratedinFIG.1(A)andFIG.1(B),aconventional area.Suchathin-filmbateryhasverylimitedscopeof lithium-ion,sodium-ion,Li—S,orNa-Sbaterycelis aplication. typicalycomposedofananodecurentcolector(e.g.Cu Ontheanodeside,asputeredNaTiz(PO4)3layerthicker foil),ananodeelectrode(anodeactivemateriallayer),a than10nmhasbeenfoundtoexhibitpoorcracking porousseparatorand/oranelectrolytecomponent,acathode 30 resistanceduringbattery charge/discharge cycles.Ittakes electrode(cathodeactivemateriallayer),andacathode butafewcyclestogetfragmented.Onthecathodeside,a curentcolector(e.g.Alfoil).Inamorecommonlyusedcel layerofsulfurthickerthan10nmdoesnotalowlithiumor configuration(FIG.1(B),theanodelayeriscomposedof sodiumionstofulypenetrateandreachfulbodyofthe particlesofananodeactivematerial(e.g.hardcarbon cathodelayer,resultinginapoorcathodeactivematerial particles),aconductive aditive (e.g.expanded graphite 35 utilizationrate.Adesirableelectrodethicknesisatleast100 flakes),andaresinbinder(e.g.SBRorPVDF).Thecathode um (not100nm),withindividualactivematerialparticle layeriscomposedofparticlesofacathodeactivematerial havingadimensiondesirablylesthan10nm.Thus,these (e.g.NaFePO4particlesinaNa-ioncelorS-carboncom- thin-filmelectrodes(withathicknes<10nm)directly positeparticlesinaLi-Scel),aconductiveaditive(e.g. depositedonacurentcolectorfalshortoftherequired carbonblackparticles),andaresinbinder(e.g.PVDF).Both 40thicknesbythre(3)ordersofmagnitude.Asafurther theanodeandthecathodelayersaretypicaly60-10um problem,alofthecathodeactivematerialsarenotvery thick(typicalysignificantlythinerthan20um)togive conductivetobothelectronsandsodium/lithiumions.A risetoapresumablysuficientamountofcurentperunit largelayerthicknesimpliesanexcesivelyhighinternal electrodearea.Usinganactivemateriallayerthicknesof resistanceandapooractivematerialutilizationrate. 10umandthesolid(CuorAlfoil)curentcolectorlayer45 Inotherwords,thereareseveralconflictingfactorsthat thicknesof10umasexamples,theresultingbaterycon- mustbeconsideredconcurentlywhenitcomestothedesign figurationhasacurentcolectorthicknes-to-activemate andselectionofacathodeoranodeactivematerialinterms riallayerthicknesratioof10/10or1/10forconventional ofmaterialtype,size,electrodelayerthicknes,andactive baterycels. materialmassloading.Thusfar,therehasbeennoefective Thisthicknesrangeof60-100um isconsideredan50solutionoferedbyanypriorartteachingtotheseoften industry-acceptedconstraintunderwhichabaterydesigner conflictingproblems.Wehavesolvedthesechallenging normallyworksunder,basedonthecurentslurycoating isues,whichhavetroubledbaterydesignersandelectro process(rolcoatingofactivematerial-binder-additivemix- chemistsalikeformorethan30years,bydevelopinganew tureslury).Thisthicknesconstraintisduetoseveral procesofproducingalkalimetal-sulfurbateriesasherein reasons:(a)theexistingbateryelectrodecoatingmachines 5disclosed. arenotequipedtocoatexcesivelythinorexcesively Thepriorartsodium orlithiumbaterycel,including thickelectrodelayers;(b)athinerlayerispreferedbased Li—SandroomtemperatureNa-Scel,istypicalymade ontheconsiderationofreducedlithiumiondifusionpath byaprocessthatincludesthefollowingsteps:(a)Thefirst lengths;but,tothinalayer(e.g.<60um)doesnotcontain stepismixingparticlesoftheanodeactivematerial(e.g. a sufficientamount of an active alkalimetal ion storage 60 hard carbon particles),a conductive filer (e.g.expanded material(hence,insuficientcurrentoutput);(c)thicker graphiteflakes),aresinbinder(e.g.PVDF)inasolvent(e.g. electrodesarepronetodelaminateorcrackupondryingor NMP)toformananodeslury.Onaseparatebasis,particles handlingafterrol-coatingofslury;and(d)thickercoating ofthecathodeactivematerial(e.g.sodiummetalphosphate requiresanexcesivelylongheatingzone(itisnotunusual particlesfortheNa-ioncelandLFPparticlesfortheLi-ion tohaveaheatingzonelongerthan10meters,makingthe65cel),aconductivefiler(e.g.acetyleneblack),aresinbinder manufacturingequipmentveryexpensive).Thisconstraint (e.g.PVDF)aremixedanddispersedinasolvent(e.g.NMP) hasmadeitimposibletofrelyincreasetheamountof toformacathodeslury.(b)ThesecondstepincludesPDF Image | FLEXIBLE AND SHAPE-CONFORMAL ROPE-SHAPE ALKALI METAL-SULFUR BATTERIES
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