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5 6 US 10,991,944B2 gammaphasesulfurusingPDXLVersion2.8.4.0Integrated ments,theanodeincludesanactivematerialselectedfrom PowderDifractionSoftware;monoclinicgammaphase lithium,sodium,potasium,magnesium,calcium,zinc,cop sulfurorientedinthekdirection,andmonoclinicsulfurthat per,titanium,nickel,cobalt,iron,oraluminum. bestmatchesmonoclinicgammaphasesulfurorientedinthe Ineachoftheforegoingembodimentsofthecel,thecel kdirectionusingPDXLVersion2.8.4.0IntegratedPowder 5 maybealithium-sulfurcel,asodium-sulfurcel,apotas DifractionSoftware. sium-sulfurcel,amagnesium-sulfurcel,andacalcium Inasecondaspect,thepresentinventionrelatestoa sulfurcel. cathodewhichmay,forexample,bepreparedbyanyofthe Ineachoftheforegoingembodimentsofthecel,thecel foregoingmethods. mayexhibitasingleplateaudischargecurvewithadis Inanotheraspect,thepresentinventionrelatestoa10chargecapacityoffrom300mAh/gtoabout170mAh/g, cathodeincludingmonoclinicphasesulfurthatisstableata orfromabout400mAh/gtoabout1300mAh/g,orfrom temperaturebelow80°C.locatedonasubstratewhichmay about600mAh/gtoabout10mAh/g,orfromabout750 beaporousmaterial.Inthisembodiment,themonoclinic mAh/gto90mAh/g,or80mAh/gafter10cyclesata phasesulfurmayoptionalybedepositedonthesubstrateby C/2rate,albasedonatotalweightofthesulfurinthe vapordeposition. 15cathode,orthecelexhibitsasingleplateaudischargecurve Ineachoftheforegoingembodiments,themonoclinic withadischargecapacityoffromabout30mAh/gtoabout phasesulfurmaycompriseaformofsulfurselectedfromthe 3000mAh/g,orfromabout400toabout2500mAh/gafter groupconsistingofmonoclinicgammaphasesulfur;mono- afirstcycleataC/10rate,albasedonatotalweightofthe clinicsulfurthatbestmatchesmonoclinicgammaphase sulfurinthecathode. sulfurusingPDXLVersion2.8.4.0IntegratedPowderDif-20 Ineachoftheforegoingembodimentsofthecel,thecel fractionSoftware;monoclinicgammaphasesulfuroriented mayhaveadischargecapacityoffromabout10mAh/gto inthekdirection,andmonoclinicsulfurthatbestmatches about1500mAh/g,orfromabout400mAh/gtoabout1200 monoclinicgammaphasesulfurorientedinthekdirection mAh/g,orfromabout600mAh/gtoabout900mAh/g,or usingPDXLVersion2.8.4.0IntegratedPowderDifraction fromabout650mAh/gto750mAh/g,after130cyclesat Software;monoclinic cyclo-hexa-cyclo-deca sulfurand25aC/2rate,albasedonatotalweightofthesulfurinthe monoclinicsulfurthatbestmatchestocyclo-decasulfur- cathode. cyclo-hexasulfurusingthePDXLVersion2.8.4.0Integrated Ineachoftheforegoingembodimentsofthecel,thecel PowderDiffractionSoftware. maybearechargeablecel. Ineachoftheforegoingembodimentsofthecathode,the Ineachoftheforegoingembodimentsofthecel,thecel substratemay beconductive,non-conductive,andmay 30mayincludeacurentcolector. comprisecarbonnanofiberssuchasamatofcarbonnano- Inanotheraspect,thepresentinventionrelatestoasulfur fibersorfre-standingcarbonnanofibers. bateryincludingapluralityofthesulfurcelsasdescribed Ineachoftheforegoingembodimentsofthethode,the ineachoftheforegoingembodiments. cathodemayhaveaninitialdischargecapacityinarangeof Ineachoftheembodimentsofthesulfurbatery,the fromabout30mAh/gtoabout250mAh/g,orfromabout35sulfurbaterymayincludeporousseparator,wherethe 350mAh/gtoabout2000mAh/g,orfromabout375mAh/g separatorisprovidedbetwenananodicsectionanda toabout170mAh/g,orfromabout400mAh/gtoabout cathodicsectionofthebatery.Theporousseparatormaybe 130mAh/g,orfromabout60mAh/gtoabout10 selectedfromaporouspolypropylenemembrane,coton, mAh/g,orfromabout750mAh/gto900mAh/g,or800 nylon,polyesters,glasfiber,polyethylene,poly(tetrafluo mAh/g,basedonatotalweightofsulfurinthecathode. 40roethylene,polyvinylchloride,anodicaluminumoxide Ineachoftheforegoingembodimentsofthecathode,the (AAO)andruber. cathodemayincludeacathodecurentcolector. Thepresentinventionprovidesbothanovelmaterialfor Ineachoftheforegoingembodimentsofthecathode,the useinthecathodeofasulfurcelorbaterynamely,a cathodemayhaveamonoclinicphasesulfurloadingina monoclinicphasesulfurthatisstableatatemperaturebelow rangeofatleast0.05mg/cm2,oratleast0.5mg/cm2from4580°C.,suchasamonoclinicgammaphasesulfur,anda about1.0mg/cm2toabout150.0mg/cm2orfromabout5.0 novelaproachthatdoesnotrequireconfinementofthe mg/cm2toabout125mg/cm2,orfromabout10mg/cm2to sulfurinsuchsulfurbateries.Themonoclinicphasesulfur wassynthesizedanddepositedusingvapordepositiononthe Ineachoftheforegoingembodimentsofthecathode,the surfaceofasubstratewhichmaybeaporousmaterial substratemaybeaporousmaterialhavingaporevolumeof50includingcarbonnanofiberssuchasamatofcarbonnano 10-95%,measuredafterthemonoclinicphasesulfuris fibersorfre-standingcarbonnanofibers. presentonthecathode. Frestandingcarbonnanofibersdepositedwithgamma Inanotheraspect,theinventionrelatestoasulfurcel monoclinicphasesulfurelectrodes:(a)alowuseofcarbon includinganyoneoftheforegoingembodimentsofthe ate-basedelectrolytes,(b)yieldasolidtosolidtransitionand cathode,ananode,andanelectrolyte.Theelectrolytemay 5therebyavoidingpolysulfideformation,(c)formastabilized beacarbonateelectrolyte.Thecarbonateelectrolytemaybe gammaphasethatremainsstableforlongperiodsinambient selectedfromethylenecarbonate,dimethylcarbonate, air,(d)eliminatetheneedforthedeadweightofbindersand methylethylcarbonate,diethylcarbonate,propylenecarbon- colectors,(e)maintainconductivecarbonchalengesfor ate,vinylenecarbonate,alylethylcarbonate,andmixtures beterelectronpathways,and(f)provideexcelentmechani thereof.Preferably,ineachoftheforegoingembodimentsof60calstabilityduringcycling.Further,themethodofforming/ thesulfurbatery,thecarbonateelectrolytemaybeselected depositingthegammamonoclinicphasesulfurcanbe fromethylenecarbonate,diethylcarbonate,propylenecar- employedforlarge-scaledevelopmentofgammaphaseand bonateandmixturesthereof. itsuseinsulfurbateries. Ineachoftheforegoingembodimentsofthecel,the Aditionaldetailsandadvantagesofthedisclosurewilbe anodemaybeanionreservoirincludinganactivematerial65setforthinpartinthedescriptionwhichfolows,and/ormay selectedfromalkalimetals,alkalineearthmetals,transition belearnedbypracticeofthedisclosure.Thedetailsand metals,graphite,aloys,andcomposites.Insomeembodi- advantagesofthedisclosuremayberealizedandatainedby about15mg/cm2.PDF Image | SYNTHESIS OF GAMMA MONOCLINIC SULFUR
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