NIMSAWARD2025-abstracts

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P1-3067Operando ToF-SIMS for Solid-state BatteriesSolid-statebatteries(SSBs)providehighersafetyandenergydensity,makingthempromisingfornext-generationenergystorage.However,interfacialdegradationcausedbymechanicalstressandchemicalsidereactionssuppresseslithiumtransportandactivematerialutilization.Therefore,developingtechniquestovisualizeelectrochemicalreactions,includinglithium-iontransport,isessentialtoelucidateandovercomeinterfaciallimitations.DetectedvariationsinLisignalintensitycorrespondingtocharge–dischargereactions.Observedchangesintheintensityoftransitionmetalionsduringcharge–dischargeprocesses.Identifiedelectrochemicalinhomogeneityrelatedtotheelectrodestructure.ConclusionOxide-type solid-state batteryToF-SIMS imagingFutureIntroductionTime-of-FlightSecondaryIonMassSpectrometry(ToF-SIMS)isapowerfultechniqueforanalyzingbatterydegradation.Itenablesdirectdetectionoflightelements,suchaslithium,andmultipleobservationsofchemicalfragments,allowingfortheevaluationofchemicalstatechangesduringchargeanddischargeprocesses.Inthisstudy,weconductedoperandoToF-SIMSanalysisofSSBstoinvestigatespectralandimagingvariationsduringoperation.OperandoToF-SIMSSolid State Battery Ionics Group, GREEN / Gen HasegawaE-mail: HASEGAWA.Gen@nims.go.jpKey Words: Solid-state Battery, ToF-SIMSSample•SEM image•Operando SIMS holder0510152025300.00.51.01.52.02.53.03.5Voltage / VCapacity / μAhCharge-discharge curves during SIMS20 μmImaging area of cathodeImaging area of anodeCathode: LiNi0.8Co0.15Al0.05O2SE: Li2OHCl0.9F0.1+ Li0.31La0.56TiO3Anode: Li4Ti5O12 16842Log(Intensity / a.u.)Before chargeCharge 300 minDischarge 300 min48Ti+48Ti+48Ti+3321684216432168412Log(Intensity / a.u.)Log(Intensity / a.u.)1122Before chargeCharge 300 minDischarge 300 min6Li+58Ni+6Li+58Ni+6Li+58Ni+•Cathode•Anode01002003004005006007000369121518 Region 1 Region 2Intensity / counts pixel–1Time / minChargeDischarge6Li+010020030040050060070005101520253035 Region 1 Region 2Intensity / counts pixel–1Time / minChargeDischarge58Ni+01002003004005006007000369121518 Region 3Intensity / counts pixel−1Time / minChargeDischarge48Ti+Side reaction (LLTO)Reversible (LTO)Irreversible (NCA)Diffusion (NCA)Reversible (NCA)•Detectedvariationsin6Li+signalintensitycorrespondingtochangesinlithiumconcentrationduringcharge–dischargecycles.•Observedintensitychangesoftransitionmetalionssuchas58Ni+and48Ti+associatedwithelectrochemicalreactions.•Inthecathode,fragmentationofsecondaryparticlesfacilitatedfurtherprogressionoftheelectrochemicalreaction.Investigatetherelationshipbetweenbatterydegradationandsecondaryionintensity.Developoperandomeasurementtechniquescombinedwithisotopediffusionanalysis.Designnext-generationsolid-statebatteriesthroughinsightsobtainedfromvisualizationanalysis.Charge: 6 μA, 3.3 V cutDischarge: −6 μA, 0.3 V cutElectrode materialsElectrochemical measurement conditions