文档名：质子陶瓷电池氧电极材料设计及稳定性研究进展
摘要：质子陶瓷电池(PCCs)可广泛用于发电、储能和可持续化学合成等研究领域,其工作温度适中、效率高,具有广阔的应用前景.然而,在中低温时,PCCs氧电极的氧析出反应(OER)和氧还原反应(ORR)动力学缓慢,材料稳定性差,导致其难以高效、稳定地运行.因此,设计和开发活性高、稳定性良好的氧电极对促进PCCs技术的发展至关重要.本工作探讨了PCCs氧电极的材料组分、结构与电化学性能之间的关系,重点阐述了影响氧电极材料稳定性的因素,分别讨论了电解质-氧电极界面,氧电极在高湿度、含CO2气氛和含Cr气氛下的稳定性,以及抑制其衰减的策略,并就氧电极材料设计及未来发展方向进行了展望.
Abstract：Protonceramiccells(PCCs)arewidelyinvestigatedasdevicesforpowergeneration,energystorage,andsustainablechemicalsynthesisbecauseoftheirmoderateoperatingtemperature,highefficiencyandgreatapplicationprospects.Nevertheless,amainchallengeforoxygenelectrodeofPCCsremainsthesluggishkineticsoftheoxygenreductionreaction(ORR)andoxygenevolutionreaction(OER)atintermediateandlowertemperaturesaswellastheinsufficientstabilityoftheoxygenelectrodematerialsintheoperatingenvironment.Designinganddevelopinghigh-performanceanddurableoxygenelectrodesisthuscrucialforpromotingtheindustrialapplicationofPCCstechnology.Thisreviewdiscussedtherelationshipsamongcomposition,structureandelectrochemicalperformanceofoxygenelectrodematerialsandsummarizedthefactorsthatimpactthestabilityofoxygenelectrode.Thestabilityofelectrolyteandoxygenelectrodeinterfaceunderhighsteamcondition,CO2atmosphereandCratmospherewasdiscussed.Inaddition,afutureresearchinoxygenelectrodestabilitywasalsoproposed.Theelementaryreactionsattheoxygenelectrodeincludeoxygenadsorptionanddissociation,charge/oxygen/protontransfer,aswellaswaterformationandexhaust.Itisconsideredthatprotonscanplayacriticalroleinthereactionprocessontheoxygenelectrodeinadditiontoelectronsandoxygenionsbasedontheelementaryreactionsoccurringontheoxygenelectrode.Tripleion-electronic-protonicconducting(TIEC)materialscanextendthetriple-phaseboundary(TPB)areatotheentiresurfaceoftheoxygenelectrode.Besidesthebasicrequirementsofhighactivityandelectrochemicalperformance,theoxygenelectrodealsoneedstohaveasufficientporosity,agoodstability,andamatchedthermalexpansioncoefficientwiththeelectrolyte.Developingnewmaterialsoroptimizingtheircompositionsisapossiblewaytoimprovetheintrinsiccharacteristicsofmaterials.Effectivedesignstrategiesincludeelementdoping(A/B/O-sitedoping)ortheconstructionofA-andB-sitedefects.TheA-siteintheperovskitestructureensuresalargelatticevolumeandpreventslatticedistortion,anddopingelementsintheA-sitewithlargeradiiisbeneficialtoiontransport.TheacceptordopingontheB-sitecanincreasetheelectronclouddensityaroundtheoxygenatoms,therebyfacilitatingprotonabsorption.Also,theoxygen-sitedopingismorecomplicated.Thesubstitutionofoxygenbyelementswithalowervalencestateandahigherelectronegativitycanpromotethemigrationrateofoxideionsandprotons.However,electronconductivityandcarrierconcentrationmaydecreaseafteraniondoping.TherealizationofoptimalTIECinsingle-phasematerialsisachallenge.Compositeelectrodeswithdifferentfunctionsexhibitsynergisticeffectsandstronginteractionsatthenanoscale,thusgarneringincreasingattention.Compositeoxygenelectrodecanimprovethemismatchedthermalmechanicalissuebetweentheoxygenelectrodeandtheelectrolyte,andenhancethechemicalstabilitytowardsCO2andH2O,therebyincreasingthelong-termstabilityofPCCs.Methodsforpreparingcompositeoxygenelectrodesincludemechanicalmixing,impregnation,self-assembly,anddissolution.Amongthesemethods,thelastthreecanbeusedtofabricatenano-sizedcompositeoxygenelectrodeswithasuperiorperformance.ThestabilityoftheoxygenelectrodeandtheinterfacebetweentheoxygenelectrodeandtheelectrolytehasasignificantimpactonthelifespanofthePCCs.TheadhesionbetweentheelectrodeandtheelectrolyteisstrengthenedviadepositinganintermediatelayertoenhancePCCsstability.Activematerialwithahighcoefficientofthermalexpansioncanbecombinedwithanegativethermalexpansionmaterialtoformacompositeoxygenelectrode,exhibitingawell-matchedthermalexpansioncharacteristicwiththeelectrolyte,whichisbeneficialtothethermalcyclingstabilityofthePCCs.Inadditiontointerfacestabilitybetweentheelectrodeandelectrolyte,thestabilityoftheoxygenelectrodematerialisalsocrucial.MostoxygenelectrodematerialscontainBaandSrelements,whichtendtoenrichandsegregateontheelectrodesurface,especiallyinatmospherescontainingH2OandCO2.Watercanpromoteelementsegregation,leadingtotheformationofsecondaryphasesthroughreactionswithimpuritiesinair,whichaffectsthecatalyticactivityoftheelectrodematerial.Thestabilityofoxygenelectrodematerialscanbesignificantlyimprovedviadoping,developingmaterialswithoutalkalielements,andusingcompositeoxygenelectrodes.Inaddition,otherpollutants(suchasCr,Si,B)maybegeneratedinthestack,whichalsoaffectsthestability.Furthermore,theoxygenelectrodeofPCCsisexposedtohumidifiedairwhenoperatedintheelectrolysiscellmode.However,thereisalimitedresearchonthepoisoningofPCCsoxygenelectrodestowardshighsteamandotherelements(Cr,Si).SummaryandprospectsPCCsisakeytechnologyforrenewableenergyconversionandstorage.Thedegradationofoxygenelectrodegreatlyincreasesthepolarizationresistanceofthecellandcausesobviouslydeclinedperformance.Itisthusurgenttoimprovethestabilityofoxygenelectrodematerials.Afurtherresearchcanbeconductedinthefollowingfields,i.e.,therelationshipbetweenthecompositionandelectrochemicalperformanceoftheoxygenelectrode,theinfluenceofmicrostructureevolutionandmorphologychangesunderahighhumidityonelectrochemicalperformance,andthecorrespondingdegradationmechanisms;thethermalcyclestabilityandinterfacestabilityofoxygenelectrodematerialsunderactualoperatingconditions;themechanismofthePCCsoxygenelectrodepoisonedbyCrandSiinahighhumidifiedatmosphere,aswellascorrespondingdetoxificationstrategies;anditisnecessaryforcommercialapplicationrequirementstoinvestigatethestabilityoflarge-areaPCCsundertypicaloperatingconditions.
作者：张晓玉 马丽丽 王睿 杨磊 刘魁 黄祖志 陈婷 王绍荣 Author：ZHANGXiaoyu MALili WANGRui YANGLei LIUKui HUANGZuzhi CHENTing WANGShaorong
作者单位：中国矿业大学,江苏徐州221116中广核风电有限公司,北京100070江西科技师范大学,南昌330038
刊名：硅酸盐学报 ISTICEIPKU
Journal：JournaloftheChineseCeramicSociety
年，卷(期)：2024, 52(7)
分类号：TM911.47
关键词：质子陶瓷电池 氧电极 材料设计 电化学性能 稳定性
Keywords：protonceramiccells oxygenelectrode materialsdesign electrochemicalperformance stability
机标分类号：O643TL364TM911.4
在线出版日期：2024年7月24日
基金项目：中央高校基本科研业务费专项，国家自然科学基金，江苏省碳达峰碳中和科技创新专项质子陶瓷电池氧电极材料设计及稳定性研究进展[
期刊论文] 硅酸盐学报--2024, 52(7)张晓玉 马丽丽 王睿 杨磊 刘魁 黄祖志 陈婷 王绍荣质子陶瓷电池(PCCs)可广泛用于发电、储能和可持续化学合成等研究领域,其工作温度适中、效率高,具有广阔的应用前景.然而,在中低温时,PCCs氧电极的氧析出反应(OER)和氧还原反应(ORR)动力学缓慢,材料稳定性差,导致其难以高...参考文献和引证文献
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质子陶瓷电池氧电极材料设计及稳定性研究进展 Research Progress on Materials Design and Stability of Oxygen Electrode in Proton Ceramic Cells
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