金属锂负极的能源化学

能源技术推动社会进步社会进步:RenewableenergySolarandwindenergyRenewableenergySolarandwindenergyetc.:widedistribution,lowEnergydevicesHumanenergydemandsTheroleofelectrolyt1.锂金属电池的挑战：金属锂枝晶Theroleofelectrolyt1.固态电解质界面膜SEI:Soliddeposition,Electrolytenature,IndependentphaseElectrolytedesignforstableSEImixedconductinginterphase+solid−electrolyteinterphaseACSEnergyLetters2018,3,1564离子溶剂复合结构还原稳定性↓,氧化稳定性↑Angew.Chem.Int.Ed.2018,57,734.EnergyStorageMater.2017,8,194–201.Batteries&Supercaps2019,2,128.Angew.Chem.Int.Ed.2018,57,14055.500X500XRateTheelectrolytegassingonLimetalanodesTheelectrolytegassingonLimetalanodesGrandchallengesofelectrolytedesignforLimetalanodeaThespecificadsorptionoftheIHPandthesolvationstructuredominatetheSEI!Small250mAhPouch250mAhPouchcell200μm200μmDendriteformationLiF-richcyclelifeStableplatingRegulatingthesolvationshell(includingsolvents,anions)rrcCompetitivefactorsNO3-ownsthecompetitivenessinformingnewsolvationshellACSEnergyLett.,2019,4,411NO3-promotesthecompletedecompositionofFSI-.CompletedecompositionofFSI-ispromotedtogenerateLiFandLiSOxinthepresenceofNO3-,thencontributingtouniformSEIandLidepositiontogetherwithLiNxOy.2.Sustained-releas溶剂分解与阴离子分解主导的SEI常规电解液局部高浓电解液(LSCE)弱溶剂化电解液(WSE)d)DFT计算得到的锂离子和溶PLLelectrolytePEO-LiTFSILLZTOPDF80-04572Theta(Degree)PLLcompositeelectrolyte.After1secPLLcompositeelectrolyte.0.91670.78330.65000.91670.78330.65000.91670.7833000Propotionofimmobilizedanions(%)Propotionofimmobilizedanions(%)EC/DECelectrolyteSElXXNucleationoverpotential.a)TheVvstduandNGelectrodes.b)TheLinucleationoverpotentials(μn)onCu,G,andNGelectrodes.Limetalnucleatesontothelithiophilicsites•LithiophilicitychemistryregulatedbyLibonds.Sci.Adv.2019,5,eaau7728.Sci.Adv.2019,5,eaau7728.PorterDA,EasterlingKE,SherifM.PhaseTransformationsinMetalsandAlloys,(RevisedReprint)[M].CRCpress,2009.•LithiophilicitychemistryregulatedbyLibonds.Sci.Adv.2019,5,eaau7728.•LithiophilicitychemistryregulatedbyLibonds.ExperimentalverificationsoftheSci.Adv.2019,5,eaau7728.•LithiophilicsitedesignResearch2019,2019,4608940.表面修饰三维复合金属锂LimitedbyelectrontransferorLiiontransfer?LiionPhasefieldconcentrationorderparameterEnergyStorageMater.2019,23,556concentrationorderparameter+concentrationPhasefieldorderparameter→→→•锂沉积会触发本征应变带来的应力响•局部变形会引起离子的重新分布•抑制电沉积反应的进行，这不利于电池的速率性能•超过阈值后，促进锂的电沉积形貌趋于平滑与致密•阻碍电沉积反应的进行以及导致材料失效的副作用也决定了最佳压力的选择SEILiSEILimetalanode•High-energy-densityLimetalbatteries•SafeLimetalanode•Keyroleofstableelectrolyte&SEI•Ion-solventinter