文档名：二维六方Mo2B2作为金属离子电池负极材料的第一性原理研究
摘要：可充电金属离子电池(RMBs)迫切需要开发新型高比容量的负极材料.采用第一性原理计算方法研究了六方h-Mo2B2MBene作为RMBs(Li、Na、Mg和K离子)负极材料的潜力.计算结果表明,h-Mo2B2MBene结构稳定且具有良好的导电性.作为RMBs负极材料组装成Li离子电池、Na离子电池、K离子电池和Mg离子电池时,其理论比容量分别为:753、314、125mA·h·g-1和1506mA·h·g-1.与传统石墨负极相比,h-Mo2B2在锂离子电池中具有更高的比容量,而Mg离子在h-Mo2B2上的超大理论容量得益于Mg离子可以携带更多的电荷.Li、Na、Mg和K离子在h-Mo2B2上具有较低的扩散势垒,分别为39、10、37meV和7meV.Li、Na、Mg和K离子在h-Mo2B2中的平均开路电压分别为:0.36、0.47、0.63V和0.63V.这些优异的性能表明,h-Mo2B2MBene可以作为锂离子、钠离子以及镁离子电池等领域中一种非常有前景的负极材料.
Abstract：IntroductionWiththecontinuousgrowthinenergystoragedemandsforportableelectronicdevices,electricvehicles,andgridenergystorage,rechargeablemetal-ionbatterieshavefoundextensiveapplicationsinenergysupplyandstorageduetotheiradvantagesoflowself-discharge,highenergydensity,andenvironmentalfriendliness.Oneoftheessentialcomponentsofmetal-ionbatteriesisthenegativeelectrodematerial,anditsphysicalandchemicalpropertiesarecrucialforbatteryperformance.However,inpracticalapplications,thereisstillashortageofhigh-performancenegativeelectrodematerialsformetal-ionbatteries.Traditionalthree-dimensionalelectrodematerialssufferfromlimitedstoragecapacityandlessthanidealcharge-dischargerates,primarilybecauseofthelimitednumberoflatticevacanciesintheirstructure.Thislimitationhinderstheirabilitytomeetmarketdemands,particularlyinscenarioswherefastercharge-dischargeratesarerequired,suchaselectricvehiclesandgridenergystorage.Incontrast,two-dimensionalmaterialsofferadvantagessuchasalargerspecificsurfaceareaandenhancedmetaliondiffusion,makingthemsuitableforenergystorageinbatteries.Amongtwo-dimensionalmaterials,theemergingclassoftwo-dimensionaltransitionmetalborides(MBenes)exhibitsexcellentelectricalconductivity,structuralstability,andhighspecificcapacity.Asaresult,anincreasingamountofresearchworkisconsideringthemaselectrodematerialsforenergystoragesystems.Comparedtotraditionalexperimentalresearchmethods,first-principlescomputationaltechniquescanbetterassistindesigningnovelhigh-performanceelectrodematerialsattheatomicandelectronicscale.Inthispaper,weaimtoexplorethepotentialofh-Mo2B2MBeneasanegativeelectrodematerialformetal-ionbatteriesusingfirst-principlescalculationmethods.Wesystematicallyinvestigateitsstructuralstability,electronicstructure,andelectrochemicalproperties.Thestudiessuggestthath-Mo2B2holdspromiseasaprospectivenegativeelectrodematerialforapplicationinmetal-ionbatteries.MethodsInthispaperthecalculationsarebasedonDensityFunctionalTheory(DFT)first-principlesmethods,implementedusingtheViennaAbinitioSimulationPackage(VASP).TheProjectorAugmentedWave(PAW)pseudopotentialapproachisutilized,withaplanewavecutoffenergyof500eV.ThePerdew-Burke-Ernzerhof(PBE)generalizedgradientapproximation(GGA)isemployedfortheexchange-correlationfunctional.Toaccountfortheinteractionbetweenmetalcationsand2Dmaterials,vanderWaalsinteractionsareconsideredinthecalculations.Duringthegeometricstructureoptimization,energyandforceconvergencecriteriaaresetto10-5eV/atomand0.01eV/?,respectively.TheK-pointgridsusedforh-Mo2B2unitcelland2×2×1supercellcalculationsare20×20×1and5×5×1,respectively.Avacuumlayerwithathicknessof20?isincludedtoeliminatethespuriousinteraction.Phononspectracalculationsareperformedusingdensityfunctionalperturbationtheory.Differentialchargecalculationsareemployedtostudychargeredistributionandtransferbetweenadsorbedmetalatomsand2Dmaterials.Baderchargeanalysisisutilizedtoassesstheamountofchargetransferbetweenthemetalionsandthe2Dmaterial.TheClimbingImageNudgedElasticBand(CI-NEB)methodisusedtocalculatethemigrationenergybarriersandmigrationpathwaysofmetalionsonh-Mo2B2.ResultsanddiscussionThe2Dh-Mo2B2studiedinthispaperbelongstotheP6/mmmspacegroupwithinthehexagonalcrystalsystem.ItcomprisesthreeatomiclayersstackedinaMo-B-Mosequence,withhexagonalBatomiclayerssituatedbetweentheupperandlowerMoatomicplanes.Toevaluatethedynamicalstabilityofh-Mo2B2,phononspectrumcalculationswereconducted,andnoimaginaryfrequencieswereobservedthroughouttheentireBrillouinzone.Thisindicatesthath-Mo2B2exhibitsdynamicalstability.Thebandstructureofh-Mo2B2revealsnumerousbandscrossingtheFermilevel,confirmingitsmetallicnature.Thisexceptionalelectricalconductivityofh-Mo2B2cansignificantlyenhancetherateperformanceofelectrodes.Adsorptionenergyisafundamentalcriterionforassessingwhetheramaterialcanbeutilizedasanegativeelectrode.TheadsorptionenergiesofLi,Na,Mg,andKontheh-Mo2B2surfacewerecalculated,andallexhibitednegativevalues,indicatingeffectiveadsorptionofallmetalatomsonamonolayerofh-Mo2B2.Rapidcharge-dischargeratesarecrucialforsecondarybatteries,andthemigrationenergybarrierofmetalionsisakeyfactordeterminingthecharge-dischargerate.Themigrationenergybarriersforthefourmetalatomsontheh-Mo2B2surfacearerankedasK(7meV)<Na(10meV)<Mg(37meV)
作者：曹宇 张国辉 王长刚 周静 蔡永茂 赵耀 Author：CAOYu ZHANGGuohui WANGChanggang ZHOUJing CAIYongmao ZHAOYao
作者单位：东北电力大学,现代电力系统仿真控制与绿色电能新技术教育部重点实验室,吉林132012;东北电力大学电气工程学院,吉林132012东北电力大学,现代电力系统仿真控制与绿色电能新技术教育部重点实验室,吉林132012;东北电力大学化学工程学院,吉林132012东北电力大学理学院,吉林132012中国铁路设计集团有限公司,天津300308
刊名：硅酸盐学报 ISTICEIPKU
Journal：JournaloftheChineseCeramicSociety
年，卷(期)：2024, 52(7)
分类号：TQ152
关键词：第一性原理计算 金属离子电池 负极材料 二维过渡金属硼化物
Keywords：first-principlescalculation metalionbattery negativeelectrodematerial two-dimensionaltransitionmetalborides
机标分类号：TM912TM242O646
在线出版日期：2024年7月24日
基金项目：国家自然科学基金，吉林省教育厅科学技术研究项目，吉林市科技创新发展计划，吉林省创新创业人才资助项目二维六方Mo2B2作为金属离子电池负极材料的第一性原理研究[
期刊论文] 硅酸盐学报--2024, 52(7)曹宇 张国辉 王长刚 周静 蔡永茂 赵耀可充电金属离子电池(RMBs)迫切需要开发新型高比容量的负极材料.采用第一性原理计算方法研究了六方h-Mo2B2MBene作为RMBs(Li、Na、Mg和K离子)负极材料的潜力.计算结果表明,h-Mo2B2MBene结构稳定且具有良好的导电性.作为...参考文献和引证文献
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二维六方Mo2B2作为金属离子电池负极材料的第一性原理研究 First Principles Study of Two-Dimensional h-Mo2B2 as a Negative Electrode for Metal-Ion Batteries
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