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Novel single-ion conducting polymer electrolytes with high toughness and high resistance against lithium dendrites

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Nano Research 2023年第6期16卷 8457-8468页

作者： David Fraile-Insagurbe Nicola Boaretto Itziar Aldalur Iñigo Raposo Francisco Javier Bonilla Michel Armand María Martínez-Ibañez Centre for Cooperative Research on Alternative Energies CIC energiGUNEBasque Research and Technology Alliance(BRTA)Alava Technology ParkAlbert Einstein 48Vitoria-Gasteiz 01510Spain University of the Basque Country(UPV/EHU) Barrio Sarrienas/nLeioa 48940Spain

Solid-state polymer electrolytes are considered as an alternative to classic liquid electrolytes,particularly for application in highenergy lithium metal *** respect to common dual-ion conductors,single-ion conducting polymer electrolytes(SICPEs)are less affected by lithium dendrites growth and thus are particularly interesting for application in lithium metal *** this work,novel SIC-PEs are developed,based on an ionomer having poly(ethylene-alt-maleimide)backbone and lithium phenylsulfonyl(trifluoromethanesulfonyl)imide pendant moieties,further blended with poly(ethylene oxide)(PEO)and poly(ethylene glycol)dimethyl ether(PEGDME).These SIC-PEs exhibit ionic conductivity around~7×10^(−6)S·cm^(−1) at 70℃,lithium transference number close to unity,and excellent mechanical properties,with fracture toughness over 30 J·cm^(−3).Additionally,the electrolytes show very high resistance against lithium dendrites growth,by cycling for more than 1200 h in Li°symmetric cells at a current density of 0.1 mA·cm^(−2).LiFePO4||Li°cells with these SIC-PEs were cycled at 70℃ and C/10,showing initial capacity of almost 160 mAh·g^(−1)and residual capacity of 45%after 100 *** work shows that single-ion conducting polymer electrolytes based on poly(ethylene-alt-maleimide)backbone are promising materials for application as electrolytes or catholytes in lithium metal polymer batteries.

关键词： single-ion conductors solid-state Li metal batteries polymer electrolytes lithium dendrites transference number mechanical properties

Understanding Lithium-ion Transport in Sulfolane- and Tetraglyme-Based Electrolytes Using Very Low-Frequency Impedance Spectroscopy

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Energy & Environmental Materials 2023年第1期6卷 368-376页

作者： Janet SHo Oleg A.Borodin Michael SDing Lin Ma Marshall A.Schroeder Glenn R.Pastel Kang Xu Energy Sciences Division Sensors and Electron Devices DirectorateUS Army Research LaboratoryAdelphi MD 20783USA

With the increasing interest in highly concentrated electrolyte systems,correct determination of the cation transference number is ***-field gradient NMR technique,which measures self-diffusion coefficients,is often applied on liquid electrolytes because of the wide accessibility and simple sample ***,since the assumptions of this technique,that is,complete salt dissociation,all ions participating in motion,and all of them moving independently,no longer hold true in concentrated solutions,the transference numbers,thus obtained are often *** the present work,impedance spectroscopy at a frequency range of 1 MHz to 0.1 mHz was used to examine the concentration effect on lithium-ion transference number under anion-blocking conditions T abc Liþfor two electrolytes:lithium bis(fluorosulfonyl)imide(LiFSI)in sulfolane(SL)and lithium bis(trifluorosulfonyl)imide(LiTFSI)in tetraglyme(G4).The T abc Liþof the former was almost an order of magnitude higher than that of the *** also appeared to increase with increasing concentration while the latter followed an opposite *** faster Li^(+)transport in the SL system is attributed to the formation of a liquid structure consisting of extended chains/bridges of SL molecules and the anions,which facilitate a cation-hopping/ligand-exchanged-typed diffusion mechanism by partially decoupling the cations from the anions and solvent *** G4 system,in contrast,is dominated by the formation of long-lived,stable[Li(G4)]+solvation cages that results in a sluggish Li+*** difference between the two transport mechanisms is discussed via comparison of the bulk ionic conductivity,viscosity,ion self-diffusion coefficients,and the Onsager transport coefficients.

关键词： anion-blocking conditions ion correlations low-frequency impedance spectroscopy transference number

Physical Characterization of Ionic Liquid-Modified Polyvinyl Alcohol and Sodium Thiocyanate Polymer Electrolytes for Electrochemical Double-Layer Capacitor Application

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Journal of Shanghai Jiaotong university(Science) 2023年第2期28卷 161-171页

作者： AZEMTSOP Manfo Theodore MEHRA Ram Mohan KUMAR Yogesh GUPTA Meenal Material Research Laboratory Department of PhysicsSBSRSharda UniversityGreater Noida 201310India Department of Electronics and Communication Engineering Sharda UniversityGreater Noida 201310India Department of Physics Atma Ram Sanatan Dharma CollegeUniversity of DelhiNew Delhi 110021India

Novel gel polymer electrolytes(GPEs)composed of polyvinyl alcohol(PVA)and sodium thiocyanate were developed via a solution casting *** ionic liquid(IL),1-ethyl-3-methyl-imidazolium tricyanomethanide([EMIM][TCM]),was doped into a polymer–salt complex system(PVA+NaSCN)to further enhance the ***-doped polymer electrolyte(ILDPE)films were characterized using X-ray diffraction(XRD),polarized optical microscopy(POM),Fourier-transform infrared(FTIR)spectroscopy,and conductivity *** was performed to check the degree of crystallinity and amorphicity of the ILDPE films,and the amorphicity of GPEs increased with the increase of the IL *** was employed to evaluate the changes in the surface morphology due to the inclusion of salt and IL in the *** compositional nature of the GPE films was examined via FTIR *** electrical and electrochemical properties were characterized by cyclic voltammetry and electrochemical impedance *** maximum conductivity for the GPE film was estimated to be 1.10×10^(-5) S/cm for 6%(mass fraction)of IL in the polymer–salt *** ionic transference number was approximately *** electrochemical double-layer capacitor(EDLC)was built from optimized GPE films and reduced graphene oxide-based *** specific capacitance calculated from the cyclic voltammograms of the EDLC cells was 3 F/g.

关键词： ionic conductivity ionic liquid(IL) mobility transference number cyclic voltammetry polymer electrolyte

两性分子掺杂自支撑单离子传导聚合物电解质及其锂金属二次电池

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中国科学:材料科学(英文版) 2023年第10期66卷 3799-3809页

作者：许鹤李婉莹黄玲曾丹黎张运丰孙玉宝程寒松 Faculty of Materials Science and Chemistry China University of Geosciences(Wuhan)Wuhan 430078China

制备高离子电导率的自支撑单离子传导聚合物电解质仍然面临挑战.本文中,我们通过聚[4,4’(二苯醚基)-5,5’-联苯并咪唑]侧链化学接枝丙烷磺酰(三氟甲基磺酰)亚胺锂,得到自支撑聚合物电解质(PBIg-LiPSI).PBI-g-LiPSI具有优异的成膜性能,... 详细信息

制备高离子电导率的自支撑单离子传导聚合物电解质仍然面临挑战.本文中,我们通过聚[4,4’(二苯醚基)-5,5’-联苯并咪唑]侧链化学接枝丙烷磺酰(三氟甲基磺酰)亚胺锂,得到自支撑聚合物电解质(PBIg-LiPSI).PBI-g-LiPSI具有优异的成膜性能,实验发现,掺杂两性分子1-甲基-3-丙烷磺酰(三氟甲基磺酰)亚胺咪唑内盐(MeImPSI)后,离子电导率和^(7)Li核磁共振峰的化学位移都随着掺杂两性分子的质量分数呈线性递增.PBI-g-LiPSI/MeImPSI(25 wt%)凝胶自支撑单离子传导聚合物电解质的室温离子电导率是0.68 mS cm^(-1),锂离子迁移数是0.95.使用该电解质隔膜的金属锂对称电池在±0.5 mA cm^(-2)@2 mA h cm^(-2)运行2100小时未发生短路,金属锂二次电池可在1C下稳定循环500圈.本工作开发了一种用于金属锂二次电池的两性分子掺杂自支撑单离子传导聚合物电解质.

关键词： single ion-conducting polymer electrolyte polybenzimidazole zwitterion transference number lithium metal

Effect of junction potential on the EMF of bielectrolyte solid-state sensors

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Journal of University of Science and Technology Beijing 2005年第1期12卷 81-84页

作者： FushenLi HuiXia LingWang YanhongZhang LifenLi MaterialsScienceandEngineeringSchool UniversityofScienceandTechnologyBeijingBeijing100083China

The EMF (electromotive force) expressions of bielectrolyte solid-state sensors derived from classical thermodynamics are not rigorous. They are only applicable in some special situations. In order to expand their applicable scope, they should be derived from irreversible thermodynamics theory. There is a junction potential term in the EMF equations of double solid electrolyte sensors derived from irreversible thermodynamics. The junction potential involves the ion transference numbers and the electron transference numbers of two kinds of solid electrolytes. When the transference numbers of reaction ions in the two solid electrolytes equal 1 only, the junction potential term is zero and two types of EMF equations become the same.

关键词： solid electrolyte sensor electromotive force junction potential transference number