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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

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Classifying Electrolyte Solutions by Comparing Charge and Mass Transport

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Energy & Environmental Materials 2022年第1期5卷 6-9页

作者： Bernhard Roling Janosch Kettner Vanessa Miß Department of Chemistry and Center for Materials Science(WZMW) University of MarburgHans-Meerwein-Strasse 4Marburg 35032Germany

The conventional classification of electrolyte solutions as“strong”or“weak”accounts for their charge transport properties,but neglects their mass transport properties,and is not readily applicable to highly concentrated ***,we use the Onsager transport formalism in combination with linear response theory to attain a more general classification taking into account both charge and mass transport *** this end,we define a molar mass transport coefficientΛ_(mass),which is related to equilibrium center-of-mass fluctuations of the mobile ions and which is the masstransport analogue of the molar ionic conductivityΛ_(charge).Three classes of electrolyte solution are then distinguished:(i)“Strong electrolytes”with 4Λ_(mass)≈Λ_(charge);(ii)“weak charge transport electrolytes”withΛ_(charge)≪4Λ_(mass);and(iii)“weak mass transport electrolytes”with 4Λ_(mass)≪Λ_(charge).While classes(i)and(ii)encompass the classical“strong”and“weak”electrolytes,respectively,many highly concentrated electrolytes fall into class(iii)and thus exhibit transport properties clearly distinct from classical strong and weak electrolytes.

关键词： charge and mass transport superconcentrated electrolytes energy storage ion correlations

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