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Classifying Electrolyte Solutions by Comparing Charge and Mass Transport

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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Ion Dynamics in Concentrated Electrolyte Solutions:Relating Equilibrium Fluctuations of the Ions to Transport Properties in Battery Cells

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Energy & Environmental Materials 2024年第1期7卷 131-138页

作者： bernhard roling Vanessa Miß Janosch Kettner Department of Chemistry University of MarburgHans-Meerwein-Str.435032 MarburgGermany

In recent years,the interest in the development of highly concentrated electrolyte solutions for battery applications has increased *** electrolyte solutions are typically characterized by a low flammability,a high thermal and electrochemical stability and by the formation of a stable solid electrolyte interphase(SEI)in contact to electrode ***,the classification of concentrated electrolyte solutions in terms of the classical scheme"strong"or"weak"has been controversially discussed in the *** this paper,a comprehensive theoretical framework is presented for a more general classification,which is based on a comparison of charge transport and mass *** combining the Onsager transport formalism with linear response theory,center-of-mass fluctuations and collective translational dipole fluctuations of the ions in equilibrium are related to transport properties in a lithium-ion battery cell,namely mass transport,charge transport and Li^(+)transport under anion-blocking *** relevance of the classification approach is substantiated by showing that i)it is straightforward to classify highly concentrated electrolytes and that ii)both fast charge transport and fast mass transport are indispensable for achieving fast Li^(+)transport under anion-blocking conditions.

关键词： batteries concentrated electrolytes linear response theory Onsager formalism transport

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