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Stabilizing electrochemical interfaces in viscoelastic liquid electrolytes.

ABSTRACT: Electrodeposition is a widely practiced method for creating metal, colloidal, and polymer coatings on conductive substrates. In the Newtonian liquid electrolytes typically used, the process is fundamentally unstable. The underlying instabilities have been linked to failure of microcircuits, dendrite formation on battery electrodes, and overlimiting conductance in ion-selective membranes. We report that viscoelastic electrolytes composed of semidilute solutions of very high-molecular weight neutral polymers suppress these instabilities by multiple mechanisms. The voltage window ?V in which a liquid electrolyte can operate free of electroconvective instabilities is shown to be markedly extended in viscoelastic electrolytes and is a power-law function, ?V : ?^1/4, of electrolyte viscosity, ?. This power-law relation is replicated in the resistance to ion transport at liquid/solid interfaces. We discuss consequences of our observations and show that viscoelastic electrolytes enable stable electrodeposition of many metals, with the most profound effects observed for reactive metals, such as sodium and lithium. This finding is of contemporary interest for high-energy electrochemical energy storage.

SUBMITTER: Wei S

PROVIDER: S-EPMC5866059 | biostudies-literature | 2018 Mar

REPOSITORIES: biostudies-literature

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Stabilizing electrochemical interfaces in viscoelastic liquid electrolytes.

Wei Shuya S Cheng Zhu Z Nath Pooja P Tikekar Mukul D MD Li Gaojin G Archer Lynden A LA

Science advances 20180323 3

Electrodeposition is a widely practiced method for creating metal, colloidal, and polymer coatings on conductive substrates. In the Newtonian liquid electrolytes typically used, the process is fundamentally unstable. The underlying instabilities have been linked to failure of microcircuits, dendrite formation on battery electrodes, and overlimiting conductance in ion-selective membranes. We report that viscoelastic electrolytes composed of semidilute solutions of very high-molecular weight neutr ...[more]

PMID: 29582017

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Project description:The article summarizes the results of our research on the behavior of ions at uncharged fluid interfaces, with a focus on moderately to highly concentrated aqueous electrolytes. The ion-specific properties of such interfaces have been analyzed. The ion-specificity series are different for water|air and water|oil; different for surface tension σ, surface Δχ potential and electrolyte adsorption, and they change with concentration. A methodology has been developed that allows to disentangle the multiple factors controlling the ion order. The direct ion-surface interactions are not always the most significant factor behind the observed ion sequences: indirect effects stemming from conjugate bulk properties are often more important. For example, the order of the surface tension with the nature of the anion (σKOH > σKCl > σKNO3 for potassium salts) is often the result of bulk nonideality and follows the order of the bulk activity coefficients (γKOH > γKCl > γKNO3) rather than that of a specific ion-surface interaction potential. The surface Δχ potential of aqueous solutions is, in many cases, insensitive to the ion distribution in the electric double layer but reflects the orientation of water at the surface, through the ion-specific dielectric permittivity ε of the solution. Even the sign of Δχ is often the result of the decrement of ε in the presence of electrolyte. A whole new level of complexity appears when the ions interact with an uncharged surfactant monolayer. A method has been developed to measure the electrolyte adsorption isotherms on monolayers of varying area per surfactant molecule via a combination of experiments-compression isotherms and surface pressure of equilibrium spread monolayers. The obtained isotherms demonstrate that the ions exhibit a maximum in their adsorption on monolayers of intermediate density. The maximum is explained with the interplay between ion-surfactant complexation, volume exclusion and osmotic effects.

Dataset Information

Stabilizing electrochemical interfaces in viscoelastic liquid electrolytes.

Publications

Stabilizing electrochemical interfaces in viscoelastic liquid electrolytes.

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