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Control of Selective Ion Transfer across Liquid-Liquid Interfaces: A Rectifying Heterojunction Based on Immiscible Electrolytes.

ABSTRACT: The current rectification displayed by solid-state p-n semiconductor diodes relies on the abundance of electrons and holes near the interface between the p-n junction. In analogy to this electronic device, we propose here the construction of a purely ionic liquid-state electric rectifying heterojunction displaying an excess of monovalent cations and anions near the interface between two immiscible solvents with different dielectric properties. This system does not need any physical membrane or material barrier to show preferential ion transfer but relies on the ionic solvation energy between the two immiscible solvents. We construct a simple device, based on an oil/water interface, displaying an asymmetric behavior of the electric current as a function of the polarity of an applied electric field. This device also exhibits a region of negative differential conductivity, analogous to that observed in brain and heart cells via voltage clamp techniques. Computer simulations and mean field theory calculations for a model of this system show that the application of an external electric field is able to control the bulk concentrations of the ionic species in the immiscible liquids in a manner that is asymmetric with respect to the polarity or direction of the applied electric field. These properties make possible to enhance or suppress selective ion transport at liquid-liquid interfaces with the application of an external electric field or electrostatic potential, mimicking the function of biological ion channels, thus creating opportunities for varied applications.

SUBMITTER: Guerrero-Garcia GI

PROVIDER: S-EPMC5126720 | biostudies-literature | 2016 Nov

REPOSITORIES: biostudies-literature

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Control of Selective Ion Transfer across Liquid-Liquid Interfaces: A Rectifying Heterojunction Based on Immiscible Electrolytes.

Guerrero-García Guillermo Iván GI Solis Francisco J FJ Raidongia Kalyan K Koltonow Andrew Robert AR Huang Jiaxing J Olvera de la Cruz Mónica M

ACS central science 20161102 11

The current rectification displayed by solid-state p-n semiconductor diodes relies on the abundance of electrons and holes near the interface between the p-n junction. In analogy to this electronic device, we propose here the construction of a purely ionic liquid-state electric rectifying heterojunction displaying an excess of monovalent cations and anions near the interface between two immiscible solvents with different dielectric properties. This system does not need any physical membrane or m ...[more]

PMID: 27924315

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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

Control of Selective Ion Transfer across Liquid-Liquid Interfaces: A Rectifying Heterojunction Based on Immiscible Electrolytes.

Publications

Control of Selective Ion Transfer across Liquid-Liquid Interfaces: A Rectifying Heterojunction Based on Immiscible Electrolytes.

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