Understanding Ion Distribution and Diffusion in Solid Polymer Electrolytes

TL;DR

This study uses molecular dynamics simulations to explore how ion distribution affects diffusion in solid polymer electrolytes, offering insights for improving energy storage materials.

Contribution

It establishes correlations between ion distribution and transport, and proposes phase diagrams based on ion parameters, advancing understanding of ion conduction mechanisms.

Findings

Identifies a crossover from discrete to percolated ion aggregates.

Provides phase diagrams as a function of ion parameters.

Determines ion diffusion coefficients across phases.

Abstract

Solid polymer electrolytes exhibit ion conduction and high mechanical properties, thus are promising materials for future energy storage devices. The ion conductivity in an SPE is intricately connected to salt ion distribution in the polymer matrix. The relationship between ion diffusion and ion distribution remains unresolved. Here, we conduct coarse grained molecular dynamics simulations and establish correlations between ion distribution and transport for a phenomenological SPE model. We propose phase diagrams of SPEs as a function of ion pair size, ion concentration and the Bjerrum length of the material. A crossover from a discrete ion aggregate to a percolated ion aggregate is demonstrated as a function of ion pair size in the SPE. Further, we determine ion diffusions for all the phases of the SPE. The work provides important design strategies for controlling ion distribution and enhancing ion conductivity in a polymer matrix.