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Molecular-to-polymeric crossover in ion diffusion in glyme-based electrolytes: from vehicular to hopping transport
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Molecular-to-polymeric crossover in ion diffusion in glyme-based electrolytes: from vehicular to hopping transport
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Paper
Molecular-to-polymeric crossover in ion diffusion in glyme-based electrolytes: from vehicular to hopping transport
2026
Overview
Ion transport in glyme-based electrolytes arises from a complex interplay between solvation structure, ion correlations, and polymer chain length. Here, combining pulsed-field gradient nuclear magnetic resonance (PFG-NMR), ionic conductivity measurements, and molecular dynamics (MD) simulations, we investigate the diffusion of monovalent cations (Li\\(^+\\), Na\\(^+\\), Cs\\(^+\\)) and TFSI\\(^-\\) anions across a wide molecular-weight range, from monoglyme to long poly(ethylene oxide) (PEO) chains up to 4000~g/mol, corresponding to \\(n\\) up to 88, where \\(n\\) is the number of ethylene oxide repeat units. We identify a crossover region at \\(n 8\\) separating two transport regimes. For short chains, ion motion is consistent with a vehicular mechanism, accompanied by pronounced ion correlations. For longer chains, ion transport decouples from polymer motion and proceeds via rapid coordination exchanges within a slowly relaxing matrix. This transition is accompanied by reduced ion clustering and enhanced anion mobility, leading to increasingly anion-dominated charge transport. Overall, our results provide a molecular picture of ion transport across the molecular-to-polymeric transition and highlight the central role of solvation shell dynamics and polymer relaxation in governing ion dynamics in glyme-based electrolytes.
Publisher
Cornell University Library, arXiv.org
Subject
