ArticleThe journal of physical chemistry letters2026
Hopping-Dominated Li+ Transport in Deeply Supercooled Polymer-in-Salt Electrolytes.
Article in The journal of physical chemistry letters, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
Deeply supercooled solvent-free lithium electrolytes can exhibit Li-ion transference numbers approaching unity under anion-blocking conditions, yet the microscopic origin of this behavior remains unclear. Here, we use long, statistically replicated molecular dynamics simulations to investigate Li-ion transport in deeply supercooled lithium (fluorosulfonyl)(trifluoromethanesulfonyl)amide, Li[FTA], and its poly(methyl methacrylate)-based polymer-in-salt electrolytes. Li+ ions exhibit translational mobility nearly an order of magnitude higher than that of FTA- anions and display pronounced non-Gaussian displacement statistics indicative of intermittent hopping. Spatially resolved analyses reveal heterogeneous dynamics: Li+ motion is suppressed near the polymer interface but enhanced in polymer-dilute regions, where Li-anion coordination is weakened and hopping events become more frequent. These results suggest that hopping-mediated, spatially heterogeneous Li+ motion is a key microscopic origin of near-unity transference numbers in deeply supercooled polymer-in-salt electrolytes and provide design principles for high-transference-number solvent-free systems.
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