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Solid-ion conductors (SICs) comprising non-ionic plastic crystals and lithiumsalts often require compositing with polymers to render them processable foruse in solid-state lithium-metal batteries. Here, we show that polymer-dopedplastic crystal SICs form a previously unrecognized plastic crystal-polymerhigh entropy interphase, where ions selectively partition and exhibit a higherfraction of matrix-separated ion pairs than in the bulk. Liithium iondiffusivity in this interphase is an order of magnitude higher than in othermicroenvironments due to an increase in the molar volume of the plastic crystalin the vicinity of the polymer, which increases the frequency of bond rotationin the plastic crystal required for ion conduction. Surprisingly, the polymerdoes not directly participate in ion transport. These insights led us toprepare SICs from specific polymers, plastic crystals, and lithium halide saltsthat concomitantly deliver fast ion conduction at ambient and sub-ambienttemperatures and sustainable passivation of the lithium anode.

Harnessing Structural and Dynamic Heterogeneity to Direct Ion Transport in Plastic Crystal-Polymer Composite Solid-Ion Conductors