Plastic crystal-embedded elastomeric electrolytes for high-energy solid-state lithium metal batteries

Abstract

The use of lithium metal anodes in all-solid-state batteries has emerged as the most promising technology for replacing conventional lithium-ion batteries. Here, we report a new class of elastomeric solid-state electrolytes having a three-dimensionally interconnected plastic crystal phase with an unprecedented combination of mechanical robustness, high ionic conductivity, low interfacial resistance, and high lithium-ion transference number. The in-situ-formed elastomer electrolyte on copper and lithium foils accommodates volume changes for prolonged lithium plating/stripping processes. Under the constrained conditions of a high-loading LiNi0.83Mn0.06Co0.11O2 cathode and limited lithium source, the full cells with the elastomer electrolytes deliver high specific energy exceeding 410 Wh kganode+cathode+electrolyte-1 at ambient temperature. The elastomeric electrolyte system presents a powerful strategy for enabling stable operation of high-energy, all-solid-state lithium metal batteries.