Importance of Bicontinuous Structure in Elastomeric Electrolytes Enabling High-Energy Solid-State Lithium-Metal Batteries
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Solid-state lithium (Li)-metal batteries (LMBs) are garnering attention as a next-generation battery surpassing conventional Li-ion batteries in terms of energy density and operational safety. In this study, various plastic crystal-embedded elastomer electrolytes (PCEEs) are investigated with different phase-separated structures, prepared by systematically adjusting the volume ratio of the phases, to elucidate the structure-property-electrochemical performance relationship of the PCEE in the LMBs. At an optimal volume ratio of elastomer phase to plastic-crystal phase, bicontinuous-structured PCEE, consisting of efficient ion-conducting, plastic-crystal pathways with long-range connectivity within a crosslinked elastomer matrix, exhibits exceptionally high ionic conductivity and excellent mechanical resilience. A full cell featuring this optimized PCEE, a 35 µm thick Li anode, and a high loading NMC-83 cathode delivers a high energy density of 437 Wh kg−1.