Role of Bicontinuous Structure in Elastomeric Electrolytes for High-Energy Solid-State Lithium-Metal Batteries |
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Authors: | Junghun Han Michael J Lee Kyungbin Lee Young Jun Lee Seung Ho Kwon Ju Hong Min Eunji Lee Wonho Lee Seung Woo Lee Bumjoon J Kim |
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Affiliation: | 1. Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), Daejeon, 34141 Republic of Korea;2. George W. Woodruff School of Mechanical Engineering, Georgia Institute of Technology, Atlanta, GA, 30332 USA;3. School of Materials Science and Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju, 61005 Republic of Korea;4. Department of Polymer Science and Engineering, Department of Energy Engineering Convergence, Kumoh National Institute of Technology, Gumi, 39177 Republic of Korea |
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Abstract: | Solid-state lithium (Li)-metal batteries (LMBs) are garnering attention as a next-generation battery technology that can surpass conventional Li-ion batteries in terms of energy density and operational safety under the condition that the issue of uncontrolled Li dendrite is resolved. 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 (i.e., 1:1), 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 (≈10−3 S cm−1) at 20 °C and excellent mechanical resilience (elongation at break ≈ 300%). A full cell featuring this optimized PCEE, a 35 µm thick Li anode, and a high loading LiNi0.83Mn0.06Co0.11O2 (NMC-83) cathode delivers a high energy density of 437 Wh kganode+cathode+electrolyte−1. The established structure–property–electrochemical performance relationship of the PCEE for solid-state LMBs is expected to inform the development of the elastomeric electrolytes for various electrochemical energy systems. |
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Keywords: | bicontinuous structures elastomeric electrolytes high-energy-density lithium-metal batteries solid-state electrolytes |
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