Role of Bicontinuous Structure in Elastomeric Electrolytes for High-Energy Solid-State Lithium-Metal Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 36349804.
- Also identified by DOI 10.1002/adma.202205194.
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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<sup>-3</sup> S cm<sup>-1</sup> ) 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 LiNi<sub>0.83</sub> Mn<sub>0.06</sub> Co<sub>0.11</sub> O<sub>2</sub> (NMC-83) cathode delivers a high energy density of 437 Wh kg<sub>anode+cathode+electrolyte</sub> <sup>-1</sup> . 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.