High-energy density solid-state lithium metal batteries are expected to become the next generation of energy storage devices. Polymeric ionic liquid-based solid polymer electrolytes (PIL-based SPEs) are an attractive choice among electrolytes, but their ionic conductivities are generally insufficient due to numerous crystallized polymer regions. To achieve higher conductivity, we use facile copolymerization of an ionic liquid (IL) monomer and poly(ethylene glycol) diacrylate monomer to obtain in situ plasticized polymer chains. The resultant PIL-based SPE exhibits decreased crystallinity, a lower glass-transition temperature, and improved ionic conductivity (1.4 × 10 S cm at 30 °C). A solid-state LiFePO (LFP)|Li battery based on the SPE displays a high reversible specific capacity of 140 mA h g at 0.2C at 25 °C and excellent cycling stability, accompanying high Coulombic efficiency of approximately 100%. The in situ plasticized PIL-based SPE is significant in developing solid-state Li metal battery systems.
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