The Polymer Society of Korea

Abstract

This work investigates how the mechanical properties of elastomeric electrolytes govern the stable operation of solid-state lithium metal batteries (LMBs). Enhancing the electrolyte’s mechanical integrity is essential to accommodate the substantial volume change of the lithium (Li) metal anode, particularly under high-loading cathode configurations and low-temperature conditions. By tuning the crosslinking density, we systematically modulate mechanical stretchability, resilience, and interfacial adhesion while preserving electrochemical properties, enabled by a bicontinuous microstructure. An optimized crosslinking density that balances strain accommodation, elastic recovery, and adhesion enables stable cycling of Li|NCM811 full cells at 25 °C. Finally, we elucidate how these mechanical factors correlate with full-cell performance at −10 °C, offering practical design guidelines for elastomeric electrolytes in solid-state LMBs.