Topological Vulcanization Strategy for Elastomeric Electrolytes with Enhanced Mechanical and Electrochemical Properties for Advanced Lithium Metal Batteries

Abstract Elastomeric electrolytes (EEs) have garnered significant attention in the realm of next‐generation energy storage systems, attributed to their distinctive mechanical properties. Nonetheless, achieving precise modulation of mechanical robustness while ensuring efficient lithium‐ion transport continues to present a significant challenge. In this study, an innovative topological vulcanization strategy is proposed to fabricate uniformly crosslinked EEs. The resultant EEs demonstrate exceptional mechanical properties, characterized by a tensile strength of 3.51 MPa and an elongation at break of 832%, alongside a room‐temperature ionic conductivity of 4 × 10 ⁻⁴ S cm ⁻¹ . Such robust and flexible electrolytes maintain superior structural integrity throughout battery operation. This approach enables stable cycling for more than 3000 h in lithium symmetric cells and achieves 95.7% capacity retention after 500 cycles at a rate of 0.5C in full cells. They also exhibit consistent and dependable performance in stretchable and pouch cells even under significant deformations, thereby confirming their suitability for advanced flexible energy storage applications.