Imidazolium-Type Poly(ionic liquid) Endows the Composite Polymer Electrolyte Membrane with Excellent Interface Compatibility for All-Solid-State Lithium Metal Batteries

Developing a poly(ethylene oxide) (PEO)-based polymer electrolyte with high ionic conductivity and robust mechanical property is beneficial for real applications of all-solid-state lithium metal batteries (ASSLMBs). Herein, an excellent organic/inorganic interface compatibility of all-solid-state composite polymer electrolytes (CPEs) is achieved using a novel imidazolium-type poly(ionic liquid) with strong electrostatic interactions, providing insights into the achievement of highly stable CPEs. The key properties such as micromorphologies, thermal behavior, crystallinity, t_Li⁺, mechanical property, lithium anode surficial morphology, and electrochemical performance are systematically investigated. The combined experimental and density functional theory (DFT) simulation results exhibit that the strong electrostatic interaction and ion-dipole interaction cooperated to improve the compatibility of the CPE, with a high ionic conductivity of 1.46 × 10^-4 S cm^-1 at 40 °C and an incredible mechanical strain of 2000% for dendrite-free and highly stable all-solid-state LMBs. This work affords a promising strategy to accelerate the development of PEO-based polymer electrolytes for real applications in ASSLMBs.