Fundamentals and Perspectives of Poly(vinylidene fluoride)-based Electrolytes for Solid-State Lithium Batteries

Solid-state lithium metal batteries are considered as viable energy storage technologies for high-energy-density and safe devices. Recently, poly(vinylidene fluoride) (PVDF)-based solid-state electrolytes with “Li salt-polymer-little bound solvent” configuration attract much attention. However, several dilemmas such as limited ionic conductivity and interfacial reactions with electrodes restrict their further advancement for practical applications. In this review, we summarized the fundamentals of the PVDF-based solid-state electrolytes including the physicochemical properties, the ion transport behavior in electrolytes and batteries, the interfacial chemistry with electrodes, the role of various fillers and the interactions between components in electrolytes to provide an in-depth and comprehensive understanding. Then, we highlighted significant strategies that toward practical applications based on our lab’s results and other publications from four aspects: increasing ionic conductivity of electrolytes, enhancing interfacial stability with electrodes, designing thin and robust electrolytes, building safe and high-energy batteries. At last, we provided our perspectives on the future development directions to push forward practical applications of the PVDF-based solid-state electrolytes.