Shining light on fillers uniform dispersion of PVDF/garnet composite electrolytes for high‐performance solid‐state Li batteries: fundamentals, progress and perspectives

Abstract Polyvinylidene fluoride (PVDF)/garnet composite polymer electrolytes (CPEs) have shown great potential in the development of solid‐state lithium metal batteries (SSLMBs) due to their excellent flexibility, high ionic conductivity and superior mechanical strength. However, uneven dispersion of garnet fillers in CPEs would lead to deterioration of lithium metal batteries (LMBs) performance and severely limit their widespread application. Considering the rapidly growing research of addressing above‐mentioned issue, herein, recent progress in the design and fabrication of uniformly dispersed fillers in PVDF/garnet CPEs for high‐performance SSLMBs is summarized. We firstly analyze the mechanism for the aggregation of inorganic fillers, and provide a detailed introduction to the strategies for solving the uneven dispersion of nanoparticles in solid electrolytes. Moreover, we also comprehensively summarize their applications in PVDF/garnet electrolytes and their impact on the electrochemical performance of SSLMBs. Finally, the application challenges and future prospects of PVDF/garnet CPEs in SSLMBs were also proposed to promote their further development. It is anticipated that this review could inspire ongoing research interest in rational designing and fabricating novel CPEs for high‐performance SSLMBs.