Polycarbonate-based composite polymer electrolytes with Al2O3 enhanced by in situ polymerized electrolyte Interlayers for all-solid-state lithium-metal batteries

Lithium-metal batteries (LMBs) have attracted significant attention as promising energy storage devices due to their high energy density. However, the practical application of LMBs is hindered by issues such as dendrite growth and electrolyte decomposition, which lead to poor cycling stability. To address these challenges, this study focuses on investigating the performance of poly(ethylene carbonate) (PEC)-based composite polymer electrolytes (CPEs) with an in situ polymerized poly(vinyl ethylene carbonate) (PVEC)-based electrolyte interlayer. The electrolytes were optimized by incorporating lithium bis(fluorosulfonyl)imide (LiFSI) salt, lithium bis(oxalato)borate (LiBOB) and lithium nitrate (LiNO3) additives, as well as Al2O3 filler. The objective was to improve the compatibility and cycling stability of LMBs by enhancing the electrolyte/electrode interfacial properties. Remarkably, the Li||Li symmetric cell utilizing the optimized CPE exhibited outstanding stability, operating for 700 h without short-circuiting at 0.1 mA cm−2, indicating excellent interfacial compatibility. Additionally, the Li||LiFePO4(LFP) cells using the same electrolyte demonstrated impressive performance, delivering initial discharge capacity of 159.32 mAh g−1 at 0.1 C with retention and coulombic efficiency close to 100 % after 100 cycles at 60 °C. This paper highlights the effectiveness of utilizing polymer electrolyte interlayers and additives like LiNO3 in CPEs to enhance the interfacial compatibility and cycling stability of LMBs.