In Situ Constructing Ultrathin, Robust-Flexible Polymeric Electrolytes with Rapid Interfacial Ion Transport in...

Safety of lithium metal batteries (LMBs) has been improved by using the solid-state polymer electrolytes, but the performance of LMBs is still troubled by the poor interface of solid electrolytes/electrodes, leading to insufficient interfacial Li⁺ transport. Here, a novel ultrathin, robust-flexible polymeric electrolyte is achieved by in situ polymerization of 1,3-dioxolane in soft nanofibrous skeleton at room temperature without any extra initiator or plasticizer, leading to the electrolyte with rapid interfacial ion transport. This facilitated Li⁺ transportation is demonstrated by molecular dynamics simulation. Consequently, the as-prepared electrolyte exhibits excellent cycling performance. The results indicate that the electrolyte works well in the LiFePO₄ //Li cell at elevated temperature up to 90 °C, and further matches with the high-voltage LiNi_0.8 Mn_0.1 Co_0.1 O₂ cathode. This study provides an effective approach to constructing a practical polymeric electrolyte for fabrication of safe, high performance LMBs.