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

Small Methods. 2022 Dec;6(12):e2201114. doi: 10.1002/smtd.202201114. Epub 2022 Nov 6.

Abstract

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 LiNi0.8 Mn0.1 Co0.1 O2 cathode. This study provides an effective approach to constructing a practical polymeric electrolyte for fabrication of safe, high performance LMBs.

Keywords: Li metal batteries; diffusion coefficients; in situ polymerization; robust-flexible polymeric electrolytes; ultrathin nanofibrous films.