In-situ polymerization of poly(1,3-dioxolane) gel electrolytes modified with LLZTO nanoparticles for high-performance lithium-metal batteries

Gel polymer electrolytes (GPEs) based on poly(1,3-dioxolane) (PDOL) have been developed due to their excellent lithium metal compatibility and convenient in-situ polymerization synthesis. A PDOL-based GPEs is obtained by in-situ polymerization, in which introduce Li6.5La3Zr1.5Ta0.5O12 (LLZTO) solid-state fillers and Succinonitrile (SN) functional additives, named as PDOL-SN/LLZTO. The PDOL-SN/LLZTO exhibits high ionic conductivity of 5.19 x 10-3 S cm-1 and high lithium-ion transference number (tLi+) of 0.79 at room temperature, as well as expanded electrochemical window of 4.85 V. For Li||Li symmetric cells, it achieves stable cycling over 2000 hours at a current density of 0.1 mA cm-2. Benefiting from the enhanced interfacial stability due to LLZTO doping, Li||LiFePO4 cells provide a high initial capacity of 146.3 mAh g-1 at 1C, with a capacity retention of 84.5% after 1000 cycles at 1C. So, the glass fibre-based PDOL provides an important approach and facile strategy for designing high-performance lithium-metal batteries.