Realization of Enhanced Interfacial Lithium-Ion Transfer in Composite Polymer Electrolytes via Grafting Oligo-PEG Molecular Brushes on Silica-Coated Nanofibers for All-Solid-State Lithium Metal Batteries

Polyether-based polymer electrolytes are attractive but still challenging for high-energy-density solid-state lithium metal batteries due to their limited Li-ion conductivity at room temperature. Herein, an oligomeric polyethylene glycol methyl ether methacrylate (PEGMEM)-modified silica-coated polyimide fibrous scaffold (PINF@PEGMEM-SiO2) was introduced in polyethylene glycol dimethyl ether (PEGDME) to enhance the Li-ion transportation at room temperature. PINF@PEGMEM-SiO2 was developed to build a continuous and interconnected interface for continuous Li-ion transportation in bulk. The carbonyl groups (C═O) of PEGMEM on SiO2 can promote the dissociation of lithium salts and enhance the migration of free Li ions at the interface. The same −C–C-O− unit contained in both PEGMEM and PEGDME ensures the compatibility of PEGMEM at the interface and PEGDME in the bulk. The prepared PEGDME-based polymer electrolyte exhibits a high ionic conductivity of 1.14 × 10–4 S cm–1 at 25 °C and an improved Li-ion transference number of 0.41. Furthermore, LiFePO4/Li and LiNi0.8Co0.1Mn0.1O2/Li cells with excellent cyclability and rate capability at ambient temperature are obtained.