Photo and thermal crosslinked poly(vinyl alcohol)-based nanofiber membrane for flexible gel polymer electrolyte

Novel dual crosslinked nanofibrous membranes (DCNMs) were fabricated by a combination of UV-photocrosslinking and thermal sol-gel crosslinking procedures and used as a matrix for gel polymer electrolytes for lithium-ion batteries (LIBs). Flexible nanofibrous membranes were obtained from the solution of poly(vinyl alcohol) (PVA), maleated PVA (PVA-MA), polyethylene glycol diacrylate (PEGDA), and tetraethyl orthosilicate (TEOS) by electrospinning technique. As a matrix for gel polymer electrolyte (GPE), it showed significantly higher ionic conductivity of 1.98 × 10⁻³ S cm⁻¹ than the commercial separators and pure PVDF based GPE. Incorporation of TEOS into the membrane composition, and formation of siloxane bonds (Si–O–Si) greatly increased the conductivity providing excellent mechanical and thermal stability. The assembled lithium metal cell with LiFePO₄ cathode exhibited excellent cycling performance and delivered a high reversible capacity of 133 mA h g⁻¹ at 0.1 C and retained 87% of the initial discharge capacity after 150 cycles with a stable coulombic efficiency near 100%. The GPE could substantially suppressed the growth of Li dendrites during the stably cycles up to 1000 h, while the cell with the commercial separator failed within 800 h. In consequence, this novel DCNM possesses a potential for application in flexible and safe Li-ion and Li-metal batteries.