Improved ionic conductivity and Li dendrite suppression of PVDF-based solid electrolyte membrane by LLZO incorporation and mechanical reinforcement

High room-temperature ionic conductivity and mechanical property are essential for the application of solid electrolyte. In this work, a poly(vinylidene fluoride) (PVDF)-based composite polymer solid electrolyte membrane (CSE) incorporated with Li7La3Zr2O12 (LLZO) fillers and high-strength porous skeleton was prepared. The introduction of LLZO increased the ionic conductivity of PVDF at room temperature by reducing the crystallinity of PVDF matrix, and the addition of skeleton greatly improved the mechanical property of electrolyte membrane and inhibited the growth of lithium dendrites. The prepared PVDF-LLZO CSE has a room-temperature ionic conductivity of 1.75 × 10−4 S/cm, and the tensile strength reaches 95 MPa, which greatly enhanced the ability of lithium dendrite suppression. The assembled LiNi0.6Co0.2Mn0.2O2 (NCM622)/CSE/Li cell shows an initial capacity of 151 mAh/g with a retention capacity of 108 mAh/g after 100 cycles at the current density of 0.5 C. This ultrathin PVDF/LLZO CSE has a great application prospect in solid-state lithium batteries.