Abstract
Solid polymer electrolytes show great application potential in the next-generation all-solid-state Li-ion batteries due to its safety, electrochemical stability, and easy-processing feature. However, low ionic conductivity of solid polymer electrolytes hinders their commercialization. Currently, dispersing ceramic fillers in polymer electrolytes has been proved to be a promising approach to address this issue. Herein, we introduce Li6.75La3Zr1.75Ta0.25O12 fillers into polyacrylonitrile-LiClO4 matrix and study the effects of Li6.75La3Zr1.75Ta0.25O12 on chemical and electrochemical properties of the polyacrylonitrile-based electrolytes. The addition of Li6.75La3Zr1.75Ta0.25O12 triggers the cyclization and segmentation of polyacrylonitrile chains, which improves the mechanical strength and thermal stability of the electrolytes. The effects of Li6.75La3Zr1.75Ta0.25O12 on the electrochemical properties of the electrolytes are thoroughly investigated. The polyacrylonitrile-based electrolyte with 20 wt% Li6.75La3Zr1.75Ta0.25O12 fillers shows a high ionic conductivity of 2.2 × 10−4 S cm−1 at 40 °C, a wide electrochemical window of 4.9 V, and much improved Li+ transference number and cycling stability in a Li||Li symmetric cell. In addition, a solid-state LiFePO4||Li full cell is assembled and tested at room temperature, demonstrating the applicability of polyacrylonitrile-based electrolytes in all-solid-state batteries.
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