The routine PP separators used were Celgard 2400. The Al-doped Li6.75La3Zr1.75Ta0.25O12 (LLZTO) powders were purchased from WuXi Kai-Star Electro-Optic Materials Co. Ltd and ball milled before use. First, LLZTO powders were dispersed in THF solvent with a concentration of around 5.0 mg ml−1. The suspension was sonicated for 4 hours and centrifuged at 500 rpm for 10 min to remove bulk powders. Then, a polyvinylidene fluoride (PVDF) binder was added with the mass ratio of LLZTO and PVDF at 9:1. The LLZTO powders and PVDF binder in THF suspension were coated on one side of the Celgard 2400 separator through vacuum filtration. The composite separators for pouch cells were synthesized by doctor blading after adjusting the viscosity of the suspension. The composite separator was dried at room temperature overnight.

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