| Summary: | Poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based gel polymer electrolytes (GPEs) are considered a promising electrolyte candidate for polymer lithium-ion batteries (LIBs) because of their free-standing shape, versatility, security, flexibility, lightweight, reliability, and so on. However, due to problems such as low ionic conductivity, PVDF-HFP can only be used on a small scale when used as a substrate alone. To overcome the above shortcomings, GPEs were designed and synthesized by a UV curing process by adding NASICON-type Li<sub>1.5</sub>Al<sub>0.5</sub>Ge<sub>1.5</sub>(PO<sub>4</sub>)<sub>3</sub> (LAGP) and garnet-type Li<sub>6.46</sub>La<sub>3</sub>Zr<sub>1.46</sub>Ta<sub>0.54</sub>O<sub>12</sub> (LLZTO) to PVDF-HFP. Experimentally, GPEs with 10% weight LLZTO in a PVDF-HFP matrix had an ionic conductivity of up to 3 × 10<sup>−4</sup> S cm<sup>−1</sup> at 25 °C. When assembled into LiFePO<sub>4</sub>/GPEs/Li batteries, a discharge-specific capacity of 81.5 mAh g<sup>−1</sup> at a current density of 1 C and a capacity retention rate of 98.1% after 100 cycles at a current density of 0.2 C occurred. Therefore, GPEs added to LLZTO have a broad application prospect regarding rechargeable lithium-ion batteries.
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