Solid-state electrolytes are widely expected to enhance the performance of lithium-ion batteries, providing higher energy density and improved safety. However, challenges still need to be solved in their practical application due to low ionic conductivity and high interfacial resistance at room temperature. In this study, we successfully developed a high-performance gel polymer electrolyte (GPEs) by blending poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP) and polyacrylonitrile (PAN) through UV curing, cross-linking with ethoxylated trimethylolpropane triacrylate (ETPTA), and incorporating Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO). At room temperature, the ionic conductivity of the GPEs was 2.8 × 10⁻⁴ S/cm, with a lithium-ion transference number of 0.6. Moreover, during lithium plating/stripping tests, the assembled Li/PPEL/Li symmetric cell exhibited stable cycling for up to 600 h at a current density of 0.1 mA/cm². Notably, the GPEs enabled the LiFePO₄/GPEs/Li battery to achieve excellent performance, delivering high discharge capacities at room temperature (164.3 mAh g⁻¹ at 0.1 C and 88.8 mAh g⁻¹ at 1 C), with a capacity retention of 89.4% after 200 cycles at 0.5 C. Therefore, solid-state batteries using this electrolyte exhibit excellent performance, including adequate capacity and cycling stability.

Gel electrolytes (GEs) play a pivotal role in the advancement of lithium metal batteries by offering high energy density and enhanced rate capability. Nevertheless, their real-world application is hampered by relatively low ionic conductivity and significant interfacial resistance at room temperatures. In this work, we developed a gel electrolyte membrane (GEM) by embedding Zeolitic Imidazolate Framework-8 (ZIF-8) metal–organic frameworks (MOFs) material into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix through UV curing. The composite membrane, with 4 wt% ZIF-8, exhibited an ionic conductivity of 1.17 × 10⁻³ S/cm, an electrochemical stability window of 4.7 V, and a lithium-ion transference number of 0.7. The test results indicate that the electrochemical performance of LFP//GEM//Li battery has an initial specific capacity of 168 mAh g⁻¹ at 0.1 C rate. At 1 C, the discharge capacity was 88 mAh g⁻¹, and at 2 C, it was 68 mAh g⁻¹. Enhanced ionic transport, improved electrochemical stability, and optimized lithium-ion migration collectively contributed to superior rate performance and prolonged cycle life. This study offers novel insights and methodological advances for next-generation lithium metal batteries technologies.

Liquid electrolytes in conventional lithium-ion batteries pose safety risks associated with flammability, leakage, and explosion, whereas solid polymer electrolytes are generally limited by insufficient ionic conductivity at ambient temperature, restricting the development of high-energy lithium batteries. To address these issues, flexible poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based gel polymer electrolyte membranes (GPEs) were prepared via a slit-coating process combined with UV curing. NASICON-type lithium aluminum titanium phosphate (Li_1.3Al_0.3Ti_1.7P₃O₁₂, LATP) and garnet-type tantalum-doped lithium lanthanum zirconate (Li_6.4La₃Zr_1.4Ta_0.6O₁₂, LLZTO) were introduced as inorganic ceramic fillers to improve the ion-transport and interfacial properties of the GPE. Among the investigated samples, the PVDF-HFP-based GPE containing 10 wt% LLZTO exhibited the best overall performance, with an ionic conductivity of 3.40 × 10⁻⁴ S·cm⁻¹ at ambient temperature and a Li⁺ transference number of 0.77. Cyclic voltammetry results showed that the LLZTO-modified electrolyte membrane exhibited sharper and more symmetric redox peaks, higher peak current response, and better curve overlap during repeated cycles, indicating improved electrochemical reversibility and interfacial stability. In addition, LLZTO incorporation enhanced the mechanical strength, broadened the electrochemical stability window, and improved the flame-retardant behavior of the membrane. The LiFePO₄/GPE/Li cell assembled with the optimized membrane delivered an initial discharge capacity of 160 mAh·g⁻¹ at 0.1 C and maintained 80 mAh·g⁻¹ at 1 C, demonstrating good rate capability. Moreover, a capacity retention of 96% was maintained after 100 cycles at 0.1 C, confirming excellent cycling stability. Therefore, this work provides an effective strategy for the structural optimization and scalable preparation of high-performance gel polymer electrolyte membranes for lithium battery applications.