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Achieving high ionic conductivity, wide voltage window, and good mechanical strength in a single material remains a key challenge for polymer-based electrolytes for use in solid-state supercapacitors (SCs). Herein, we report cross-linked composite gel polymer electrolytes (CGPEs) based on multi-cross-linkable H-shaped poly(ethylene oxide)-poly(propylene oxide) (PEO-PPO) tetrablock copolymer precursors, SiO 2 nanoparticles, and 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, an ionic liquid (IL). Self-standing CGPE membranes with a high IL content were prepared using in situ cross-linking reactions between the silane groups present in the precursor and the SiO 2 surface. The incorporation of an optimal amount of SiO 2 increased the cross-linking density of the resulting CGPE while reducing polymer-chain ordering and, consequently, increasing both ionic conductivity and mechanical strength. As a result, the CGPE with 0.1 wt % SiO 2 exhibited a high ionic conductivity (2.22 × 10 -3 S cm -1 at 25 °C), good tensile strength (453 kPa), and high thermal stability up to 330 °C. Finally, an all-solid-state SC assembled with the prepared CGPE showed a high operating voltage (3 V), a large specific capacitance (103.9 F g -1 at 1 A g -1 ), and excellent durability (94% capacitance retention over 10,000 charge/discharge cycles), which highlights its strong potential as a solid-state electrolyte for SCs.

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Cross-Linked Composite Gel Polymer Electrolyte Based on an H-Shaped Poly(ethylene oxide)–Poly(propylene oxide) Tetrablock Copolymer with SiO<sub>2</sub> Nanoparticles for Solid-State Supercapacitor Applications

Cross-Linked Composite Gel Polymer Electrolyte Based on an H-Shaped Poly(ethylene oxide)–Poly(propylene oxide) Tetrablock Copolymer with SiO2 Nanoparticles for Solid-State Supercapacitor Applications

Cross-Linked Composite Gel Polymer Electrolyte Based on an H-Shaped Poly(ethylene oxide)–Poly(propylene oxide) Tetrablock Copolymer with SiO₂ Nanoparticles for Solid-State Supercapacitor Applications