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<p>In this study, a novel hybrid gel polymer electrolyte (GPE) was developed using a multi-step strategy involving surface-modified silica nanoparticles and an electrospun polyvinylidene fluoride (PVDF) membrane. Initially, silica nanoparticles were functionalized with (3-chloropropyl) trimethoxysilane (CPTMS), followed by grafting with 1-butyl-3-vinylimidazolium bromide (BVImBr) to form ionic liquid (IL) moieties on the particle surface (SiO<sub>2</sub>@IL). Ion exchange with lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) was then performed to introduce TFSI<sup>−</sup> anions. The resulting IL-functionalized nanoparticles (SiO<sub>2</sub>@IL-TFSI) were immobilized onto the electrospun PVDF membrane via physisorbed free radical polymerization, forming a robust organic–inorganic composite. Finally, the hybrid membrane was soaked in a propylene carbonate/ lithium hexafluorophosphate (PC/LiPF₆) solution to produce the GPE. The hybrid GPE demonstrated high porosity, excellent electrolyte uptake, and improved lithium-ion transport, achieving a room-temperature ionic conductivity of 1.76 mS cm<sup>−1</sup> and an electrochemical stability window of 4.7&#xa0;V. Electrochemical testing revealed enhanced rate capability, with higher discharge capacities retained at increasing C-rates compared to the pristine GPE. After 50 charge–discharge cycles at 0.2&#xa0;C, the hybrid system maintained a capacity retention of 91% with high coulombic efficiency. These results underscore the synergistic effect of the IL-modified nanoparticles and nanofibrous membrane architecture, making the proposed GPE a promising candidate for high-performance lithium-ion batteries (LiBs) with thermo-mechanical stability.</p> Graphical abstract <p></p>

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Hybrid gel polymer electrolyte based on ionic liquid-functionalized SiO2 and electrospun PVDF membrane for high-performance lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2026年3月17日

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  • Seifollah Jamalpour,
  • Amin Rahdari,
  • Ashkan Shekhi

摘要

In this study, a novel hybrid gel polymer electrolyte (GPE) was developed using a multi-step strategy involving surface-modified silica nanoparticles and an electrospun polyvinylidene fluoride (PVDF) membrane. Initially, silica nanoparticles were functionalized with (3-chloropropyl) trimethoxysilane (CPTMS), followed by grafting with 1-butyl-3-vinylimidazolium bromide (BVImBr) to form ionic liquid (IL) moieties on the particle surface (SiO2@IL). Ion exchange with lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) was then performed to introduce TFSI− anions. The resulting IL-functionalized nanoparticles (SiO2@IL-TFSI) were immobilized onto the electrospun PVDF membrane via physisorbed free radical polymerization, forming a robust organic–inorganic composite. Finally, the hybrid membrane was soaked in a propylene carbonate/ lithium hexafluorophosphate (PC/LiPF₆) solution to produce the GPE. The hybrid GPE demonstrated high porosity, excellent electrolyte uptake, and improved lithium-ion transport, achieving a room-temperature ionic conductivity of 1.76 mS cm−1 and an electrochemical stability window of 4.7 V. Electrochemical testing revealed enhanced rate capability, with higher discharge capacities retained at increasing C-rates compared to the pristine GPE. After 50 charge–discharge cycles at 0.2 C, the hybrid system maintained a capacity retention of 91% with high coulombic efficiency. These results underscore the synergistic effect of the IL-modified nanoparticles and nanofibrous membrane architecture, making the proposed GPE a promising candidate for high-performance lithium-ion batteries (LiBs) with thermo-mechanical stability.

Graphical abstract