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<p>Developing advanced gel polymer electrolytes (GPEs) with high ionic conductivity and thermal stability is crucial for next-generation lithium-ion batteries. In this study, a zwitterionic polyurethane was synthesized via a two-step process using polycaprolactone (PCL), methylene diphenyl diisocyanate (MDI), butanediol (BDO), and methyldiethanolamine (MDEA), and subsequently functionalized with propane sultone (PS) to introduce sulfonate groups. Silica (SiO₂) nanoparticles were incorporated to form nanocomposite membranes, which were then processed via phase inversion and activated with a liquid electrolyte to generate porous GPEs. Structural, thermal, mechanical, and electrochemical properties of the membranes were systematically characterized. The presence of sulfonate and hydroxyl-rich silica groups enhanced Li⁺ion coordination, increased porosity, and improved electrolyte uptake. The optimized composite (CGPE2-1) with 1 wt% SiO₂ exhibited an electrochemical stability window up to 4.8&#xa0;V and ionic conductivity of 1.58 mS·cm⁻¹ at room temperature. Electrochemical performance tests conducted in Li/LiFePO₄ half-cells demonstrated excellent cycling stability, with the GPE-based cell retaining 91.7% of its initial capacity (128.3 mAh·g⁻¹) after 50 cycles and achieving a coulombic efficiency of 97.3%. The membrane also showed good mechanical integrity. These results highlight the potential of this zwitterionic polyurethane/silica GPE for safe and efficient lithium-ion energy storage systems.</p>

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Designing sulfonated polyurethane-based membranes with SiO₂ nanoparticles: toward high-performance porous gel polymer electrolytes for lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2026年2月11日

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  • Seyed Masoud Nasirzade,
  • Roghayeh Maghsoudi,
  • Seyed Reza Ghaffarian,
  • Seifollah Jamalpour

摘要

Developing advanced gel polymer electrolytes (GPEs) with high ionic conductivity and thermal stability is crucial for next-generation lithium-ion batteries. In this study, a zwitterionic polyurethane was synthesized via a two-step process using polycaprolactone (PCL), methylene diphenyl diisocyanate (MDI), butanediol (BDO), and methyldiethanolamine (MDEA), and subsequently functionalized with propane sultone (PS) to introduce sulfonate groups. Silica (SiO₂) nanoparticles were incorporated to form nanocomposite membranes, which were then processed via phase inversion and activated with a liquid electrolyte to generate porous GPEs. Structural, thermal, mechanical, and electrochemical properties of the membranes were systematically characterized. The presence of sulfonate and hydroxyl-rich silica groups enhanced Li⁺ion coordination, increased porosity, and improved electrolyte uptake. The optimized composite (CGPE2-1) with 1 wt% SiO₂ exhibited an electrochemical stability window up to 4.8 V and ionic conductivity of 1.58 mS·cm⁻¹ at room temperature. Electrochemical performance tests conducted in Li/LiFePO₄ half-cells demonstrated excellent cycling stability, with the GPE-based cell retaining 91.7% of its initial capacity (128.3 mAh·g⁻¹) after 50 cycles and achieving a coulombic efficiency of 97.3%. The membrane also showed good mechanical integrity. These results highlight the potential of this zwitterionic polyurethane/silica GPE for safe and efficient lithium-ion energy storage systems.