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<p>Solid-state electrolytes are crucial for developing next-generation batteries with enhanced safety and energy density. Among them, the polymethyl methacrylate (PMMA)-based gel polymer electrolytes (GPEs) have emerged as promising materials for high-performance battery systems. However, PMMA-based electrolytes suffer from intrinsically low ionic conductivity. While blending with quaternary ammonium salts offers an effective solution, it often leads to salt deposition during cycling, compromising long-term stability. In this work, a novel GPE is developed by grafting long-chain quaternary ammonium salt (C<sub>16</sub>DMAAC) onto the PMMA backbone. This molecular design simultaneously regulates polymer chain disorder and immobilizes free anions, enabling a high Li-ion transfer number of 0.59, ionic conductivity of 7.23 × 10<sup>−4</sup> S/cm, and an expanded electrochemical stability window of 4.9 V. Moreover, the incorporated ammonium cations in the C<sub>16</sub>DMAAC segment optimize the Li<sup>+</sup> solvation structure, promoting the formation of a robust, inorganic-rich solid electrolyte interphase (SEI). The excellent cycling stability is demonstrated by the Li∥NCM811 full cell, which retains 92% of its initial capacity over 200 cycles at 0.5 C, and 80% retention after 300 cycles at 2 C. This work presents a promising strategy for designing novel electrolyte structures by grafting quaternary ammonium salts into polymer chains to improve battery stability and lifespan.</p>

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A novel design of C16DMAAC-modified solid-state polymer electrolyte reinforcing battery stability and lifetime

  • 期刊论文

  • 发表日期：

    2026年1月1日

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  • Dong Yang,
  • Shifeng Zhang,
  • Daiman Zhu,
  • Xueling Liu,
  • Yan Chai,
  • Rui Gao,
  • Liang Wang,
  • Yongli Li

摘要

Solid-state electrolytes are crucial for developing next-generation batteries with enhanced safety and energy density. Among them, the polymethyl methacrylate (PMMA)-based gel polymer electrolytes (GPEs) have emerged as promising materials for high-performance battery systems. However, PMMA-based electrolytes suffer from intrinsically low ionic conductivity. While blending with quaternary ammonium salts offers an effective solution, it often leads to salt deposition during cycling, compromising long-term stability. In this work, a novel GPE is developed by grafting long-chain quaternary ammonium salt (C16DMAAC) onto the PMMA backbone. This molecular design simultaneously regulates polymer chain disorder and immobilizes free anions, enabling a high Li-ion transfer number of 0.59, ionic conductivity of 7.23 × 10−4 S/cm, and an expanded electrochemical stability window of 4.9 V. Moreover, the incorporated ammonium cations in the C16DMAAC segment optimize the Li+ solvation structure, promoting the formation of a robust, inorganic-rich solid electrolyte interphase (SEI). The excellent cycling stability is demonstrated by the Li∥NCM811 full cell, which retains 92% of its initial capacity over 200 cycles at 0.5 C, and 80% retention after 300 cycles at 2 C. This work presents a promising strategy for designing novel electrolyte structures by grafting quaternary ammonium salts into polymer chains to improve battery stability and lifespan.