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<p>Lithium metal batteries (LMBs) are promising candidates for next-generation energy storage systems due to their high theoretical energy density. However, lithium dendrite growth and safety concerns remain critical challenges. To address these issues, we propose a novel gel polymer electrolyte (GPE) design strategy by coating a PEGDE/PEA-based crosslinked polymer (PEGA) electrolyte onto a commercial polypropylene (PP) separator, which serves as a structural substrate. The PEGA gel polymer electrolyte exhibited enhanced mechanical properties, representing an improvement of 15% compared to the bare PP separator, and demonstrated excellent flame retardancy as confirmed by the self-extinguishing time (SET) test. Furthermore, the PEGA polymer matrix coordinates with Li<sup>+</sup> to form direct ion transport pathways, achieving enhanced ionic conductivity (1.02 mS/cm) and a high Li<sup>+</sup> transference number (0.602) compared to the liquid electrolyte (LE, 0.358). As a result, the PEGA gel polymer electrolyte demonstrated stable cycling for over 500&#xa0;h and effective dendrite suppression in the Li||Li symmetric cell test. Moreover, the Li||NCM622 cells employing the PEGA gel polymer electrolyte achieved a high capacity retention of 97.54% after 50 cycles, demonstrating its practical applicability in battery systems.</p> Graphical Abstract <p></p>

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Uniform Li+ transport in a flame-retardant 3D crosslinked gel polymer electrolyte for safe lithium metal batteries

  • 期刊论文

  • 发表日期：

    2026年6月15日

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  • Sanghyeon Woo,
  • Chi Keung Song,
  • Yurim Lee,
  • Woo-Jin Song

摘要

Lithium metal batteries (LMBs) are promising candidates for next-generation energy storage systems due to their high theoretical energy density. However, lithium dendrite growth and safety concerns remain critical challenges. To address these issues, we propose a novel gel polymer electrolyte (GPE) design strategy by coating a PEGDE/PEA-based crosslinked polymer (PEGA) electrolyte onto a commercial polypropylene (PP) separator, which serves as a structural substrate. The PEGA gel polymer electrolyte exhibited enhanced mechanical properties, representing an improvement of 15% compared to the bare PP separator, and demonstrated excellent flame retardancy as confirmed by the self-extinguishing time (SET) test. Furthermore, the PEGA polymer matrix coordinates with Li+ to form direct ion transport pathways, achieving enhanced ionic conductivity (1.02 mS/cm) and a high Li+ transference number (0.602) compared to the liquid electrolyte (LE, 0.358). As a result, the PEGA gel polymer electrolyte demonstrated stable cycling for over 500 h and effective dendrite suppression in the Li||Li symmetric cell test. Moreover, the Li||NCM622 cells employing the PEGA gel polymer electrolyte achieved a high capacity retention of 97.54% after 50 cycles, demonstrating its practical applicability in battery systems.

Graphical Abstract