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<p>Hybrid solid electrolytes (HSEs), which combine inorganic fillers with polymer matrices, are promising candidates for next-generation lithium-ion batteries due to their enhanced safety and stability. However, achieving both mechanical durability and flame retardancy remains a significant challenge. In this study, a dip-coated HSE (D-HSE) is fabricated by applying a thin ceramic layer onto an aligned electrospun polyacrylonitrile (PAN) nanofiber scaffold. The aligned PAN scaffold exhibits higher tensile strength than random fibers. The uniform LLZO layer acts as a mechanical reinforcement and thermal barrier, preventing direct contact between PAN and lithium while enhancing Li-ion transport and flame resistance. The dip-coating process enables uniform ceramic deposition without increasing separator thickness, thereby ensuring both mechanical integrity and efficient ion transport. Electrochemical evaluations reveal that the D-HSE exhibited a wide electrochemical stability window, high ionic conductivity, and a favorable lithium-ion transference number. It demonstrates stable cycling, high critical current density, and effective dendrite suppression in Li||Li symmetric cells and Li||NCM811 half-cells. Furthermore, Graphite||LFP pouch cell testing confirms its stability under practical conditions. This study presents a design strategy for hybrid solid electrolytes that combines high performance and practical feasibility through a simple fabrication process based on aligned nanofiber architecture and uniform ceramic coating.</p>

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Aligned electrospun polyacrylonitrile nanofibers coated with Li7La3Zr2O12 solid electrolytes for mechanically robust and flame-retardant membranes

  • 期刊论文

  • 发表日期：

    2025年12月22日

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  • Heesu Kim,
  • Youngmin Moon,
  • Chi Keung Song,
  • Woo-jin Song,
  • Sangbaek Park

摘要

Hybrid solid electrolytes (HSEs), which combine inorganic fillers with polymer matrices, are promising candidates for next-generation lithium-ion batteries due to their enhanced safety and stability. However, achieving both mechanical durability and flame retardancy remains a significant challenge. In this study, a dip-coated HSE (D-HSE) is fabricated by applying a thin ceramic layer onto an aligned electrospun polyacrylonitrile (PAN) nanofiber scaffold. The aligned PAN scaffold exhibits higher tensile strength than random fibers. The uniform LLZO layer acts as a mechanical reinforcement and thermal barrier, preventing direct contact between PAN and lithium while enhancing Li-ion transport and flame resistance. The dip-coating process enables uniform ceramic deposition without increasing separator thickness, thereby ensuring both mechanical integrity and efficient ion transport. Electrochemical evaluations reveal that the D-HSE exhibited a wide electrochemical stability window, high ionic conductivity, and a favorable lithium-ion transference number. It demonstrates stable cycling, high critical current density, and effective dendrite suppression in Li||Li symmetric cells and Li||NCM811 half-cells. Furthermore, Graphite||LFP pouch cell testing confirms its stability under practical conditions. This study presents a design strategy for hybrid solid electrolytes that combines high performance and practical feasibility through a simple fabrication process based on aligned nanofiber architecture and uniform ceramic coating.