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<p>High-energy lithium-sulfur (Li-S) batteries are anticipated to be pivotal in next-generation energy storage systems. However, their practical implementation is severely hindered by the shuttling of polysulfides between the sulfur cathode and the lithium metal anode, as well as the safety hazards introduced using liquid electrolytes. To address these challenges, we apply molybdenum disulfide (MoS<sub>2</sub>) interlayer onto a polypropylene (PP) separator via electrostatic spraying, leveraging the Lewis acidity of MoS<sub>2</sub> to initiate the ring-opening polymerization of 1,3-dioxolane. This process effortlessly converts a commercial liquid electrolyte into a gel polymer electrolyte (GPE) before cycling, enhancing battery safety and effectively protecting lithium anodes. Furthermore, the MoS<sub>2</sub> interlayer serves as a critical component in capturing lithium polysulfides during cycling. The GPE demonstrates exceptional performance characteristics: it maintains an ionic conductivity of 7.2 × 10<sup>−4</sup> S cm<sup>−1</sup> at 30 °C, extends an electrochemical window up to 4.7 V, and achieves a high lithium-ion transference number of 0.7. Moreover, the MoS<sub>2</sub>/PP composite separator with the GPE remains stable even at temperatures as high as 200 °C. Consequently, Li-S batteries equipped with GPE display excellent cycle stability, with a capacity retention of 613 mAh g<sup>−1</sup> after 500 cycles at 0.5 C and achieve a high coulombic efficiency of 98.5%. This research offers an effective approach to developing high-performance and safe Li-S batteries.</p>

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A multi-functional separator for quasi-solid-state lithium-sulfur batteries: simultaneously driving in-situ polymerization and capturing polysulfides

  • 期刊论文

  • 发表日期：

    2025年4月28日

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  • Guoxian Wu,
  • Xin Ao,
  • Zhixin Wang,
  • Kangzhe Yu,
  • Yuanyuan He,
  • Deli Xu,
  • Hao Tang,
  • Jie Liu,
  • Bingbing Tian

摘要

High-energy lithium-sulfur (Li-S) batteries are anticipated to be pivotal in next-generation energy storage systems. However, their practical implementation is severely hindered by the shuttling of polysulfides between the sulfur cathode and the lithium metal anode, as well as the safety hazards introduced using liquid electrolytes. To address these challenges, we apply molybdenum disulfide (MoS2) interlayer onto a polypropylene (PP) separator via electrostatic spraying, leveraging the Lewis acidity of MoS2 to initiate the ring-opening polymerization of 1,3-dioxolane. This process effortlessly converts a commercial liquid electrolyte into a gel polymer electrolyte (GPE) before cycling, enhancing battery safety and effectively protecting lithium anodes. Furthermore, the MoS2 interlayer serves as a critical component in capturing lithium polysulfides during cycling. The GPE demonstrates exceptional performance characteristics: it maintains an ionic conductivity of 7.2 × 10−4 S cm−1 at 30 °C, extends an electrochemical window up to 4.7 V, and achieves a high lithium-ion transference number of 0.7. Moreover, the MoS2/PP composite separator with the GPE remains stable even at temperatures as high as 200 °C. Consequently, Li-S batteries equipped with GPE display excellent cycle stability, with a capacity retention of 613 mAh g−1 after 500 cycles at 0.5 C and achieve a high coulombic efficiency of 98.5%. This research offers an effective approach to developing high-performance and safe Li-S batteries.