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<p>Lithium||sulfur batteries promise high energy density but are plagued by sluggish polysulfide conversion under lean-electrolyte conditions. Here we show the formation of chiral LiPS-LiTFSI dimers, fundamentally reshaping the intrinsic chemistry of polysulfides. Building on this finding, we design biomimetic MOF catalysts (MOF-L-His-Cu) in which L-histidine-Cu centers selectively recognize the chiral dimers, accelerating sulfur redox via enzyme-like kinetics. Such MOF-L-His-Cu catalyst achieves 1.84-fold higher activity than its D-enantiomer, enabling lithium||sulfur pouch cells with specific energy of 408 Wh kg<sup>−1</sup> (based on the mass of the whole pouch cell deducting the package) at high sulfur loading (12 mg cm<sup>−2</sup>) and low electrolyte/sulfur ratio (3 μL mg<sup>−1</sup>). Our findings suggest that chiral coordination could be a previously overlooked factor in lithium||sulfur chemistry. This insight may inform the design of selective electrocatalysts for next-generation energy storage, representing a potential step forward in the field.</p>

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Chiral LiPS–LiTFSI dimers enabling biomimetic electrocatalysis in lithium||sulfur batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月5日

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  • Yangyang Dong,
  • Dong Cai,
  • Hongtian Ning,
  • Meiling Shu,
  • Haijin Ni,
  • Shuo Yang,
  • Xuemei Zhou,
  • Huagui Nie,
  • Haoran Tu,
  • Chenghua Sun,
  • Songbai Han,
  • Zhi Yang

摘要

Lithium||sulfur batteries promise high energy density but are plagued by sluggish polysulfide conversion under lean-electrolyte conditions. Here we show the formation of chiral LiPS-LiTFSI dimers, fundamentally reshaping the intrinsic chemistry of polysulfides. Building on this finding, we design biomimetic MOF catalysts (MOF-L-His-Cu) in which L-histidine-Cu centers selectively recognize the chiral dimers, accelerating sulfur redox via enzyme-like kinetics. Such MOF-L-His-Cu catalyst achieves 1.84-fold higher activity than its D-enantiomer, enabling lithium||sulfur pouch cells with specific energy of 408 Wh kg−1 (based on the mass of the whole pouch cell deducting the package) at high sulfur loading (12 mg cm−2) and low electrolyte/sulfur ratio (3 μL mg−1). Our findings suggest that chiral coordination could be a previously overlooked factor in lithium||sulfur chemistry. This insight may inform the design of selective electrocatalysts for next-generation energy storage, representing a potential step forward in the field.