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<p>Lithium–sulfur batteries promise high energy density storage but show poor stabilities owing to uncontrolled polysulfide dissolution. Although limiting polysulfide solvation to establish quasi-solid-state sulfur reaction can decouple electrode reactions from the electrolyte volume, this approach suffers from slow reaction kinetics. Here we propose a surface-localized polysulfide-solvation strategy to mediate the reaction of ‘quasi-solid’ polysulfide by leveraging an organic phase mediator with a weakly solvating electrolyte. This electrolyte restricts polysulfide dissolution globally while the phase mediator complexes with the surface polysulfide, promoting polysulfide solvation at the surface and facilitating fast surface-localized solution-phase sulfur reactions. Lithium–sulfur batteries using surface-localized phase mediation show excellent rate performance with 494 mA h g<sup>−</sup><sup>1</sup><sub>-sulfur</sub> at 16 C and stabilized cycling for 300 cycles with 90.2% capacity retention. The strategy enables steady operation of a 2.4 Ah 331 Wh kg<sup>−</sup><sup>1</sup> pouch cell. Our work highlights the advantages of surface phase mediation in controlling electrode reaction pathways and kinetics via electrolyte rational design.</p><p></p>

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Surface-localized phase mediation accelerates quasi-solid-state reaction kinetics in sulfur batteries

  • 期刊论文

  • 发表日期：

    2025年2月13日

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  • Yatao Liu,
  • Yun An,
  • Chi Fang,
  • Yaokun Ye,
  • Yifeng An,
  • Mengxue He,
  • Yongfeng Jia,
  • Xufeng Hong,
  • Yumei Liu,
  • Song Gao,
  • Yizhou Hao,
  • Jianhao Chen,
  • Jiaxin Zheng,
  • Yunfeng Lu,
  • Ruqiang Zou,
  • Quanquan Pang

摘要

Lithium–sulfur batteries promise high energy density storage but show poor stabilities owing to uncontrolled polysulfide dissolution. Although limiting polysulfide solvation to establish quasi-solid-state sulfur reaction can decouple electrode reactions from the electrolyte volume, this approach suffers from slow reaction kinetics. Here we propose a surface-localized polysulfide-solvation strategy to mediate the reaction of ‘quasi-solid’ polysulfide by leveraging an organic phase mediator with a weakly solvating electrolyte. This electrolyte restricts polysulfide dissolution globally while the phase mediator complexes with the surface polysulfide, promoting polysulfide solvation at the surface and facilitating fast surface-localized solution-phase sulfur reactions. Lithium–sulfur batteries using surface-localized phase mediation show excellent rate performance with 494 mA h g−1-sulfur at 16 C and stabilized cycling for 300 cycles with 90.2% capacity retention. The strategy enables steady operation of a 2.4 Ah 331 Wh kg−1 pouch cell. Our work highlights the advantages of surface phase mediation in controlling electrode reaction pathways and kinetics via electrolyte rational design.