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<p>Elucidating the mechanisms governing sulfur redox reactions is important for the development of high-energy-density Li||S batteries. Despite progress, the kinetics of the solid-solid conversion from Li<sub>2</sub>S<sub>2</sub> to Li<sub>2</sub>S remain poorly understood. This work demonstrates that spin-state transitions within reaction intermediates are the key factor of the sluggish kinetics. Guided by density functional theory and machine-learning-assisted catalyst screening, we find a negative correlation between the spin moment of the catalyst and the Gibbs free energy barrier for the Li<sub>2</sub>S<sub>2</sub> to Li<sub>2</sub>S conversion. Among a series of dual-metal doped catalysts, a Co,Ni-doped MoS<sub>2</sub> catalyst, with its high spin moment, modulates the spin states of the reactants, reducing the high free-energy barrier associated with spin-state transitions. Therefore, Li||S batteries incorporating this catalyst show accelerated sulfur conversion, particularly during solid-solid transitions, suppressed polysulfide shuttling, and have stable electrochemical performance. A pouch cell achieves a capacity of 13.2 Ah and a specific energy of 435 Wh kg<sup>-1</sup>. These findings show mechanistic understanding into the role of spin moments in sulfur conversion, enabling to design efficient and durable catalysts for Li||S batteries.</p>

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Breaking the rate limiting barrier in lithium||sulfur batteries via spin state engineering

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月24日

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  • Qingbin Jiang,
  • Huifang Xu,
  • Xinyu Ye,
  • Lingwen Liu,
  • Kwan San Hui,
  • Chao Wu,
  • Kang Gao,
  • Kaitong Sun,
  • Haifeng Li,
  • Yunshan Zheng,
  • Cheng-zong Yuan,
  • Zhongliang Li,
  • Mingdeng Wei,
  • Chenyang Zha,
  • Jie Zeng,
  • Mingkai Liu,
  • Yuanmiao Sun,
  • Hui-Ming Cheng,
  • Kwun Nam Hui

摘要

Elucidating the mechanisms governing sulfur redox reactions is important for the development of high-energy-density Li||S batteries. Despite progress, the kinetics of the solid-solid conversion from Li2S2 to Li2S remain poorly understood. This work demonstrates that spin-state transitions within reaction intermediates are the key factor of the sluggish kinetics. Guided by density functional theory and machine-learning-assisted catalyst screening, we find a negative correlation between the spin moment of the catalyst and the Gibbs free energy barrier for the Li2S2 to Li2S conversion. Among a series of dual-metal doped catalysts, a Co,Ni-doped MoS2 catalyst, with its high spin moment, modulates the spin states of the reactants, reducing the high free-energy barrier associated with spin-state transitions. Therefore, Li||S batteries incorporating this catalyst show accelerated sulfur conversion, particularly during solid-solid transitions, suppressed polysulfide shuttling, and have stable electrochemical performance. A pouch cell achieves a capacity of 13.2 Ah and a specific energy of 435 Wh kg-1. These findings show mechanistic understanding into the role of spin moments in sulfur conversion, enabling to design efficient and durable catalysts for Li||S batteries.