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<p>A rational design principle for selecting optimal anion dopants in transition-metal compounds to enhance sulfur redox activity is lacking in Li-S batteries. Herein, we propose an accurate <i>p-p-s</i> orbital electronic coupling descriptor (involving the <i>p</i>-orbitals of anion dopants and anions in transition-metal compounds and the <i>s</i>-orbitals of Li in lithium polysulfides) as a criterion for choosing anion dopants to guide the development of efficient anion-doped Li-S catalysts through machine-learning, theoretical, and experimental validation. We reveal the relationship between the electronic properties of various anion-doped WSe<sub>2</sub> and the thermodynamics and kinetics of sulfur redox. Our findings show that moderate <i>p-p-s</i> orbital electronic coupling optimizes polysulfide adsorption, facilitating Li<sub>2</sub>S nucleation and decomposition, thereby minimizing Gibbs free energy and maximizing catalytic efficiency for sulfur redox. A volcano relationship between the <i>p-p-s</i> coupling strength and catalytic activity is established. The optimal B-WSe<sub>2</sub>/MXene catalyst achieves a ~ 3 Ah pouch cell with 430 Wh kg<sup>−1</sup> specific energy and good cycle life (81.3% capacity retention over 71 cycles). These findings provide a guideline for designing efficient anion-doped Li-S catalysts with moderate <i>p-p-s</i> coupling to enable rapid sulfur catalytic conversion in Li-S batteries.</p>

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Design rules for anion-doped catalysts revealed by p-p-s orbital coupling in Li-S chemistry

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月4日

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  • Wei Wang,
  • Xinying Wang,
  • Huanhuan Yang,
  • Zhipeng Yu,
  • Weicai Zhang,
  • Haoliang Huang,
  • Zaowen Zhao,
  • Xuerong Zheng,
  • Lifeng Liu,
  • Yida Deng,
  • Yunyong Li

摘要

A rational design principle for selecting optimal anion dopants in transition-metal compounds to enhance sulfur redox activity is lacking in Li-S batteries. Herein, we propose an accurate p-p-s orbital electronic coupling descriptor (involving the p-orbitals of anion dopants and anions in transition-metal compounds and the s-orbitals of Li in lithium polysulfides) as a criterion for choosing anion dopants to guide the development of efficient anion-doped Li-S catalysts through machine-learning, theoretical, and experimental validation. We reveal the relationship between the electronic properties of various anion-doped WSe2 and the thermodynamics and kinetics of sulfur redox. Our findings show that moderate p-p-s orbital electronic coupling optimizes polysulfide adsorption, facilitating Li2S nucleation and decomposition, thereby minimizing Gibbs free energy and maximizing catalytic efficiency for sulfur redox. A volcano relationship between the p-p-s coupling strength and catalytic activity is established. The optimal B-WSe2/MXene catalyst achieves a ~ 3 Ah pouch cell with 430 Wh kg−1 specific energy and good cycle life (81.3% capacity retention over 71 cycles). These findings provide a guideline for designing efficient anion-doped Li-S catalysts with moderate p-p-s coupling to enable rapid sulfur catalytic conversion in Li-S batteries.