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<p>Electrocatalyst activity and stability demonstrate a “seesaw” relationship. Introducing vacancies (Vo) enhances the activity by improving reactant affinity and increasing accessible active sites. However, deficient or excessive Vo reduces polysulfide adsorption and lowers catalytic stability. Herein, a novel “heteroatoms synergistic anchoring vacancies” strategy is proposed to address the trade-off between high activity and stability. Phosphorus-doped CoSe<sub>2</sub> with remained rich selenium vacancies (P-CS-Vo-0.5) was synthesized by producing abundant selenium Vo followed by controlled P atom doping. Atomic-scale microstructure analysis elucidated a dynamic process of surface vacancy generation and the subsequent partial occupation of these vacancies by P atoms. Density functional theory simulations and in situ Raman tests revealed that the Se vacancies provide highly active catalytic sites, accelerating polysulfide conversion, while P incorporation effectively reduces the surface energy of Se vacancies and suppresses their inward migration, enhancing structural robustness. The battery with the optimal P-CS-Vo-0.5 separator delivers an initial discharge capacity of 1306.7 mAh g<sup>−1</sup> at 0.2C, and maintain 5.04&#xa0;mAh&#xa0;cm<sup>−2</sup> at a high sulfur loading (5.7&#xa0;mg&#xa0;cm<sup>−2</sup>, 5.0&#xa0;μL&#xa0;mg<sup>−1</sup>), achieving 95.1% capacity retention after 80 cycles. This strategy of modifying local atomic environments offers a new route to designing highly active and stable catalysts. </p>

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Heteroatoms Synergistic Anchoring Vacancies in Phosphorus-Doped CoSe2 Enable Ultrahigh Activity and Stability in Li–S Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年6月23日

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  • Xiaoya Zhou,
  • Wei Mao,
  • Chengwei Ye,
  • Qi Liang,
  • Peng Wang,
  • Xuebin Wang,
  • Shaochun Tang

摘要

Electrocatalyst activity and stability demonstrate a “seesaw” relationship. Introducing vacancies (Vo) enhances the activity by improving reactant affinity and increasing accessible active sites. However, deficient or excessive Vo reduces polysulfide adsorption and lowers catalytic stability. Herein, a novel “heteroatoms synergistic anchoring vacancies” strategy is proposed to address the trade-off between high activity and stability. Phosphorus-doped CoSe2 with remained rich selenium vacancies (P-CS-Vo-0.5) was synthesized by producing abundant selenium Vo followed by controlled P atom doping. Atomic-scale microstructure analysis elucidated a dynamic process of surface vacancy generation and the subsequent partial occupation of these vacancies by P atoms. Density functional theory simulations and in situ Raman tests revealed that the Se vacancies provide highly active catalytic sites, accelerating polysulfide conversion, while P incorporation effectively reduces the surface energy of Se vacancies and suppresses their inward migration, enhancing structural robustness. The battery with the optimal P-CS-Vo-0.5 separator delivers an initial discharge capacity of 1306.7 mAh g−1 at 0.2C, and maintain 5.04 mAh cm−2 at a high sulfur loading (5.7 mg cm−2, 5.0 μL mg−1), achieving 95.1% capacity retention after 80 cycles. This strategy of modifying local atomic environments offers a new route to designing highly active and stable catalysts.