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<p>As a novel material, high-entropy compounds have attracted extensive attention in the field of lithium–sulfur battery host materials due to their diverse elemental composition with a wide range of properties. The ability to effectively mitigate the shuttle effect of lithium polysulfides and catalyze the bidirectional conversion of Li<sub>2</sub>S<sub>2</sub>/Li<sub>2</sub>S is crucial to enhance the overall performance of the battery. In this study, a unique sulfur host nanosized high-entropy material comprising selenium-doped HEO (AlCrFeCoNi)<sub>3</sub>O<sub>4-x</sub>-Se<sub>x</sub> is fabricated using an in situ thermal reduction and selenylation method. In the high-entropy compounds, the introduction of Se causes that the generation of oxygen vacancies during the lattice distortion serves as ion transfer pathway and the formation of M-Se bonds provides a high adsorption capability for LiPSs. Moreover, the polymetallic cooperative high-entropy nanoparticles also provide numerous active sites favoring redox kinetics of the sulfur electrode. The resulting selenium-doped HEO (AlCrFeCoNi)<sub>3</sub>O<sub>4-<i>x</i></sub>-Se<sub><i>x</i></sub> not only enhances discharge capacity but also maintains excellent capacity cycling stability. As a result, the HEO-Se/S composite exhibits a specific capacity of 1233.9&#xa0;mAh&#xa0;g<sup>−1</sup> at 0.1C and experiences minimal capacity fading at a rate of 0.038% per cycle over 500 cycles at 0.2C, while host materials with sulfur loading of 4.33&#xa0;mg&#xa0;cm<sup>−2</sup> and E/S ratio of 5.88&#xa0;μL&#xa0;mg<sup>−1</sup> exhibit excellent capacity retention after 100 cycles at 0.2C. This work offers new insights into synthesizing high-entropy nanomaterials for improving the electrochemical performance of Li–S batteries.</p> Graphical abstract <p></p>

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Defectizing high-entropy oxide with the introduction of Se to facilitate the kinetics for highly cycle-stable lithium–sulfur batteries

  • 期刊论文

  • 发表日期：

    2025年6月18日

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  • Wen-Xu Li,
  • Wei-Ran Wang,
  • Dan Li,
  • Qi-Fu Jin,
  • Jin-Bao Gao,
  • Jian-Xun Zhao,
  • Qing-Cheng Liang,
  • Qing-Bao Zhang,
  • Peng Chen

摘要

As a novel material, high-entropy compounds have attracted extensive attention in the field of lithium–sulfur battery host materials due to their diverse elemental composition with a wide range of properties. The ability to effectively mitigate the shuttle effect of lithium polysulfides and catalyze the bidirectional conversion of Li2S2/Li2S is crucial to enhance the overall performance of the battery. In this study, a unique sulfur host nanosized high-entropy material comprising selenium-doped HEO (AlCrFeCoNi)3O4-x-Sex is fabricated using an in situ thermal reduction and selenylation method. In the high-entropy compounds, the introduction of Se causes that the generation of oxygen vacancies during the lattice distortion serves as ion transfer pathway and the formation of M-Se bonds provides a high adsorption capability for LiPSs. Moreover, the polymetallic cooperative high-entropy nanoparticles also provide numerous active sites favoring redox kinetics of the sulfur electrode. The resulting selenium-doped HEO (AlCrFeCoNi)3O4-x-Sex not only enhances discharge capacity but also maintains excellent capacity cycling stability. As a result, the HEO-Se/S composite exhibits a specific capacity of 1233.9 mAh g−1 at 0.1C and experiences minimal capacity fading at a rate of 0.038% per cycle over 500 cycles at 0.2C, while host materials with sulfur loading of 4.33 mg cm−2 and E/S ratio of 5.88 μL mg−1 exhibit excellent capacity retention after 100 cycles at 0.2C. This work offers new insights into synthesizing high-entropy nanomaterials for improving the electrochemical performance of Li–S batteries.

Graphical abstract