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<p>Exploring sodium-ion layered oxides with broad compositional diversity is an important approach for the development of high-performance positive electrodes. Structural chemistry determined by composition plays a decisive role in performance improvement, but the relationship between composition and structure becomes more elusive in complex multi-component systems. Here we propose an electronegativity entropy weight concept to understand entropy-dominated phases formation. Electronegativity and configurational entropy are used to quantify key interactions in layered materials. Guided by this understanding, we design a sodium-deficient layered oxide with an O3 stacking sequence. This material demonstrates good structural and thermal stability, along with air stability (negligible performance degradation after air exposure), cycling stability (93.02% capacity retention after 200 cycles), and rate capability (retaining 69.1% capacity retention from 86.5 mA g⁻¹ to 1.73 A g⁻¹). Even in potassium-ion batteries with larger inserted ions, the material still exhibits cycling stability. This strategy provides valuable compositional guidance for the rational design of high-performance layered oxide materials.</p>

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Electronegativity and entropy design of layered oxides for sodium-ion batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月8日

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  • Lu Gan,
  • Hu-Rong Yao,
  • Jingwen Dai,
  • Zefeng Lai,
  • Xin-Guang Yuan,
  • Wei-Huan He,
  • Qi-lin Zheng,
  • Min Wen,
  • Wei-Wei Yuan,
  • Min Lin,
  • Jian-Mao Xiao,
  • Ze Yu,
  • Yu-Jie Guo,
  • Jinling Liu,
  • Fanghua Ning,
  • Fei Zhan,
  • Denglong Chen,
  • Lituo Zheng,
  • Zhigao Huang,
  • Chuying OuYang,
  • Yu-Guo Guo

摘要

Exploring sodium-ion layered oxides with broad compositional diversity is an important approach for the development of high-performance positive electrodes. Structural chemistry determined by composition plays a decisive role in performance improvement, but the relationship between composition and structure becomes more elusive in complex multi-component systems. Here we propose an electronegativity entropy weight concept to understand entropy-dominated phases formation. Electronegativity and configurational entropy are used to quantify key interactions in layered materials. Guided by this understanding, we design a sodium-deficient layered oxide with an O3 stacking sequence. This material demonstrates good structural and thermal stability, along with air stability (negligible performance degradation after air exposure), cycling stability (93.02% capacity retention after 200 cycles), and rate capability (retaining 69.1% capacity retention from 86.5 mA g⁻¹ to 1.73 A g⁻¹). Even in potassium-ion batteries with larger inserted ions, the material still exhibits cycling stability. This strategy provides valuable compositional guidance for the rational design of high-performance layered oxide materials.