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<p>Sodium-ion batteries present a promising alternative to lithium-ion systems in specific applications owing to advantages in safety and cost. However, their energy density remains a key limitation. Anionic redox in oxygen offers a pathway to boost capacity in layered oxide cathodes, yet it often induces irreversible oxygen release and structural degradation at high voltages. Here, we introduce a high-entropy P3-type cathode, Na<sub>0.67</sub>Mn<sub>0.75</sub>Fe<sub>0.05</sub>Ti<sub>0.033</sub>Sn<sub>0.057</sub>Mg<sub>0.017</sub>Cr<sub>0.043</sub>-Zn<sub>0.05</sub>O<sub>2</sub> (HE-NMO), where multi-element transition-metal mixing effectively regulates the non-bonding oxygen orbitals involved in anionic redox. This entropy-mediated regulation disperses the non-bonding O 2p orbitals, stabilizing localized electron holes generated during oxygen oxidation and suppressing irreversible O–O dimerization and oxygen release. HE-NMO exhibits a discharge capacity of 166.6 mAh g<sup>−1</sup> and a retention of 86.1% after 50 cycles at 2 C under high-voltage operation. Our work establishes high-entropy design as an effective paradigm for controlling anionic redox at the orbital level, advancing high-energy, durable sodium-ion batteries.</p>

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Regulating non-bonding oxygen orbitals via high-entropy design for stable anionic redox

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月16日

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  • Wenji Yin,
  • Ziqin Zhang,
  • Jiming Peng,
  • Gemeng Liang,
  • Qichang Pan,
  • Fenghua Zheng,
  • Qingyu Li,
  • Hongqiang Wang,
  • Sijiang Hu

摘要

Sodium-ion batteries present a promising alternative to lithium-ion systems in specific applications owing to advantages in safety and cost. However, their energy density remains a key limitation. Anionic redox in oxygen offers a pathway to boost capacity in layered oxide cathodes, yet it often induces irreversible oxygen release and structural degradation at high voltages. Here, we introduce a high-entropy P3-type cathode, Na0.67Mn0.75Fe0.05Ti0.033Sn0.057Mg0.017Cr0.043-Zn0.05O2 (HE-NMO), where multi-element transition-metal mixing effectively regulates the non-bonding oxygen orbitals involved in anionic redox. This entropy-mediated regulation disperses the non-bonding O 2p orbitals, stabilizing localized electron holes generated during oxygen oxidation and suppressing irreversible O–O dimerization and oxygen release. HE-NMO exhibits a discharge capacity of 166.6 mAh g−1 and a retention of 86.1% after 50 cycles at 2 C under high-voltage operation. Our work establishes high-entropy design as an effective paradigm for controlling anionic redox at the orbital level, advancing high-energy, durable sodium-ion batteries.