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<p>The instability of oxygen redox activity in layered oxide cathodes, particularly the formation of localized electron holes on oxygen (O<sup>−</sup>) and subsequent anion dimerization, has been demonstrated to trigger rapid capacity degradation and severe voltage hysteresis. Our study primarily focuses on P3-type Na<sub>2/3</sub>Cu<sub>1/3</sub>Mn<sub>2/3</sub>O<sub>2</sub>, which demonstrates reversible oxygen redox with an exceptionally low voltage hysteresis of 0.05 V. Spectroscopic analyses demonstrate a reversible O<sup>2−</sup>→O<sup>−</sup> evolution in Na<sub>2/3</sub>Cu<sub>1/3</sub>Mn<sub>2/3</sub>O<sub>2</sub> without O–O dimerization. Furthermore, Multilateral non-invasive magnetic methods reveal that strong Cu-O-Mn superexchange interactions during the metal-ligand redox process lead to delocalization of O<sup>−</sup> species and inhibition of irreversible O–O bonding, thereby enabling ultralow voltage hysteresis. This work establishes magnetic exchange engineering as a transformative strategy to unlock reversible oxygen redox in high-energy battery electrodes.</p>

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Metal-ligand redox assisted by strong Cu-O-Mn superexchange interaction in a prototype layered oxide cathode

  • 期刊论文

  • 发表日期：

    2026年3月31日

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  • Chunjing Hu,
  • Jiefan Liu,
  • Xiaobing Lou,
  • Ming Shen,
  • Bingwen Hu,
  • Chao Li

摘要

The instability of oxygen redox activity in layered oxide cathodes, particularly the formation of localized electron holes on oxygen (O−) and subsequent anion dimerization, has been demonstrated to trigger rapid capacity degradation and severe voltage hysteresis. Our study primarily focuses on P3-type Na2/3Cu1/3Mn2/3O2, which demonstrates reversible oxygen redox with an exceptionally low voltage hysteresis of 0.05 V. Spectroscopic analyses demonstrate a reversible O2−→O− evolution in Na2/3Cu1/3Mn2/3O2 without O–O dimerization. Furthermore, Multilateral non-invasive magnetic methods reveal that strong Cu-O-Mn superexchange interactions during the metal-ligand redox process lead to delocalization of O− species and inhibition of irreversible O–O bonding, thereby enabling ultralow voltage hysteresis. This work establishes magnetic exchange engineering as a transformative strategy to unlock reversible oxygen redox in high-energy battery electrodes.