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<p>P3-type manganese-iron-based cathodes with high specific capacity and abundant resource have attracted considerable attention for sodium-ion batteries. However, the long-term cycle stability of P3-type cathodes is still not satisfactory. In this work, we design a new quaternary manganese-iron-based cathode material (P3-Na<sub>0.54</sub>Mn<sub>0.64</sub>Fe<sub>0.16</sub>Mg<sub>0.1</sub>Cu<sub>0.1</sub>O<sub>2</sub>) by Cu substitution. The strong covalent Cu–O bonds improve the structural stability and the reversibility of O redox during charge and discharge processes. Cu substitution also mitigates the structure change with less unit cell volume variation, and improves the Na-ion transport kinetics effectively. As a result, NMFMC delivers much improved cycling stability and rate capability compared with NMFM. It reveals that the charge compensation of NMFMC is mainly contributed by Mn<sup>3+/4+</sup>, Fe<sup>3+/3.5+</sup> and O<sup>2−/−</sup> during the charge and discharge processes, and Cu substitution can also enhance the activity and reversibility of Fe redox. This strategy provides a new pathway toward improving the stability and O redox reversibility of P3-type cathode materials for sodium-ion batteries.</p>

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Copper-substituted P3-type Na0.54Mn0.64Fe0.16Mg0.1Cu0.1O2 cathode material for sodium-ion batteries with enhanced anionic redox reversibility

  • 期刊论文

  • 发表日期：

    2025年1月31日

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  • Zhe Mei,
  • Xun-Lu Li,
  • Cui Ma,
  • Jie Zeng,
  • Chong-Yu Du,
  • Rui-Jie Luo,
  • Xuan Xu,
  • Zhe Qian,
  • Zi-Ting Zhou,
  • Ya Zhang,
  • Qian Cheng,
  • Yao-Guo Fang,
  • Yong-Ning Zhou

摘要

P3-type manganese-iron-based cathodes with high specific capacity and abundant resource have attracted considerable attention for sodium-ion batteries. However, the long-term cycle stability of P3-type cathodes is still not satisfactory. In this work, we design a new quaternary manganese-iron-based cathode material (P3-Na0.54Mn0.64Fe0.16Mg0.1Cu0.1O2) by Cu substitution. The strong covalent Cu–O bonds improve the structural stability and the reversibility of O redox during charge and discharge processes. Cu substitution also mitigates the structure change with less unit cell volume variation, and improves the Na-ion transport kinetics effectively. As a result, NMFMC delivers much improved cycling stability and rate capability compared with NMFM. It reveals that the charge compensation of NMFMC is mainly contributed by Mn3+/4+, Fe3+/3.5+ and O2−/− during the charge and discharge processes, and Cu substitution can also enhance the activity and reversibility of Fe redox. This strategy provides a new pathway toward improving the stability and O redox reversibility of P3-type cathode materials for sodium-ion batteries.