<p>Layered O3-type oxides have attracted significant interest as high-capacity cathode materials for sodium-ion batteries, owing to their ample sodium storage and competitive energy density. However, their practical implementation is hindered by irreversible phase transitions and sluggish Na<sup>+</sup> diffusion kinetics, leading to rapid capacity decay. Herein, we realize a unique dual-spacing modulation in O3-NaNi<sub>0.5</sub>Mn<sub>0.5</sub>O<sub>2</sub> cathodes via rational Cu substitution to effectively mitigate these intrinsic challenges. Comprehensive structural characterization reveals that this targeted modulation simultaneously expands the Na<sup>+</sup> layer spacing to facilitate ionic transport and contracts the transition metal slabs to enhance structural coherence. Consequently, the optimized NaNi<sub>0.45</sub>Mn<sub>0.5</sub>Cu<sub>0.05</sub>O<sub>2</sub> electrode delivers a high reversible capacity of 129.0&#xa0;mA h g<sup>− 1</sup> at 0.5&#xa0;C, with exceptional cycling stability (83.3% capacity retention after 100 cycles) and outstanding rate capability (94.6&#xa0;mA h g<sup>− 1</sup> at 5&#xa0;C). Furthermore, even within an extended voltage window (2.0–4.3&#xa0;V), the material maintains a retention of 69.3% due to enhanced structural integrity. When paired with a commercial hard carbon anode, the resulting full cell demonstrates performance analogous to the half-cell configuration, underscoring its promising potential for large-scale commercialization.</p> Graphical Abstract <p></p>

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Enhanced rate and cycling performance of O3-NaNi0.5Mn0.5O2 via unique dual-spacing modulation as sodium-ion cathode materials

  • Yi Xie,
  • Qingsong Luo,
  • Lina Han,
  • Lingxin Yu,
  • Baolong Li,
  • Xiaoyuan Zeng,
  • Yingjie Zhang,
  • Peng Dong

摘要

Layered O3-type oxides have attracted significant interest as high-capacity cathode materials for sodium-ion batteries, owing to their ample sodium storage and competitive energy density. However, their practical implementation is hindered by irreversible phase transitions and sluggish Na+ diffusion kinetics, leading to rapid capacity decay. Herein, we realize a unique dual-spacing modulation in O3-NaNi0.5Mn0.5O2 cathodes via rational Cu substitution to effectively mitigate these intrinsic challenges. Comprehensive structural characterization reveals that this targeted modulation simultaneously expands the Na+ layer spacing to facilitate ionic transport and contracts the transition metal slabs to enhance structural coherence. Consequently, the optimized NaNi0.45Mn0.5Cu0.05O2 electrode delivers a high reversible capacity of 129.0 mA h g− 1 at 0.5 C, with exceptional cycling stability (83.3% capacity retention after 100 cycles) and outstanding rate capability (94.6 mA h g− 1 at 5 C). Furthermore, even within an extended voltage window (2.0–4.3 V), the material maintains a retention of 69.3% due to enhanced structural integrity. When paired with a commercial hard carbon anode, the resulting full cell demonstrates performance analogous to the half-cell configuration, underscoring its promising potential for large-scale commercialization.

Graphical Abstract