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<p>Layered transition metal oxide cathodes (Na<sub><i>x</i></sub>TMO<sub>2</sub>) demonstrate a classic type of cathode for Sodium-ion batteries (SIBs), however their practical application faces a long-standing challenge of irreversible phase transitions at high voltages, which causes unsatisfied specific energy and cycling stability, particularly for P-type (Na<sup>+</sup> located at prismatic sites) cathodes. This phenomenon is conventionally ascribed to the Na<sup>+</sup> re-coordination from prismatic to octahedral (O-type) configuration upon Na<sup>+</sup> extraction, whereby the TMO<sub>2</sub> slab gliding and abrupt <i>c</i>-lattice change are always coupled, and a straightforward solution to this situation remains elusive. Here, we reveal that, the TMO<sub>2</sub> slab gliding and the lattice contraction can be decoupled, and the rapid lattice contraction under high state-of-charge underlies the fundamental origin for the irreversible phase transitions. By pre-engineering 15.8% O-type stacking faults to a P-type Na<sub>0.7</sub>Mn<sub>0.8</sub>Ni<sub>0.2</sub>O<sub>2</sub>, the dramatic volume variation and irreversible phase transitions at high voltage (4.5 V vs. Na<sup>+</sup>/Na) can be primarily eliminated. This work advances the understanding on the phase transitions at deep desodiation states, and paves up a feasible way to realize high-energy layered oxides.</p>

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Decoupling slab gliding and lattice contraction in Na layered oxides to enable high-voltage Na-ion batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月10日

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  • Qinhao Shi,
  • Fanghua Ning,
  • Xuan Yu,
  • Fanjie Xia,
  • Ruijuan Qi,
  • Guofeng Cheng,
  • Yi Qiu,
  • Haoyang Liang,
  • Hongfei Zheng,
  • Tao Zhang,
  • Shigang Lu,
  • Tu Lan,
  • Jinsong Wu,
  • Yingchun Lyu,
  • Huaican Chen,
  • Wen Wen,
  • Zhenpeng Yao,
  • Jiujun Zhang,
  • Jun Lu,
  • Yufeng Zhao

摘要

Layered transition metal oxide cathodes (NaxTMO2) demonstrate a classic type of cathode for Sodium-ion batteries (SIBs), however their practical application faces a long-standing challenge of irreversible phase transitions at high voltages, which causes unsatisfied specific energy and cycling stability, particularly for P-type (Na+ located at prismatic sites) cathodes. This phenomenon is conventionally ascribed to the Na+ re-coordination from prismatic to octahedral (O-type) configuration upon Na+ extraction, whereby the TMO2 slab gliding and abrupt c-lattice change are always coupled, and a straightforward solution to this situation remains elusive. Here, we reveal that, the TMO2 slab gliding and the lattice contraction can be decoupled, and the rapid lattice contraction under high state-of-charge underlies the fundamental origin for the irreversible phase transitions. By pre-engineering 15.8% O-type stacking faults to a P-type Na0.7Mn0.8Ni0.2O2, the dramatic volume variation and irreversible phase transitions at high voltage (4.5 V vs. Na+/Na) can be primarily eliminated. This work advances the understanding on the phase transitions at deep desodiation states, and paves up a feasible way to realize high-energy layered oxides.