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Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides.

  • Author(s): Zhao, Enyue;
  • Li, Qinghao;
  • Meng, Fanqi;
  • Liu, Jue;
  • Wang, Junyang;
  • He, Lunhua;
  • Jiang, Zheng;
  • Zhang, Qinghua;
  • Yu, Xiqian;
  • Gu, Lin;
  • Yang, Wanli;
  • Li, Hong;
  • Wang, Fangwei;
  • Huang, Xuejie
  • et al.
Abstract

Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.

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