Stabilizing Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Li‐rich Cathode Oxides

Lattice oxygen redox (l‐OR) has become an essential complementation for the traditional transition‐metal (TM) redox charge compensation to achieve the 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 researched. We reveal that the oxygen lattice structure evolution upon the l‐OR in Li‐rich TM oxides with tridimensional (3D)‐disordered cation framework is relatively stable, directly contrasting the obviously distorted oxygen lattice framework in Li‐rich oxides with two‐dimensional (2D)/3D‐ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing oxygen lattice involving 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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