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Abstract Li‐rich oxide cathodes are of prime importance for the development of high‐energy lithium‐ion batteries (LIBs). Li‐rich layered oxides, however, always undergo irreversible structural evolution, leading to inevitable capacity and voltage decay during cycling. Meanwhile, Li‐rich cation‐disordered rock‐salt oxides usually exhibit sluggish kinetics and inferior cycling stability, despite their firm structure and stable voltage output. Herein, a new Li‐rich rock‐salt oxide Li 2 Ni 1/3 Ru 2/3 O 3 with Fd ‐3 m space group, where partial cation‐ordering arrangement exists in cationic sites, is reported. Results demonstrate that a cathode fabricated from Li 2 Ni 1/3 Ru 2/3 O 3 delivers a large capacity, outstanding rate capability as well as good cycling performance with negligible voltage decay, in contrast to the common cations disordered oxides with space group Fm ‐3 m . First principle calculations also indicate that rock‐salt oxide with space group Fd ‐3 m possesses oxygen activity potential at the state of delithiation, and good kinetics with more 0‐TM (TM = transition metals) percolation networks. In situ Raman results confirm the reversible anionic redox chemistry, confirming O 2− /O − evolution during cycles in Li‐rich rock‐salt cathode for the first time. These findings open up the opportunity to design high‐performance oxide cathodes and promote the development of high‐energy LIBs.
Li et al. (Wed,) studied this question.