期刊
ADVANCED MATERIALS
卷 31, 期 11, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201807825
关键词
Fd-3m space group; Li-ion batteries; Li-rich material; reversible anionic redox; rock-salt structure
类别
资金
- CSC (China Scholarship Council) scholarship
- National Basic Research Program of China [2014CB932300]
- NSF of China [21633003, 51802149, 11704245, 11874199]
- NSF of Jiangsu Province, China [BK20170630]
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 Li2Ni1/3Ru2/3O3 with Fd-3m space group, where partial cation-ordering arrangement exists in cationic sites, is reported. Results demonstrate that a cathode fabricated from Li2Ni1/3Ru2/3O3 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-3m. First principle calculations also indicate that rock-salt oxide with space group Fd-3m 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 O2-/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.
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