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Tuning Oxygen Redox Chemistry in Li‐Rich Mn‐Based Layered Oxide Cathodes by Modulating Cation Arrangement
Author(s) -
Zhang Jicheng,
Cheng Fangyi,
Chou Shulei,
Wang Jianli,
Gu Lin,
Wang Heng,
Yoshikawa Hirofumi,
Lu Yong,
Chen Jun
Publication year - 2019
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.201901808
Subject(s) - redox , cathode , oxygen , materials science , oxide , manganese oxide , inorganic chemistry , oxygen reduction , chemical engineering , nanotechnology , electrochemistry , chemistry , electrode , metallurgy , organic chemistry , engineering
Li‐rich Mn‐based oxides (LRMO) are promising cathode materials to build next‐generation lithium‐ion batteries with high energy density exceeding 400 W h kg −1 . However, due to a lack of in‐depth understanding of oxygen redox chemistry in LRMO, voltage decay is not resolved thoroughly. Here, it is demonstrated that the oxygen redox chemistry could be tuned by modulating cation arrangement. It declares that the materials with Li/Ni disorder and Li vacancies can inhibit the formation of OO dimers. Because of the high chemical activity, OO dimers could accelerate lattice oxygen release and NiO/spinel formation. The samples without forming OO dimers show improved performance in suppressing oxygen overoxidation and mitigating cation dissolution. As a result, the optimized cathode exhibits a high capacity over 280 mA h g −1 at 0.1 C and a high plateau voltage of 3.58 V with a very low voltage decay of 1.6% after 150 cycles at 1 C. This study opens an attractive path in designing Li‐rich electrodes with stabilized redox chemistry.