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- W4367315940 abstract "Oxygen-redox electrochemistry is attracting tremendous attention due to its enhanced energy density for layered oxide cathodes. However, quantified effects of ligand–metal bond covalency on the oxygen-redox behaviors are not fully understood, limiting a rational structure design for enhancing the oxygen redox reversibility. Here, using Li2Ru1–xMnxO3 (0 ≤ x ≤ 0.8) which includes both 3d- and 4d-based cations as model compounds, we provide a quantified relation between the ligand–metal bond covalency and oxygen-redox electrochemistry. Supported by theoretical calculations, we reveal a linear positive correlation between the transition metal (TM)–O bond covalency and the overlap area of TM nd and O 2p orbitals. Furthermore, based on the electrochemical tests on the Li2Ru1–xMnxO3 systems, we found that the enhanced TM–O bond covalency can increase the reversibility of oxygen-redox electrochemistry. Due to the strong Ru–O bond covalency, the thus designed Ru-doped Li-rich Li1.2Mn0.54Ni0.13Co0.13O2 cathode shows an enhanced initial coulombic efficiency, increased capacity retention, and suppressed voltage decay during cycling. This systematic study provides a rational structure design principle for the development of oxygen-redox-based layered oxide cathodes." @default.
- W4367315940 created "2023-04-29" @default.
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- W4367315940 date "2023-04-28" @default.
- W4367315940 modified "2023-10-18" @default.
- W4367315940 title "Quantifying Effects of Ligand–Metal Bond Covalency on Oxygen-Redox Electrochemistry in Layered Oxide Cathodes" @default.
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- W4367315940 doi "https://doi.org/10.1021/acs.inorgchem.3c00344" @default.
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