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Orbital Stabilization of Anionic Redox via Surface Restructuration for Li-Rich Mn-Based Layered Oxides
Chuan Gao1, Yue Yu1, Junfei Cai1
1Beijing Key Laboratory of Theory and Technology for Advanced Batteries Materials, School of Materials Science and Engineering, Peking University, Beijing, P. R. China.
Surface modification of lithium-rich layered oxides with nickel ions suppresses oxygen release and enhances battery performance. This strategy enables high capacity and long-term cycling stability for advanced cathode materials.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Lithium-rich layered oxides offer high capacity via cationic and anionic redox reactions.
- Anionic redox can lead to O-O dimer formation, oxygen release, and performance degradation.
Purpose of the Study:
- To engineer a lithium-rich manganese-based layered oxide cathode with enhanced stability and capacity.
- To investigate the effect of surface reconstruction on anionic redox processes.
Main Methods:
- Surface reconstruction of lithium-rich manganese-based layered oxides.
- Site-specific nickel ion occupation at 4a Wyckoff sites within the Li2MnO3 phase.
- Electrochemical performance testing (capacity, rate capability, cycling stability).
Main Results:
- Engineered cathode achieved 325 mAh g⁻¹ reversible capacity at 0.1C.
- Demonstrated excellent rate capability (272.8 mAh g⁻¹ at 1C).
- Exhibited 90% capacity retention after 300 cycles, suppressing O-O dimer formation and oxygen release.
Conclusions:
- Surface nickel occupation effectively suppresses detrimental O-O dimer formation and oxygen release.
- This surface engineering strategy enables high energy density and long-term cycling stability.
- Provides insights for developing advanced high-energy-density cathode materials.
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