Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 10, Pages 12159-12168Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c01351
Keywords
lithium-rich manganese-based layered oxides; chlorine doping; anion redox; transition-metal migration; electrochemical performance
Funding
- National Natural Science Foundation of China [51971250, 5130424, 11474147]
- National Key Research and Development Program of China [2018YFB010400]
- Innovation Program of Central South University [2016CXS003]
- State Key Laboratory of Powder Metallurgy at Central South University
- Shenzhen GuoTuo Technology Co., Ltd.
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In this study, chlorine-doped Co-free LLOs were successfully synthesized, and it was found that Cl doping can decrease irreversible lattice oxygen loss, enhance the reversibility of oxygen redox, and inhibit transition-metal migration, leading to improved capacity, voltage retention, and rate capability during cycling.
Lithium-rich manganese-based layered oxide cathodes (LLOs) with oxygen redox reactions are considered to be potential candidates for the next generation of high-energy-density Li-ion batteries. However, the oxygen redox process that enables ultrahigh specific capacity usually leads to irreversible O-2 release and cation migration, which induce structure degradation and severe capacity/voltage losses and thus limit the commercial application of LLOs. Herein, we successfully synthesized chlorine (Cl)-doped Co-free LLOs (Li1.2Mn0.53Ni0.27O1.976Cl0.024) and analyzed the effect of anion doping on oxygen redox and structure stability of LLOs. Cl doping has been proven to decrease the irreversible lattice oxygen loss to enhance the redox reversibility of oxygen and inhibit the transition-metal migration during cycles, which substantially enhances the capacity and voltage retention and improves the rate capability during cycling. This work provides new insights for the development of high-performance TM oxide cathode materials with reversible oxygen redox.
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