Gradient Li-rich oxide cathode particles immunized against oxygen release by a molten salt treatment

Zhi Zhu, Daiwei Yu, Yang Yang, Cong Su, Yimeng Huang, Yanhao Dong, Iradwikanari Waluyo, Baoming Wang, Adrian Hunt, Xiahui Yao, Jinhyuk Lee, Weijiang Xue and Ju Li ()
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Zhi Zhu: Massachusetts Institute of Technology
Daiwei Yu: Massachusetts Institute of Technology
Yang Yang: Massachusetts Institute of Technology
Cong Su: Massachusetts Institute of Technology
Yimeng Huang: Massachusetts Institute of Technology
Yanhao Dong: Massachusetts Institute of Technology
Iradwikanari Waluyo: Brookhaven National Laboratory
Baoming Wang: Massachusetts Institute of Technology
Adrian Hunt: Brookhaven National Laboratory
Xiahui Yao: Massachusetts Institute of Technology
Jinhyuk Lee: Massachusetts Institute of Technology
Weijiang Xue: Massachusetts Institute of Technology
Ju Li: Massachusetts Institute of Technology

Nature Energy, 2019, vol. 4, issue 12, 1049-1058

Abstract: Abstract Lithium-rich transition metal oxide (Li1+XM1−XO2) cathodes have high energy density above 900 Wh kg−1 due to hybrid anion- and cation-redox (HACR) contributions, but critical issues such as oxygen release and voltage decay during cycling have prevented their application for years. Here we show that a molten molybdate-assisted LiO extraction at 700 °C creates lattice-coherent but depth (r)-dependent Li1+X(r)M1−X(r)O2 particles with a Li-rich (X ≈ 0.2) interior, a Li-poor (X ≈ −0.05) surface and a continuous gradient in between. The gradient Li-rich single crystals eliminate the oxygen release to the electrolyte and, importantly, still allow stable oxygen redox contributions within. Both the metal valence states and the crystal structure are well maintained during cycling. The gradient HACR cathode displays a specific density of 843 Wh kg−1 after 200 cycles at 0.2C and 808 Wh kg−1 after 100 cycles at 1C, with very little oxygen release and consumption of electrolyte. This high-temperature immunization treatment can be generalized to leach other elements to avoid unexpected surface reactions in batteries.

Date: 2019
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DOI: 10.1038/s41560-019-0508-x

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