Enabling the high capacity of lithium-rich anti-fluorite lithium iron oxide by simultaneous anionic and cationic redox

Chun Zhan, Zhenpeng Yao, Jun Lu (), Lu Ma, Victor A. Maroni, Liang Li, Eungje Lee, Esen E. Alp, Tianpin Wu, Jianguo Wen, Yang Ren, Christopher Johnson, Michael M. Thackeray, Maria K. Y. Chan, Chris Wolverton () and Khalil Amine ()
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Chun Zhan: Argonne National Laboratory
Zhenpeng Yao: Northwestern University
Jun Lu: Argonne National Laboratory
Lu Ma: Argonne National Laboratory
Victor A. Maroni: Argonne National Laboratory
Liang Li: Argonne National Laboratory
Eungje Lee: Argonne National Laboratory
Esen E. Alp: Argonne National Laboratory
Tianpin Wu: Argonne National Laboratory
Jianguo Wen: Argonne National Laboratory
Yang Ren: Argonne National Laboratory
Christopher Johnson: Argonne National Laboratory
Michael M. Thackeray: Argonne National Laboratory
Maria K. Y. Chan: Argonne National Laboratory
Chris Wolverton: Northwestern University
Khalil Amine: Argonne National Laboratory

Nature Energy, 2017, vol. 2, issue 12, 963-971

Abstract: Abstract Anionic redox reactions in cathodes of lithium-ion batteries are allowing opportunities to double or even triple the energy density. However, it is still challenging to develop a cathode, especially with Earth-abundant elements, that enables anionic redox activity for real-world applications, primarily due to limited strategies to intercept the oxygenates from further irreversible oxidation to O2 gas. Here we report simultaneous iron and oxygen redox activity in a Li-rich anti-fluorite Li5FeO4 electrode. During the removal of the first two Li ions, the oxidation potential of O2− is lowered to approximately 3.5 V versus Li+/Li0, at which potential the cationic oxidation occurs concurrently. These anionic and cationic redox reactions show high reversibility without any obvious O2 gas release. Moreover, this study provides an insightful guide to designing high-capacity cathodes with reversible oxygen redox activity by simply introducing oxygen ions that are exclusively coordinated by Li+.

Date: 2017
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DOI: 10.1038/s41560-017-0043-6

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