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In situ formed partially disordered phases as earth-abundant Mn-rich cathode materials

Zijian Cai, Bin Ouyang, Han-Ming Hau, Tina Chen, Raynald Giovine, Krishna Prasad Koirala, Linze Li, Huiwen Ji, Yang Ha, Yingzhi Sun, Jianping Huang, Yu Chen, Vincent Wu, Wanli Yang, Chongmin Wang, Raphaële J. Clément, Zhengyan Lun () and Gerbrand Ceder ()
Additional contact information
Zijian Cai: University of California Berkeley
Bin Ouyang: Florida State University
Han-Ming Hau: University of California Berkeley
Tina Chen: University of California Berkeley
Raynald Giovine: University of California Santa Barbara
Krishna Prasad Koirala: Pacific Northwest National Laboratory
Linze Li: Pacific Northwest National Laboratory
Huiwen Ji: University of Utah
Yang Ha: Lawrence Berkeley National Laboratory
Yingzhi Sun: University of California Berkeley
Jianping Huang: Lawrence Berkeley National Laboratory
Yu Chen: University of California Berkeley
Vincent Wu: University of California Santa Barbara
Wanli Yang: Lawrence Berkeley National Laboratory
Chongmin Wang: Pacific Northwest National Laboratory
Raphaële J. Clément: University of California Santa Barbara
Zhengyan Lun: University of California Berkeley
Gerbrand Ceder: University of California Berkeley

Nature Energy, 2024, vol. 9, issue 1, 27-36

Abstract: Abstract Earth-abundant cathode materials are urgently needed to enable scaling of the Li-ion industry to multiply terawatt hours of annual production, necessitating reconsideration of how good cathode materials can be obtained. Irreversible transition metal migration and phase transformations in Li-ion cathodes are typically believed to be detrimental because they may trigger voltage hysteresis, poor kinetics and capacity degradation. Here we challenge this conventional consensus by reporting an unusual phase transformation from disordered Li- and Mn-rich rock salts to a new phase (named δ), which displays partial spinel-like ordering with short coherence length and exhibits high energy density and rate capability. Unlike other Mn-based cathodes, the δ phase exhibits almost no voltage fade upon cycling. We identify the driving force and kinetics of this in situ cathode formation and establish design guidelines for Li- and Mn-rich compositions that combine high energy density, high rate capability and good cyclability, thereby enabling Mn-based energy storage.

Date: 2024
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DOI: 10.1038/s41560-023-01375-9

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