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Unveiling the Role of Transition-Metal Ions in the Thermal Degradation of Layered Ni-Co-Mn Cathodes for Lithium Rechargeable Batteries

Cited 19 time in Web of Science Cited 22 time in Scopus
Authors

Jung, Sung-Kyun; Kim, Hyungsub; Song, Seok Hyun; Lee, Seongsu; Kim, Jongsoon; Kang, Kisuk

Issue Date
2022-03-01
Publisher
John Wiley & Sons Ltd.
Citation
Advanced Functional Materials, Vol.32 No.13, p. 2108790
Abstract
The need for batteries with high energy density and safety has motivated the development of Ni-rich layered cathodes with high thermal stability, requiring a revisit of the role of the transition-metal ion in the phase transition accompanying the oxygen evolution of highly charged cathodes. Here, the role of the transition-metal ion in LixNi0.5Co0.2Mn0.3O2 (x = 0.5, 0.33) is revealed in the phase transition and O-2 evolution occurring at high temperatures using combined in situ high-temperature neutron diffraction (ND) and gas analyses. The thermal migration of each transition-metal ion upon heating is directly visualized at different states of charge using Rietveld refinement of ND patterns as well as the maximum entropy method. The oxygen evolution observed for the highly charged state at low temperature is accompanied by M3O4-type spinel (M = Ni, Co, and Mn) phase formation with preferential occupation of Co in the tetrahedral site. Co3+/Co2+ reduction accompanying the oxygen evolution rather can mitigate and delay the formation of the rock-salt phase. The findings provide insight into the manipulation of the composition of Ni-rich layered cathode for the design of cathodes with high energy density and safety.
ISSN
1616-301X
URI
https://hdl.handle.net/10371/179801
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College of Engineering/Engineering Practice School (공과대학/대학원)Dept. of Materials Science and Engineering (재료공학부)Journal Papers (저널논문_재료공학부)
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