Issue 23, 2024

Intrinsic mechanism of Co/Mn elemental manipulation in enhancing the cycling stability of single-crystal ultrahigh-nickel layered cathodes

Abstract

Ultrahigh-nickel layers suffer from poor cycling stability. Ultrahigh-nickel single-crystal cathodes with Co/Mn elements doped in the transition metal layer are considered promising to overcome this challenge via effectively mitigating the microcrack issue. However, the intrinsic mechanism by which Co/Mn elements enhance the cycling stability of single-crystal ultrahigh-nickel cathodes, as well as the dominant role of structural evolution and surface side reactions in the cycling fading of single-crystal cathodes, remains unclear. Herein, the single-crystal LiNiO2 (SC-N) with manipulated Co/Mn doping as LiNi0.9Co0.1O2 (SC-NC) and LiNi0.9Mn0.1O2 (SC-NM) oxides are synthesized to reveal the correlation between crystal structural evolution and electrochemical performance. The alleviated intensity and delayed onset potential of H2/H3 phase transition in the SC-NM cathode effectively mitigate the abrupt anisotropic lattice collapse, thereby enhancing the morphology integrity of the particles. Despite a higher cation mixing degree, the excellent structural stability derived from the reversible H2/H3 phase transition also provides favorable kinetics for repeated lithiation/delithiation. As a result, the Co-free SC-NM cathode can exhibit unconventional cycling stability with a capacity retention of 93.8% after 100 cycles at 0.5C between 2.7 and 4.3 V compared to the SC-N and SC-NC cathodes with capacity retention values of 71.7% and 81.1%, respectively under the same condition. This study emphasizes the importance of regulating the crystal structure evolution via Co/Mn manipulation in constructing high-performance single-crystal ultrahigh-nickel layered cathodes.

Graphical abstract: Intrinsic mechanism of Co/Mn elemental manipulation in enhancing the cycling stability of single-crystal ultrahigh-nickel layered cathodes

Supplementary files

Article information

Article type
Paper
Submitted
01 Mar 2024
Accepted
23 Apr 2024
First published
24 Apr 2024

J. Mater. Chem. A, 2024,12, 13724-13732

Intrinsic mechanism of Co/Mn elemental manipulation in enhancing the cycling stability of single-crystal ultrahigh-nickel layered cathodes

D. Han, J. Chen, W. Li, L. Xie, Z. Yan, Z. Tang, H. Wu, J. Peng, O. Dolotko, Y. Zhao, W. Hua, Y. Wu and W. Tang, J. Mater. Chem. A, 2024, 12, 13724 DOI: 10.1039/D4TA01437E

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