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Energy Materials and Systems (EMS) Laboratory

Research Highlights

2026 Eliminating lattice collapse in dopant-free LiNi0.9Mn0.1O2 cathodes via electrochemically induced partial cation disorder

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작성자 최고관리자 작성일 26-01-01 13:44

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Author
Junghwa Lee, Zhelong Jiang, Nicolas Liang, Jin Hwan Kwak, Howie Nguyen, Grace Busse, Yiseul Yoo, Hari Ramachandran, Kipil Lim, Peter Csernica, Tianyi Li ,Xin Xu, Kyung Yoon Chung, Kathrin Michel, Joop Frerichs, William Gent, Raphaële Clément, Jungjin Park,* William Chueh*
Journal
Nature Energy
Vol
11
Page
87-97
Year
2026

Layered oxide cathodes for lithium-ion batteries typically undergo large expansion and contraction during cycling, including a particularly abrupt shrinkage along the c lattice (c-collapse) at high states-of-charge, which limits their lifetime. Here, we suppress the c-collapse in compositionally-simple LiNi0.9Mn0.1O2 by electrochemically inducing partial disorder that is permanently retained throughout the bulk. Our approach leverages irreversible oxygen oxidation in Li-excess Ni-rich oxides to activate partial disordering of the cation sublattice, while preserving the long-range layered structure. By varying the initial Li-excess, we obtain Li-stoichiometric transition metal oxides with tunable cation disorder. Surprisingly, when the concentration of transition metal ions occupying Li sites (TMLi) reaches ≥12%, the c lattice parameter remains nearly invariant during (de)lithiation, reducing chemical strain, preserving microstructural integrity, and extending battery cycle life. The resulting material displays high specific capacity, long-term stability, small voltage hysteresis, and negligible voltage decay. This concept opens the possibility of designing materials by inducing persistent intrinsic disorder electrochemically.


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