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<p>Layered oxide cathodes for lithium-ion batteries typically undergo large expansion and contraction during cycling, including a particularly abrupt shrinkage along the <i>c</i> lattice (<i>c</i>-collapse) at high states of charge, which limits their lifetime. Here we suppress the <i>c</i>-collapse in compositionally simple LiNi<sub>0.9</sub>Mn<sub>0.1</sub>O<sub>2</sub> 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 (TM<sub>Li</sub>) reaches ≥12%, the <i>c</i>-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.</p>

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

  • 期刊论文

  • 发表日期：

    2025年11月27日

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  • Junghwa Lee,
  • Zhelong Jiang,
  • Nicolas B. Liang,
  • Jin Hwan Kwak,
  • Howie Nguyen,
  • Grace M. Busse,
  • Yiseul Yoo,
  • Hari Ramachandran,
  • Kipil Lim,
  • Peter M. Csernica,
  • Tianyi Li,
  • Xin Xu,
  • Kyung Yoon Chung,
  • Kathrin Michel,
  • Joop E. Frerichs,
  • William E. Gent,
  • Raphaële J. Clément,
  • Jungjin Park,
  • William C. Chueh

摘要

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.