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 LiNi_0.9Mn_0.1O₂ 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.

Article in Nature Energy : Eliminating lattice collapse in dopant-free LiNi_0.9Mn_0.1O₂ cathodes via electrochemically induced partial cation disorder

News & Views in Nature Energy : Electrochemically induced imperfections

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