Abstract
Multielectron reaction electrode materials using partial oxygen redox can be potentially used as cathodes in lithium-ion batteries, as they offer numerous advantages, including high reversible capacity and energy density and low cost. Here, a reversible three-electron reaction is demonstrated utilizing topotactic phase transition between antifluorite and rocksalt in a cation-disordered antifluorite-type cubic Li6CoO4 cathode. This cubic phase is synthesized by a simple mechanochemical treatment of conventionally prepared tetragonal Li6CoO4. It displays a reversible capacity of 487 mAh g-1, a high value because of a reversible three-electron reaction using Co2+/Co3+, Co3+/Co4+, and O2-/O22- redox, occurring without O2 gas evolution. The mechanochemical treatment is assumed to reduce its lattice distortion by cation-disordering and facilitate a reversible topotactic phase transition between antifluorite and rocksalt structures via a dynamic cation pushing mechanism.
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