Unlocking the Potential of Cation-Disordered Oxides for Rechargeable Lithium Batteries

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Science  09 Jan 2014:
DOI: 10.1126/science.1246432

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Nearly all high energy density cathodes for rechargeable lithium batteries are well-ordered materials where lithium and other cations occupy distinct sites. Cation-disordered materials are generally disregarded as cathodes because lithium diffusion tends to be limited by their structures. The performance of Li1.211Mo0.467Cr0.3O2 shows that lithium diffusion can be facile in disordered materials. Using ab initio computations, we demonstrate that this unexpected behavior is due to percolation of certain diffusion channels that are active in disordered structures, but is unique to Li excess materials. This leads to a unified understanding of high performance in both layered and Li excess materials, and opens up an exciting new direction for designing disordered electrode materials with high capacity and high energy density.

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