Alexander Urban

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

Disorderly Flow Lithium batteries are becoming ever more important in society. While their application used to be confined to portable electronics, they are now becoming the enabling technology for electric vehicles and grid storage for renewables. Generally, the flow of lithium ions into and out of battery electrodes is thought to require ordered materials. Lee et al. (p. 519, published online 9 January) used a combination of experimental work and computations to identify disordered electrode materials with high Li diffusion. The improved energy density properties could be attributed to compositions with excess lithium beyond the stoichiometric limit, leading to intermixing between the lithium and transition metal sublattices and the formation of a percolation network providing specific lithium transport pathways. Cation-disordered compounds achieve high lithium (Li) storage capacity, with scope for high–energy density Li battery electrodes. Nearly all high–energy density cathodes for rechargeable lithium batteries are well-ordered materials in which 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 a certain type of active diffusion channels in disordered Li-excess materials. A unified understanding of high performance in both layered and Li-excess materials may enable the design of disordered-electrode materials with high capacity and high energy density.