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We find that cation short-range order (SRO) is important in determining the amount of kinetically extractable Li in DRX materials as the Li transport relies on percolation through a 3D network. However, in this study, we show that even minor deviations from randomness, not detectable by typical X-ray diffraction (XRD), can have profound influence on performance. f, g Voltage profiles of LMZO and LMTO between 1.5 and 4.7вЂ‰V for the first 10 cycles at room temperature d, e SEM images (scale bars, 500вЂ‰nm) of shaker-milled LMTO (s-LMTO) and LMZO (s-LMZO) with similar particle sizes of ~100вЂ‰nm. The low-angle shift in the pattern of LMZO compared with that of LMTO indicates the larger lattice parameter of LMZO. c XRD patterns of LMZO and LMTO indexed according to the rocksalt structure. The migrating Li ion is highlighted in cyan. The energy barrier depends on the local environment and size of the tetrahedron. b Schematic energy landscape of Li migration from its octahedral coordination through a tetrahedral vacancy into another octahedron. The highlighted blue tetrahedral site represents a typical migration pathway for Li diffusion. Both cations and anions are in octahedral coordination. The black spheres represent metal cations (including lithium and TMs), and the red spheres represent oxygen anions. a Crystal structure of an ideal cation-disordered rocksalt-type lithium metal oxide. If the cation arrangement is random, any DRX with the same Li to TM ratio should have an equivalent distribution of Li-migration channel types and thus similar Li transport properties.Д¬haracterization and electrochemical performance of Li 1.2Mn 0.4Zr 0.4O 2 (LMZO) and Li 1.2Mn 0.4Ti 0.4O 2 (LMTO). The Li-migration barrier depends on the tetrahedron height 3, 16, 17, 18 and the number of transition metal (TM) ions within the environment (i.e. The highlighted tetrahedron represents a channel through which Li migrates 15 (Fig. A prevailing assumption when studying DRX cathodes is that all the cation species are randomly distributed.ДЇigure 1a presents a typical DRX crystal structure. Many new cathode materials, in some cases containing only earth-abundant elements (e.g., Fe, Mn, and Ti) have been developed in this category, such as Li 1.3Mn 0.4Nb 0.3O 2 5, Li 1.2Mn 0.4Ti 0.4O 2 6, Li 1.2Ni 1/3Ti 1/3Mo 2/15O 2 7, Li 4Mn 2O 5 8, and Li 2FeV 0.5Ti 0.5O 4 9 as well as their fluorinated variants 10, 11, 12, 13, 14. Their ability to function without requiring cation ordering has enabled novel cathodes with remarkable chemical diversity 3, 4. However, we demonstrate in this paper that in the recently discovered class of Li-excess cation-disordered rocksalt (DRX) cathodes, the chemistry of then non-redox-active stabilizers plays a critical role in performance through subtle structural changes.ДRX materials were recently shown to have facile LiВ transport enabled by a percolating network of Li-rich environments 3. Traditionally, one thinks of redox-active elements, such as Ni and Co, and stabilizers, such as Mn 4+ in NMC-class materials 2. Rational design of cathodes requires an understanding of the precise role that each chemical component has in determining performance. The development of cost-effective lithium (Li) ion batteries depends on the discovery of high-energy-density cathode materials composed of non-precious elements 1.

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