Disordered Rocksalts as High?Energy and Earth?Abundant Li?Ion Cathodes

Disordered rocksalts with lithium excess (DRX) offer a new direction in Li?ion cathode design beyond conventional Ni? and Co?based materials. This review highlights the design principles, synthesis strategies, and performance optimization of DRX oxides and oxyfluorides for energy?dense, sustainable batteries using Earth?abundant transition metals and tailored cation disorder.To address the growing demand for energy and support the shift toward transportation electrification and intermittent renewable energy, there is an urgent need for low?cost, energy?dense electrical storage. Research on Li?ion electrode materials has predominantly focused on ordered materials with well?defined lithium diffusion channels, limiting cathode design to resource?constrained Ni? and Co?based oxides and lower?energy polyanion compounds. Recently, disordered rocksalts with lithium excess (DRX) have demonstrated high capacity and energy density when lithium excess and/or local ordering allow statistical percolation of lithium sites through the structure. This cation disorder can be induced by high temperature synthesis or mechanochemical synthesis methods for a broad range of compositions. DRX oxides and oxyfluorides containing Earth?abundant transition metals have been prepared using various synthesis routes, including solid?state, molten?salt, and sol?gel reactions. This review outlines DRX design principles and explains the effect of synthesis conditions on cation disorder and short?range cation ordering (SRO), which determines the cycling stability and rate capability. In addition, strategies to enhance Li transport and capacity retention with Mn?rich DRX possessing partial spinel?like ordering are discussed. Finally, the review considers the optimization of carbon and electrolyte in DRX materials and addresses key challenges and opportunities for commercializing DRX cathodes.

» Publication Date: 06/05/2025

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