Issue 9, 2025

Exploring a new synthesis route to lithium-excess disordered rock salt (DRX) cathode materials

Abstract

Lithium-excess disordered rock salt (DRX) materials are promising candidates for Co/Ni-free Li-ion cathodes due to their high specific energy (800+ W h kg−1) and compositional flexibility. DRX cathodes are typically synthesized using solid-state reactions, which are difficult to scale and provide little-to-no control over particle morphology. To address this bottleneck, the present study reports a two-step, solution-based reaction route to prepare Mn/Ti-based DRX oxyfluoride cathodes with nominal compositions of Li1.25Mn0.5Ti0.3O1.95F0.05 and Li1.35Mn0.7Ti0.1O1.85F0.15. More specifically, a glycine–nitrate combustion reaction is used to produce a lithiated transition metal oxide, which is further reacted with LiF to produce high-purity DRX powders. Remarkably, this route yields 80–90% pure DRX after annealing for 1 h at 800–1000 °C, and 19F solid-state nuclear magnetic resonance (ssNMR) spectra demonstrate that F anions are successfully incorporated into the DRX structure. Cathodes prepared using this approach exhibit promising electrochemical performance, with Li1.35Mn0.7Ti0.1O1.85F0.15 attaining reversible capacities ∼210 mA h g−1 and moderate cycling stability in half cells (65% capacity retention over 150 cycles). Overall, these results demonstrate that utilizing novel metal oxide precursors presents a viable and largely unexplored method to produce high-performance Co/Ni-free DRX cathodes.

Graphical abstract: Exploring a new synthesis route to lithium-excess disordered rock salt (DRX) cathode materials

Supplementary files

Article information

Article type
Paper
Submitted
27 Dec 2024
Accepted
06 Apr 2025
First published
23 Apr 2025

Mater. Adv., 2025,6, 2990-3001

Exploring a new synthesis route to lithium-excess disordered rock salt (DRX) cathode materials

M. S. Chambers, T. Li, Z. Liang, J. Keum, K. H. Stone, R. J. Clément, B. L. Armstrong and E. C. Self, Mater. Adv., 2025, 6, 2990 DOI: 10.1039/D4MA01287A

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