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Design principles for high transition metal capacity in disordered rocksalt Li-ion cathodes

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Abstract

The discovery of facile Li transport in disordered, Li-excess rocksalt materials has opened a vast new chemical space for the development of high energy density, low cost Li-ion cathodes. We develop a strategy for obtaining optimized compositions within this class of materials, exhibiting high capacity and energy density as well as good reversibility, by using a combination of low-valence transition metal redox and a high-valence redox active charge compensator, as well as fluorine substitution for oxygen. Furthermore, we identify a new constraint on high-performance compositions by demonstrating the necessity of excess Li capacity as a means of counteracting high-voltage tetrahedral Li formation, Li-binding by fluorine and the associated irreversibility. Specifically, we demonstrate that 10–12% of Li capacity is lost due to tetrahedral Li formation, and 0.4–0.8 Li per F dopant is made inaccessible at moderate voltages due to Li–F binding. We demonstrate the success of this strategy by realizing a series of high-performance disordered oxyfluoride cathode materials based on Mn2+/4+ and V4+/5+ redox.

Graphical abstract: Design principles for high transition metal capacity in disordered rocksalt Li-ion cathodes

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Publication details

The article was received on 19 Mar 2018, accepted on 24 May 2018 and first published on 24 May 2018


Article type: Paper
DOI: 10.1039/C8EE00816G
Citation: Energy Environ. Sci., 2018, Advance Article
  • Open access: Creative Commons BY-NC license
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    Design principles for high transition metal capacity in disordered rocksalt Li-ion cathodes

    D. A. Kitchaev, Z. Lun, W. D. Richards, H. Ji, R. J. Clément, M. Balasubramanian, D. Kwon, K. Dai, J. K. Papp, T. Lei, B. D. McCloskey, W. Yang, J. Lee and G. Ceder, Energy Environ. Sci., 2018, Advance Article , DOI: 10.1039/C8EE00816G

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