Reversible Mn2+/Mn4+ double redox in lithium-excess cathode materials

Jinhyuk Lee (), Daniil A. Kitchaev, Deok-Hwang Kwon, Chang-Wook Lee, Joseph K. Papp, Yi-Sheng Liu, Zhengyan Lun, Raphaële J. Clément, Tan Shi, Bryan D. McCloskey, Jinghua Guo, Mahalingam Balasubramanian and Gerbrand Ceder ()
Additional contact information
Jinhyuk Lee: University of California
Daniil A. Kitchaev: Massachusetts Institute of Technology
Deok-Hwang Kwon: University of California
Chang-Wook Lee: Advanced Photon Source, Argonne National Laboratory
Joseph K. Papp: University of California
Yi-Sheng Liu: Lawrence Berkeley National Laboratory
Zhengyan Lun: University of California
Raphaële J. Clément: University of California
Tan Shi: University of California
Bryan D. McCloskey: University of California
Jinghua Guo: Lawrence Berkeley National Laboratory
Mahalingam Balasubramanian: Advanced Photon Source, Argonne National Laboratory
Gerbrand Ceder: University of California

Nature, 2018, vol. 556, issue 7700, 185-190

Abstract: Abstract There is an urgent need for low-cost, resource-friendly, high-energy-density cathode materials for lithium-ion batteries to satisfy the rapidly increasing need for electrical energy storage. To replace the nickel and cobalt, which are limited resources and are associated with safety problems, in current lithium-ion batteries, high-capacity cathodes based on manganese would be particularly desirable owing to the low cost and high abundance of the metal, and the intrinsic stability of the Mn4+ oxidation state. Here we present a strategy of combining high-valent cations and the partial substitution of fluorine for oxygen in a disordered-rocksalt structure to incorporate the reversible Mn2+/Mn4+ double redox couple into lithium-excess cathode materials. The lithium-rich cathodes thus produced have high capacity and energy density. The use of the Mn2+/Mn4+ redox reduces oxygen redox activity, thereby stabilizing the materials, and opens up new opportunities for the design of high-performance manganese-rich cathodes for advanced lithium-ion batteries.

Date: 2018
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DOI: 10.1038/s41586-018-0015-4

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