Ultrahigh power and energy density in partially ordered lithium-ion cathode materials

Huiwen Ji, Jinpeng Wu, Zijian Cai, Jue Liu, Deok-Hwang Kwon, Hyunchul Kim, Alexander Urban, Joseph K. Papp, Emily Foley, Yaosen Tian, Mahalingam Balasubramanian, Haegyeom Kim, Raphaële J. Clément, Bryan D. McCloskey, Wanli Yang and Gerbrand Ceder ()
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Huiwen Ji: University of California Berkeley
Jinpeng Wu: The Advanced Light Source, Lawrence Berkeley National Laboratory
Zijian Cai: University of California Berkeley
Jue Liu: Neutron Scattering Division, Oak Ridge National Laboratory
Deok-Hwang Kwon: University of California Berkeley
Hyunchul Kim: Materials Sciences Division, Lawrence Berkeley National Laboratory
Alexander Urban: Columbia University
Joseph K. Papp: University of California Berkeley
Emily Foley: University of California Santa Barbara
Yaosen Tian: University of California Berkeley
Mahalingam Balasubramanian: Advanced Photon Source, Argonne National Laboratory
Haegyeom Kim: Materials Sciences Division, Lawrence Berkeley National Laboratory
Raphaële J. Clément: University of California Santa Barbara
Bryan D. McCloskey: Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory
Wanli Yang: The Advanced Light Source, Lawrence Berkeley National Laboratory
Gerbrand Ceder: University of California Berkeley

Nature Energy, 2020, vol. 5, issue 3, 213-221

Abstract: Abstract The rapid market growth of rechargeable batteries requires electrode materials that combine high power and energy and are made from earth-abundant elements. Here we show that combining a partial spinel-like cation order and substantial lithium excess enables both dense and fast energy storage. Cation overstoichiometry and the resulting partial order is used to eliminate the phase transitions typical of ordered spinels and enable a larger practical capacity, while lithium excess is synergistically used with fluorine substitution to create a high lithium mobility. With this strategy, we achieved specific energies greater than 1,100 Wh kg–1 and discharge rates up to 20 A g–1. Remarkably, the cathode materials thus obtained from inexpensive manganese present a rare case wherein an excellent rate capability coexists with a reversible oxygen redox activity. Our work shows the potential for designing cathode materials in the vast space between fully ordered and disordered compounds.

Date: 2020
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DOI: 10.1038/s41560-020-0573-1

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