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Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries

Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries High-entropy (HE) ceramics, by analogy with HE metallic alloys, are an emerging class of solid solutions composed of a large number of species. These materials offer the benefit of large compositional flexibility and can be used in a wide variety of applications, including thermoelectrics, catalysts, superionic conductors and battery electrodes. We show here that the HE concept can lead to very substantial improvements in performance in battery cathodes. Among lithium-ion cathodes, cation-disordered rocksalt (DRX)-type materials are an ideal platform within which to design HE materials because of their demonstrated chemical flexibility. By comparing a group of DRX cathodes containing two, four or six transition metal (TM) species, we show that short-range order systematically decreases, whereas energy density and rate capability systematically increase, as more TM cation species are mixed together, despite the total metal content remaining fixed. A DRX cathode with six TM species achieves 307 mAh g−1 (955 Wh kg−1) at a low rate (20 mA g−1), and retains more than 170 mAh g−1 when cycling at a high rate of 2,000 mA g−1. To facilitate further design in this HE DRX space, we also present a compatibility analysis of 23 different TM ions, and successfully synthesize a phase-pure HE DRX compound containing 12 TM species as a proof of concept. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Nature Materials Springer Journals

Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries

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References (72)

Publisher
Springer Journals
Copyright
Copyright © This is a U.S. government work and not under copyright protection in the U.S.; foreign copyright protection may apply 2020
ISSN
1476-1122
eISSN
1476-4660
DOI
10.1038/s41563-020-00816-0
Publisher site
See Article on Publisher Site

Abstract

High-entropy (HE) ceramics, by analogy with HE metallic alloys, are an emerging class of solid solutions composed of a large number of species. These materials offer the benefit of large compositional flexibility and can be used in a wide variety of applications, including thermoelectrics, catalysts, superionic conductors and battery electrodes. We show here that the HE concept can lead to very substantial improvements in performance in battery cathodes. Among lithium-ion cathodes, cation-disordered rocksalt (DRX)-type materials are an ideal platform within which to design HE materials because of their demonstrated chemical flexibility. By comparing a group of DRX cathodes containing two, four or six transition metal (TM) species, we show that short-range order systematically decreases, whereas energy density and rate capability systematically increase, as more TM cation species are mixed together, despite the total metal content remaining fixed. A DRX cathode with six TM species achieves 307 mAh g−1 (955 Wh kg−1) at a low rate (20 mA g−1), and retains more than 170 mAh g−1 when cycling at a high rate of 2,000 mA g−1. To facilitate further design in this HE DRX space, we also present a compatibility analysis of 23 different TM ions, and successfully synthesize a phase-pure HE DRX compound containing 12 TM species as a proof of concept.

Journal

Nature Materials – Springer Journals

Published: Oct 12, 2020

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