Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries
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-puremore »
- Authors:
-
[1];
[3];
[2];
[4];
[1];
[2];
[1];
[2];
[3];
[2];
[1]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of California, Santa Barbara, CA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
- OSTI Identifier:
- 1766546
- Alternate Identifier(s):
- OSTI ID: 1776801
- Grant/Contract Number:
- AC02-05CH11231; AC02-06CH11357; SC0012704; NSF-DMR-1720256; ACI1053575
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 2; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; batteries; theory and computation
Citation Formats
Lun, Zhengyan, Ouyang, Bin, Kwon, Deok-Hwang, Ha, Yang, Foley, Emily E., Huang, Tzu-Yang, Cai, Zijian, Kim, Hyunchul, Balasubramanian, Mahalingam, Sun, Yingzhi, Huang, Jianping, Tian, Yaosen, Kim, Haegyeom, McCloskey, Bryan D., Yang, Wanli, Clément, Raphaële J., Ji, Huiwen, and Ceder, Gerbrand. Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries. United States: N. p., 2020.
Web. doi:10.1038/s41563-020-00816-0.
Lun, Zhengyan, Ouyang, Bin, Kwon, Deok-Hwang, Ha, Yang, Foley, Emily E., Huang, Tzu-Yang, Cai, Zijian, Kim, Hyunchul, Balasubramanian, Mahalingam, Sun, Yingzhi, Huang, Jianping, Tian, Yaosen, Kim, Haegyeom, McCloskey, Bryan D., Yang, Wanli, Clément, Raphaële J., Ji, Huiwen, & Ceder, Gerbrand. Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries. United States. https://doi.org/10.1038/s41563-020-00816-0
Lun, Zhengyan, Ouyang, Bin, Kwon, Deok-Hwang, Ha, Yang, Foley, Emily E., Huang, Tzu-Yang, Cai, Zijian, Kim, Hyunchul, Balasubramanian, Mahalingam, Sun, Yingzhi, Huang, Jianping, Tian, Yaosen, Kim, Haegyeom, McCloskey, Bryan D., Yang, Wanli, Clément, Raphaële J., Ji, Huiwen, and Ceder, Gerbrand. Mon .
"Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries". United States. https://doi.org/10.1038/s41563-020-00816-0. https://www.osti.gov/servlets/purl/1766546.
@article{osti_1766546,
title = {Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries},
author = {Lun, Zhengyan and Ouyang, Bin and Kwon, Deok-Hwang and Ha, Yang and Foley, Emily E. and Huang, Tzu-Yang and Cai, Zijian and Kim, Hyunchul and Balasubramanian, Mahalingam and Sun, Yingzhi and Huang, Jianping and Tian, Yaosen and Kim, Haegyeom and McCloskey, Bryan D. and Yang, Wanli and Clément, Raphaële J. and Ji, Huiwen and Ceder, Gerbrand},
abstractNote = {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.},
doi = {10.1038/s41563-020-00816-0},
journal = {Nature Materials},
number = 2,
volume = 20,
place = {United States},
year = {Mon Oct 12 00:00:00 EDT 2020},
month = {Mon Oct 12 00:00:00 EDT 2020}
}
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