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Title: Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials

Recent progress in the understanding of percolation theory points to cation-disordered lithium-excess transition metal oxides as high-capacity lithium-ion cathode materials. Nevertheless, the oxygen redox processes required for these materials to deliver high capacity can trigger oxygen loss, which leads to the formation of resistive surface layers on the cathode particles. Here, we demonstrate here that, somewhat surprisingly, fluorine can be incorporated into the bulk of disordered lithium nickel titanium molybdenum oxides using a standard solid-state method to increase the nickel content, and that this compositional modification is very effective in reducing oxygen loss, improving energy density, average voltage, and rate performance. We argue that the valence reduction on the anion site, offered by fluorine incorporation, opens up significant opportunities for the design of high-capacity cation-disordered cathode materials.
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [3] ;  [1] ;  [1] ; ORCiD logo [3] ;  [4] ;  [5]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  2. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  4. Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
  5. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
Publication Date:
Grant/Contract Number:
AC02-05CH11231; DGE-1106400
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Batteries
OSTI Identifier:
1419450

Lee, Jinhyuk, Papp, Joseph K., Clément, Raphaële J., Sallis, Shawn, Kwon, Deok-Hwang, Shi, Tan, Yang, Wanli, McCloskey, Bryan D., and Ceder, Gerbrand. Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials. United States: N. p., Web. doi:10.1038/s41467-017-01115-0.
Lee, Jinhyuk, Papp, Joseph K., Clément, Raphaële J., Sallis, Shawn, Kwon, Deok-Hwang, Shi, Tan, Yang, Wanli, McCloskey, Bryan D., & Ceder, Gerbrand. Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials. United States. doi:10.1038/s41467-017-01115-0.
Lee, Jinhyuk, Papp, Joseph K., Clément, Raphaële J., Sallis, Shawn, Kwon, Deok-Hwang, Shi, Tan, Yang, Wanli, McCloskey, Bryan D., and Ceder, Gerbrand. 2017. "Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials". United States. doi:10.1038/s41467-017-01115-0. https://www.osti.gov/servlets/purl/1419450.
@article{osti_1419450,
title = {Mitigating oxygen loss to improve the cycling performance of high capacity cation-disordered cathode materials},
author = {Lee, Jinhyuk and Papp, Joseph K. and Clément, Raphaële J. and Sallis, Shawn and Kwon, Deok-Hwang and Shi, Tan and Yang, Wanli and McCloskey, Bryan D. and Ceder, Gerbrand},
abstractNote = {Recent progress in the understanding of percolation theory points to cation-disordered lithium-excess transition metal oxides as high-capacity lithium-ion cathode materials. Nevertheless, the oxygen redox processes required for these materials to deliver high capacity can trigger oxygen loss, which leads to the formation of resistive surface layers on the cathode particles. Here, we demonstrate here that, somewhat surprisingly, fluorine can be incorporated into the bulk of disordered lithium nickel titanium molybdenum oxides using a standard solid-state method to increase the nickel content, and that this compositional modification is very effective in reducing oxygen loss, improving energy density, average voltage, and rate performance. We argue that the valence reduction on the anion site, offered by fluorine incorporation, opens up significant opportunities for the design of high-capacity cation-disordered cathode materials.},
doi = {10.1038/s41467-017-01115-0},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {2017},
month = {10}
}

Works referenced in this record:

Solvents’ Critical Role in Nonaqueous Lithium–Oxygen Battery Electrochemistry
journal, May 2011
  • McCloskey, B. D.; Bethune, D. S.; Shelby, R. M.
  • The Journal of Physical Chemistry Letters, Vol. 2, Issue 10, p. 1161-1166
  • DOI: 10.1021/jz200352v