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Title: Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides

Abstract

© 2017 The Author(s). Lithium-rich layered transition metal oxide positive electrodes offer access to anion redox at high potentials, thereby promising high energy densities for lithium-ion batteries. However, anion redox is also associated with several unfavorable electrochemical properties, such as open-circuit voltage hysteresis. Here we reveal that in Li 1.17-x Ni 0.21 Co 0.08 Mn 0.54 O 2 , these properties arise from a strong coupling between anion redox and cation migration. We combine various X-ray spectroscopic, microscopic, and structural probes to show that partially reversible transition metal migration decreases the potential of the bulk oxygen redox couple by > 1 V, leading to a reordering in the anionic and cationic redox potentials during cycling. First principles calculations show that this is due to the drastic change in the local oxygen coordination environments associated with the transition metal migration. We propose that this mechanism is involved in stabilizing the oxygen redox couple, which we observe spectroscopically to persist for 500 charge/discharge cycles.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3];  [5]; ORCiD logo [6];  [7];  [2];  [8];  [9];  [6];  [7];  [10]; ORCiD logo [10];  [10];  [5];  [5]; ORCiD logo [11]; ORCiD logo [10] more »; ORCiD logo [3];  [12] « less
+ Show Author Affiliations
  1. Stanford Univ., CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  2. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS); Shandong Univ., Jinan (China). School of Physics, National Key Lab. of Crystal Materials
  5. Samsung Advanced Inst. of Technology, Samsung-ro, Yeongtong-gu Suwon-si (South Korea)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  7. Stanford Univ., CA (United States). Dept. of Computer Science
  8. Energy1lab, Samsung SDI, Samsung-ro, Yeongtong-gu Suwon-si (South Korea)
  9. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  10. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
  12. Stanford Univ., CA (United States). Dept. of Materials Science and Engineering; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1417012
Alternate Identifier(s):
OSTI ID: 1416944
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231
Resource 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
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; Batteries; Solid-state chemistry

Citation Formats

Gent, William E., Lim, Kipil, Liang, Yufeng, Li, Qinghao, Barnes, Taylor, Ahn, Sung-Jin, Stone, Kevin H., McIntire, Mitchell, Hong, Jihyun, Song, Jay Hyok, Li, Yiyang, Mehta, Apurva, Ermon, Stefano, Tyliszczak, Tolek, Kilcoyne, David, Vine, David, Park, Jin-Hwan, Doo, Seok-Kwang, Toney, Michael F., Yang, Wanli, Prendergast, David, and Chueh, William C. Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides. United States: N. p., 2017. Web. doi:10.1038/s41467-017-02041-x.
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Gent, William E., Lim, Kipil, Liang, Yufeng, Li, Qinghao, Barnes, Taylor, Ahn, Sung-Jin, Stone, Kevin H., McIntire, Mitchell, Hong, Jihyun, Song, Jay Hyok, Li, Yiyang, Mehta, Apurva, Ermon, Stefano, Tyliszczak, Tolek, Kilcoyne, David, Vine, David, Park, Jin-Hwan, Doo, Seok-Kwang, Toney, Michael F., Yang, Wanli, Prendergast, David, & Chueh, William C. Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides. United States. https://doi.org/10.1038/s41467-017-02041-x
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Gent, William E., Lim, Kipil, Liang, Yufeng, Li, Qinghao, Barnes, Taylor, Ahn, Sung-Jin, Stone, Kevin H., McIntire, Mitchell, Hong, Jihyun, Song, Jay Hyok, Li, Yiyang, Mehta, Apurva, Ermon, Stefano, Tyliszczak, Tolek, Kilcoyne, David, Vine, David, Park, Jin-Hwan, Doo, Seok-Kwang, Toney, Michael F., Yang, Wanli, Prendergast, David, and Chueh, William C. Tue . "Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides". United States. https://doi.org/10.1038/s41467-017-02041-x. https://www.osti.gov/servlets/purl/1417012.
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@article{osti_1417012,
title = {Coupling between oxygen redox and cation migration explains unusual electrochemistry in lithium-rich layered oxides},
author = {Gent, William E. and Lim, Kipil and Liang, Yufeng and Li, Qinghao and Barnes, Taylor and Ahn, Sung-Jin and Stone, Kevin H. and McIntire, Mitchell and Hong, Jihyun and Song, Jay Hyok and Li, Yiyang and Mehta, Apurva and Ermon, Stefano and Tyliszczak, Tolek and Kilcoyne, David and Vine, David and Park, Jin-Hwan and Doo, Seok-Kwang and Toney, Michael F. and Yang, Wanli and Prendergast, David and Chueh, William C.},
abstractNote = {© 2017 The Author(s). Lithium-rich layered transition metal oxide positive electrodes offer access to anion redox at high potentials, thereby promising high energy densities for lithium-ion batteries. However, anion redox is also associated with several unfavorable electrochemical properties, such as open-circuit voltage hysteresis. Here we reveal that in Li 1.17-x Ni 0.21 Co 0.08 Mn 0.54 O 2 , these properties arise from a strong coupling between anion redox and cation migration. We combine various X-ray spectroscopic, microscopic, and structural probes to show that partially reversible transition metal migration decreases the potential of the bulk oxygen redox couple by > 1 V, leading to a reordering in the anionic and cationic redox potentials during cycling. First principles calculations show that this is due to the drastic change in the local oxygen coordination environments associated with the transition metal migration. We propose that this mechanism is involved in stabilizing the oxygen redox couple, which we observe spectroscopically to persist for 500 charge/discharge cycles.},
doi = {10.1038/s41467-017-02041-x},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Tue Dec 12 00:00:00 EST 2017},
month = {Tue Dec 12 00:00:00 EST 2017}
}
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