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Title: Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging

Abstract

Lithium-rich layered oxides (LRLO) are among the leading candidates for the next-generation cathode material for energy storage, delivering 50% excess capacity over commercially used compounds. Despite excellent prospects, voltage fade has prevented effective use of the excess capacity, and a major challenge has been a lack of understanding of the mechanisms underpinning the voltage fade. Here, using operando three-dimensional Bragg coherent diffractive imaging, we directly observe the nucleation of a mobile dislocation network in LRLO nanoparticles. The dislocations form more readily in LRLO as compared with a classical layered oxide, suggesting a link between the defects and voltage fade. We show microscopically how the formation of partial dislocations contributes to the voltage fade. The insights allow us to design and demonstrate an effective method to recover the original high-voltage functionality. Furthermore, our findings reveal that the voltage fade in LRLO is reversible and call for new paradigms for improved design of oxygen-redox active materials.

Authors:
 [1];  [2];  [2];  [2];  [2];  [2]; ORCiD logo [3];  [3];  [3];  [4];  [2];  [2];  [2];  [5];  [6];  [7];  [7];  [2];  [2]
+ Show Author Affiliations
  1. Univ. of California-San Diego, La Jolla, CA (United States); Cornell Univ., Ithaca, NY (United States)
  2. Univ. of California-San Diego, La Jolla, CA (United States)
  3. Chinese Academy of Sciences, Zhejiang (China)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  6. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European XFEL GmbH, Schenefeld (Germany)
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1770701
Alternate Identifier(s):
OSTI ID: 1481914
Grant/Contract Number:  
EE0007744; AC02-06CH11357; SC0001805; SC0012583
Resource Type:
Accepted Manuscript
Journal Name:
Nature Energy
Additional Journal Information:
Journal Volume: 3; Journal Issue: 8; Journal ID: ISSN 2058-7546
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Singer, A., Zhang, M., Hy, S., Cela, D., Fang, C., Wynn, T. A., Qiu, B., Xia, Y., Liu, Z., Ulvestad, A., Hua, N., Wingert, J., Liu, H., Sprung, M., Zozulya, A. V., Maxey, E., Harder, R., Meng, Y. S., and Shpyrko, O. G. Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging. United States: N. p., 2018. Web. doi:10.1038/s41560-018-0184-2.
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Singer, A., Zhang, M., Hy, S., Cela, D., Fang, C., Wynn, T. A., Qiu, B., Xia, Y., Liu, Z., Ulvestad, A., Hua, N., Wingert, J., Liu, H., Sprung, M., Zozulya, A. V., Maxey, E., Harder, R., Meng, Y. S., & Shpyrko, O. G. Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging. United States. https://doi.org/10.1038/s41560-018-0184-2
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Singer, A., Zhang, M., Hy, S., Cela, D., Fang, C., Wynn, T. A., Qiu, B., Xia, Y., Liu, Z., Ulvestad, A., Hua, N., Wingert, J., Liu, H., Sprung, M., Zozulya, A. V., Maxey, E., Harder, R., Meng, Y. S., and Shpyrko, O. G. Mon . "Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging". United States. https://doi.org/10.1038/s41560-018-0184-2. https://www.osti.gov/servlets/purl/1770701.
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@article{osti_1770701,
title = {Nucleation of dislocations and their dynamics in layered oxide cathode materials during battery charging},
author = {Singer, A. and Zhang, M. and Hy, S. and Cela, D. and Fang, C. and Wynn, T. A. and Qiu, B. and Xia, Y. and Liu, Z. and Ulvestad, A. and Hua, N. and Wingert, J. and Liu, H. and Sprung, M. and Zozulya, A. V. and Maxey, E. and Harder, R. and Meng, Y. S. and Shpyrko, O. G.},
abstractNote = {Lithium-rich layered oxides (LRLO) are among the leading candidates for the next-generation cathode material for energy storage, delivering 50% excess capacity over commercially used compounds. Despite excellent prospects, voltage fade has prevented effective use of the excess capacity, and a major challenge has been a lack of understanding of the mechanisms underpinning the voltage fade. Here, using operando three-dimensional Bragg coherent diffractive imaging, we directly observe the nucleation of a mobile dislocation network in LRLO nanoparticles. The dislocations form more readily in LRLO as compared with a classical layered oxide, suggesting a link between the defects and voltage fade. We show microscopically how the formation of partial dislocations contributes to the voltage fade. The insights allow us to design and demonstrate an effective method to recover the original high-voltage functionality. Furthermore, our findings reveal that the voltage fade in LRLO is reversible and call for new paradigms for improved design of oxygen-redox active materials.},
doi = {10.1038/s41560-018-0184-2},
journal = {Nature Energy},
number = 8,
volume = 3,
place = {United States},
year = {Mon Jul 16 00:00:00 EDT 2018},
month = {Mon Jul 16 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1038/s41560-018-0184-2
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Cited by: 231 works
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Figures / Tables:

Figure 1 Figure 1: Formation of a dislocation network during charge. Isosurface rendering of a LRLO particle measured in operando during charge. (a) At a charge state of 4.0 V vs Li+ no dislocations are observed in the particle. The inset shows XXX (b) At 4.3 V two edge dislocations have formedmore » during lithium extraction (shown by small spheres in the particle). The inset shows XXX (c) At 4.4 V a dislocation network emerges (colors are used to represent different dislocations). The direction of the scattering vector q003 is indicated and the size of the particle is around 300x300x500 nm3. The dislocations have a component of the Burgers vector along the q003 vector and a schematic of the dislocation is shown at the bottom.« less
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