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

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.

doi:10.1038/s41560-018-0184-2

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

Journal Article · Mon Jul 16 00:00:00 EDT 2018 · Nature Energy

DOI:https://doi.org/10.1038/s41560-018-0184-2· OSTI ID:1770701

Singer, A. ^[1]; Zhang, M. ^[2]; Hy, S. ^[2]; Cela, D. ^[2]; Fang, C. ^[2]; Wynn, T. A. ^[2];

^[3]; Xia, Y. ^[3]; Liu, Z. ^[3]; Ulvestad, A. ^[4]; Hua, N. ^[2]; Wingert, J. ^[2]; Liu, H. ^[2]; Sprung, M. ^[5]; Zozulya, A. V. ^[6]; Maxey, E. ^[7]; Harder, R. ^[7]; Meng, Y. S. ^[2]; Shpyrko, O. G. ^[2]

Univ. of California-San Diego, La Jolla, CA (United States); Cornell Univ., Ithaca, NY (United States)
Univ. of California-San Diego, La Jolla, CA (United States)
Chinese Academy of Sciences, Zhejiang (China)
Argonne National Lab. (ANL), Argonne, IL (United States)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European XFEL GmbH, Schenefeld (Germany)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

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.

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Research Organization:: Univ. of California, San Diego, CA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: EE0007744; AC02-06CH11357; SC0001805; SC0012583

OSTI ID:: 1770701

Alternate ID(s):: OSTI ID: 1481914

Journal Information:: Nature Energy, Vol. 3, Issue 8; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 231 works

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