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Title: Visualizing electrode assembly movement and lithiation heterogeneity in lithium-metal batteries using operando energy dispersive X-ray diffraction

Abstract

There is renewed interest in Li-metal anodes in order to increase the energy density of battery cells. Here, we demonstrate an operando X-ray crystallography method to visualize lithiation gradients and electrode assembly movement during electrochemical cycling of a Li-metal cell containing a Ni-Mn-Co layered oxide cathode (NMC811). During charge, deposition of Li+ ions from the cathode increases the Li foil thickness; during discharge, the thickness decreases as Li+ ions are stripped off the foil. Additionally, the resulting periodic movement is observed through tracking of Bragg peaks from the ordered phases of the cathode and separator. In addition to this 3.6 μm/mAh displacement, continuous mossy Li build-up on the anode causes an irreversible drift of the assembly, which is similar to 11.3 μm/cycle. Furthermore, our data indicate significant lithiation gradients in the NMC811 cathode during the oxide relithiation, which is not observed during the delithiation.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Argonne National Laboratory (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
2217012
Alternate Identifier(s):
OSTI ID: 1896564
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Power Sources
Additional Journal Information:
Journal Volume: 553; Journal ID: ISSN 0378-7753
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; NMC811 oxide; anode expansion and contraction; cathode lithiation gradients; lithium metal; lithium plating and stripping

Citation Formats

Shkrob, Ilya A., Badami, Pavan, Okasinski, John S., Rodrigues, Marco-Tulio F., and Abraham, Daniel P. Visualizing electrode assembly movement and lithiation heterogeneity in lithium-metal batteries using operando energy dispersive X-ray diffraction. United States: N. p., 2022. Web. doi:10.1016/j.jpowsour.2022.232273.
Shkrob, Ilya A., Badami, Pavan, Okasinski, John S., Rodrigues, Marco-Tulio F., & Abraham, Daniel P. Visualizing electrode assembly movement and lithiation heterogeneity in lithium-metal batteries using operando energy dispersive X-ray diffraction. United States. https://doi.org/10.1016/j.jpowsour.2022.232273
Shkrob, Ilya A., Badami, Pavan, Okasinski, John S., Rodrigues, Marco-Tulio F., and Abraham, Daniel P. Fri . "Visualizing electrode assembly movement and lithiation heterogeneity in lithium-metal batteries using operando energy dispersive X-ray diffraction". United States. https://doi.org/10.1016/j.jpowsour.2022.232273. https://www.osti.gov/servlets/purl/2217012.
@article{osti_2217012,
title = {Visualizing electrode assembly movement and lithiation heterogeneity in lithium-metal batteries using operando energy dispersive X-ray diffraction},
author = {Shkrob, Ilya A. and Badami, Pavan and Okasinski, John S. and Rodrigues, Marco-Tulio F. and Abraham, Daniel P.},
abstractNote = {There is renewed interest in Li-metal anodes in order to increase the energy density of battery cells. Here, we demonstrate an operando X-ray crystallography method to visualize lithiation gradients and electrode assembly movement during electrochemical cycling of a Li-metal cell containing a Ni-Mn-Co layered oxide cathode (NMC811). During charge, deposition of Li+ ions from the cathode increases the Li foil thickness; during discharge, the thickness decreases as Li+ ions are stripped off the foil. Additionally, the resulting periodic movement is observed through tracking of Bragg peaks from the ordered phases of the cathode and separator. In addition to this 3.6 μm/mAh displacement, continuous mossy Li build-up on the anode causes an irreversible drift of the assembly, which is similar to 11.3 μm/cycle. Furthermore, our data indicate significant lithiation gradients in the NMC811 cathode during the oxide relithiation, which is not observed during the delithiation.},
doi = {10.1016/j.jpowsour.2022.232273},
journal = {Journal of Power Sources},
number = ,
volume = 553,
place = {United States},
year = {Fri Oct 28 00:00:00 EDT 2022},
month = {Fri Oct 28 00:00:00 EDT 2022}
}

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