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Title: Impact of Charge Voltage on Factors Influencing Capacity Fade in Layered NMC622: Multimodal X-ray and Electrochemical Characterization

Abstract

Ni-rich NMC is an attractive Li-ion battery cathode due to its combination of energy density, thermal stability, and reversibility. While higher delivered energy density can be achieved with a more positive charge voltage limit, this approach compromises sustained reversibility. Improved understanding of the local and bulk structural transformations as a function of charge voltage, and their associated impacts on capacity fade are critically needed. Through simultaneous operando synchrotron X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) of cells cycled at 3–4.3 or 3–4.7 V, this study presents an in-depth investigation into the effects of voltage window on local coordination, bulk structure, and oxidation state. These measurements are complemented by ex situ X-ray fluorescence (XRF) mapping and scanning electrochemical microscopy mapping (SECM) of the negative electrode, X-ray photoelectron spectroscopy (XPS) of the positive electrode, and cell level electrochemical impedance spectroscopy (EIS). Initially, cycling between 3 and 4.7 V leads to greater delivered capacity due to greater lithium extraction, accompanied by increased structural distortion, moderately higher Ni oxidation, and substantially higher Co oxidation. Continued cycling at this high voltage results in suppressed Ni and Co redox, greater structural distortion, increased levels of transition metal dissolution, higher cell impedance, and 3× greater capacitymore » fade.« less

Authors:
 [1];  [1]; ORCiD logo [2];  [1]; ORCiD logo [1];  [1];  [1];  [3];  [4];  [4]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
+ Show Author Affiliations
  1. State Univ. of New York (SUNY), Stony Brook, NY (United States)
  2. State Univ. of New York (SUNY), Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1856776
Report Number(s):
BNL-222890-2022-JAAM
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 13; Journal Issue: 43; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Ni rich NMC; operando X-ray diffraction; operando X-ray absorption spectroscopy; capacity fading mechanisms; high potential charging

Citation Formats

Quilty, Calvin D., Wheeler, Garrett P., Wang, Lei, McCarthy, Alison H., Yan, Shan, Tallman, Killian R., Dunkin, Mikaela R., Tong, Xiao, Ehrlich, Steven, Ma, Lu, Takeuchi, Kenneth J., Takeuchi, Esther S., Bock, David C., and Marschilok, Amy C. Impact of Charge Voltage on Factors Influencing Capacity Fade in Layered NMC622: Multimodal X-ray and Electrochemical Characterization. United States: N. p., 2021. Web. doi:10.1021/acsami.1c14272.
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Quilty, Calvin D., Wheeler, Garrett P., Wang, Lei, McCarthy, Alison H., Yan, Shan, Tallman, Killian R., Dunkin, Mikaela R., Tong, Xiao, Ehrlich, Steven, Ma, Lu, Takeuchi, Kenneth J., Takeuchi, Esther S., Bock, David C., & Marschilok, Amy C. Impact of Charge Voltage on Factors Influencing Capacity Fade in Layered NMC622: Multimodal X-ray and Electrochemical Characterization. United States. https://doi.org/10.1021/acsami.1c14272
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Quilty, Calvin D., Wheeler, Garrett P., Wang, Lei, McCarthy, Alison H., Yan, Shan, Tallman, Killian R., Dunkin, Mikaela R., Tong, Xiao, Ehrlich, Steven, Ma, Lu, Takeuchi, Kenneth J., Takeuchi, Esther S., Bock, David C., and Marschilok, Amy C. Mon . "Impact of Charge Voltage on Factors Influencing Capacity Fade in Layered NMC622: Multimodal X-ray and Electrochemical Characterization". United States. https://doi.org/10.1021/acsami.1c14272. https://www.osti.gov/servlets/purl/1856776.
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@article{osti_1856776,
title = {Impact of Charge Voltage on Factors Influencing Capacity Fade in Layered NMC622: Multimodal X-ray and Electrochemical Characterization},
author = {Quilty, Calvin D. and Wheeler, Garrett P. and Wang, Lei and McCarthy, Alison H. and Yan, Shan and Tallman, Killian R. and Dunkin, Mikaela R. and Tong, Xiao and Ehrlich, Steven and Ma, Lu and Takeuchi, Kenneth J. and Takeuchi, Esther S. and Bock, David C. and Marschilok, Amy C.},
abstractNote = {Ni-rich NMC is an attractive Li-ion battery cathode due to its combination of energy density, thermal stability, and reversibility. While higher delivered energy density can be achieved with a more positive charge voltage limit, this approach compromises sustained reversibility. Improved understanding of the local and bulk structural transformations as a function of charge voltage, and their associated impacts on capacity fade are critically needed. Through simultaneous operando synchrotron X-ray diffraction (XRD) and X-ray absorption spectroscopy (XAS) of cells cycled at 3–4.3 or 3–4.7 V, this study presents an in-depth investigation into the effects of voltage window on local coordination, bulk structure, and oxidation state. These measurements are complemented by ex situ X-ray fluorescence (XRF) mapping and scanning electrochemical microscopy mapping (SECM) of the negative electrode, X-ray photoelectron spectroscopy (XPS) of the positive electrode, and cell level electrochemical impedance spectroscopy (EIS). Initially, cycling between 3 and 4.7 V leads to greater delivered capacity due to greater lithium extraction, accompanied by increased structural distortion, moderately higher Ni oxidation, and substantially higher Co oxidation. Continued cycling at this high voltage results in suppressed Ni and Co redox, greater structural distortion, increased levels of transition metal dissolution, higher cell impedance, and 3× greater capacity fade.},
doi = {10.1021/acsami.1c14272},
journal = {ACS Applied Materials and Interfaces},
number = 43,
volume = 13,
place = {United States},
year = {Mon Oct 25 00:00:00 EDT 2021},
month = {Mon Oct 25 00:00:00 EDT 2021}
}
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