Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content
Abstract
Ni-rich LiNi1–x–yMnxCoyO2 (NMC) materials are attractive as cathodes for Li-ion batteries due to their high energy density and low Co content. However, these materials may display poor electrochemical reversibility relating to structural and interfacial instabilities. The influence of Ni content and level of delithiation during charge on degradation mechanisms and relevance to electrochemical cycling behavior are probed for LiNi0.6Mn0.2Co0.2O2 (NMC622) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode materials in a full cell configuration under two upper voltage limits (4.1 and 4.3 V). The combined use of dQ/dV analysis of electrochemical voltage profiles, operando XRD, and postcycling scanning electron microscopy (SEM) measurements indicates that a major contributor to capacity fade is the large anisotropic volume change from an H2 $$\leftrightarrows$$ H3 phase transition and associated mechanical degradation particularly for NMC811. Notably, transition metal dissolution and deposition on the negative electrode are found to correlate with the structural changes occurring in the cathode under high voltage charge. X-ray photoelectron spectroscopy (XPS) analyses of the cycled cathodes reveal a more organic-rich cathode–electrolyte interphase (CEI) when cycling to 4.3 V with lower relative amounts of LiF. Surface reconstruction is not a significant factor under these cycling conditions as determined by soft X-ray absorption spectroscopy (sXAS) analysis. The results emphasize the opportunity to match the electrochemical test parameters with the specific NMC active material to mitigate degradation and extend cycle life.
- Authors:
-
[5];
[5];
[5];
[5]
- State Univ. of New York (SUNY), Stony Brook, NY (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
- Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- State Univ. of New York (SUNY), Stony Brook, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2m#S); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Mercedes-Benz Research and Development North America; New York State Energy Research and Development Authority (NYSERDA); New York State Department of Economic Development (DED)
- OSTI Identifier:
- 1984421
- Report Number(s):
- BNL-224470-2023-JAAM
Journal ID: ISSN 1932-7447
- Grant/Contract Number:
- SC0012704; SC0012673; 75039; 76890
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 127; Journal Issue: 15; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electrochemical cells; Electrodes; Materials; Phase transitions; Transition metals
Citation Formats
West, Patrick J., Quilty, Calvin D., Wang, Zhongling, Ehrlich, Steven N., Ma, Lu, Jaye, Cherno, Fischer, Daniel A., Tong, Xiao, Kiss, Andrew M., Takeuchi, Esther S., Marschilok, Amy C., Takeuchi, Kenneth J., and Bock, David C. Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content. United States: N. p., 2023.
Web. doi:10.1021/acs.jpcc.2c08971.
West, Patrick J., Quilty, Calvin D., Wang, Zhongling, Ehrlich, Steven N., Ma, Lu, Jaye, Cherno, Fischer, Daniel A., Tong, Xiao, Kiss, Andrew M., Takeuchi, Esther S., Marschilok, Amy C., Takeuchi, Kenneth J., & Bock, David C. Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content. United States. https://doi.org/10.1021/acs.jpcc.2c08971
West, Patrick J., Quilty, Calvin D., Wang, Zhongling, Ehrlich, Steven N., Ma, Lu, Jaye, Cherno, Fischer, Daniel A., Tong, Xiao, Kiss, Andrew M., Takeuchi, Esther S., Marschilok, Amy C., Takeuchi, Kenneth J., and Bock, David C. Thu .
"Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content". United States. https://doi.org/10.1021/acs.jpcc.2c08971. https://www.osti.gov/servlets/purl/1984421.
@article{osti_1984421,
title = {Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content},
author = {West, Patrick J. and Quilty, Calvin D. and Wang, Zhongling and Ehrlich, Steven N. and Ma, Lu and Jaye, Cherno and Fischer, Daniel A. and Tong, Xiao and Kiss, Andrew M. and Takeuchi, Esther S. and Marschilok, Amy C. and Takeuchi, Kenneth J. and Bock, David C.},
abstractNote = {Ni-rich LiNi1–x–yMnxCoyO2 (NMC) materials are attractive as cathodes for Li-ion batteries due to their high energy density and low Co content. However, these materials may display poor electrochemical reversibility relating to structural and interfacial instabilities. The influence of Ni content and level of delithiation during charge on degradation mechanisms and relevance to electrochemical cycling behavior are probed for LiNi0.6Mn0.2Co0.2O2 (NMC622) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode materials in a full cell configuration under two upper voltage limits (4.1 and 4.3 V). The combined use of dQ/dV analysis of electrochemical voltage profiles, operando XRD, and postcycling scanning electron microscopy (SEM) measurements indicates that a major contributor to capacity fade is the large anisotropic volume change from an H2 $\leftrightarrows$ H3 phase transition and associated mechanical degradation particularly for NMC811. Notably, transition metal dissolution and deposition on the negative electrode are found to correlate with the structural changes occurring in the cathode under high voltage charge. X-ray photoelectron spectroscopy (XPS) analyses of the cycled cathodes reveal a more organic-rich cathode–electrolyte interphase (CEI) when cycling to 4.3 V with lower relative amounts of LiF. Surface reconstruction is not a significant factor under these cycling conditions as determined by soft X-ray absorption spectroscopy (sXAS) analysis. The results emphasize the opportunity to match the electrochemical test parameters with the specific NMC active material to mitigate degradation and extend cycle life.},
doi = {10.1021/acs.jpcc.2c08971},
journal = {Journal of Physical Chemistry. C},
number = 15,
volume = 127,
place = {United States},
year = {Thu Apr 06 00:00:00 EDT 2023},
month = {Thu Apr 06 00:00:00 EDT 2023}
}
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The Formation Mechanism of Fluorescent Metal Complexes at the Li x Ni 0.5 Mn 1.5 O 4−δ /Carbonate Ester Electrolyte Interface
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Transition metal dissolution and deposition in Li-ion batteries investigated by operando X-ray absorption spectroscopy
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Mapping the Anode Surface-Electrolyte Interphase: Investigating a Life Limiting Process of Lithium Primary Batteries
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Collapse of LiNi 1– x – y Co x Mn y O 2 Lattice at Deep Charge Irrespective of Nickel Content in Lithium-Ion Batteries
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An Unavoidable Challenge for Ni-Rich Positive Electrode Materials for Lithium-Ion Batteries
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A Comparative Investigation of Single Crystal and Polycrystalline Ni‐Rich NCMs as Cathodes for Lithium‐Ion Batteries
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Formation of LiF‐rich Cathode‐Electrolyte Interphase by Electrolyte Reduction
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Enabling High-Voltage Lithium-Metal Batteries under Practical Conditions
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Research progress on the surface/interface modification of high-voltage lithium oxide cathode materials
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