Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy
Abstract
Ni-rich NMC materials are a particularly promising class of Li-ion cathodes for various applications. LiNi0.6Mn0.2Co0.2O2 (NMC622) offers a unique balance of thermal stability and energy density, thus attracting attention for electric vehicle implementation. However, upon extended cycling, capacity fade is prevalent due to structural degradation, which is a major drawback for layered oxide cathodes. Therefore, exploring the underlying phenomena that drive detrimental structural response can lead to future improvements. For the first time, operando X-ray absorption spectroscopy (XAS) was performed on NMC622 pouch cells at three different stages. An extensive description of the first cycle (de)lithiation mechanisms was achieved through X-ray absorption near-edge structure analyses and extended X-ray absorption fine structure modeling. Transition metal specific electrochemical participation and structural variation revealed that much of the delivered capacity and distortion is a result of Ni redox behavior, while the local structure of Co and Mn are impacted due to their interdependencies. Key mechanistic components were identified, as the local structural variation from redox processes and Ni3+ Jahn–Teller distortion were decoupled. Further, operando XAS was used to investigate the structural response of NMC622 to extended cycling and was supported by X-ray diffraction, X-ray photoelectron spectroscopy, and electrochemical impedance spectroscopy analyses. In thismore »
- Authors:
-
- Stony Brook Univ., NY (United States)
- Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II) and Center for Functional Nanomaterials (CFN); Energy Frontier Research Centers (EFRC) (United States). Center for Mesoscale Transport Properties (m2m)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Mercedes-Benz Research and Development North America (MBRDNA); New York State Energy Research and Development Authority (NYSERDA); New York State Department of Economic Development (DED)
- OSTI Identifier:
- 1772730
- Report Number(s):
- BNL-221150-2021-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: 125; Journal Issue: 1; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; NMC622; operando; X-ray absorption spectroscopy; Jahn-Teller distortion
Citation Formats
Tallman, Killian R., Wheeler, Garrett P., Kern, Christopher J., Stavitski, Eli, Tong, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Bock, David C., and Takeuchi, Esther S. Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy. United States: N. p., 2020.
Web. doi:10.1021/acs.jpcc.0c08095.
Tallman, Killian R., Wheeler, Garrett P., Kern, Christopher J., Stavitski, Eli, Tong, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Bock, David C., & Takeuchi, Esther S. Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy. United States. https://doi.org/10.1021/acs.jpcc.0c08095
Tallman, Killian R., Wheeler, Garrett P., Kern, Christopher J., Stavitski, Eli, Tong, Xiao, Takeuchi, Kenneth J., Marschilok, Amy C., Bock, David C., and Takeuchi, Esther S. Fri .
"Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy". United States. https://doi.org/10.1021/acs.jpcc.0c08095. https://www.osti.gov/servlets/purl/1772730.
@article{osti_1772730,
title = {Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy},
author = {Tallman, Killian R. and Wheeler, Garrett P. and Kern, Christopher J. and Stavitski, Eli and Tong, Xiao and Takeuchi, Kenneth J. and Marschilok, Amy C. and Bock, David C. and Takeuchi, Esther S.},
abstractNote = {Ni-rich NMC materials are a particularly promising class of Li-ion cathodes for various applications. LiNi0.6Mn0.2Co0.2O2 (NMC622) offers a unique balance of thermal stability and energy density, thus attracting attention for electric vehicle implementation. However, upon extended cycling, capacity fade is prevalent due to structural degradation, which is a major drawback for layered oxide cathodes. Therefore, exploring the underlying phenomena that drive detrimental structural response can lead to future improvements. For the first time, operando X-ray absorption spectroscopy (XAS) was performed on NMC622 pouch cells at three different stages. An extensive description of the first cycle (de)lithiation mechanisms was achieved through X-ray absorption near-edge structure analyses and extended X-ray absorption fine structure modeling. Transition metal specific electrochemical participation and structural variation revealed that much of the delivered capacity and distortion is a result of Ni redox behavior, while the local structure of Co and Mn are impacted due to their interdependencies. Key mechanistic components were identified, as the local structural variation from redox processes and Ni3+ Jahn–Teller distortion were decoupled. Further, operando XAS was used to investigate the structural response of NMC622 to extended cycling and was supported by X-ray diffraction, X-ray photoelectron spectroscopy, and electrochemical impedance spectroscopy analyses. In this work, reduced capacity was found in the cell after 100 cycles and is attributed to structural degradation and cathode–electrolyte interphase buildup from repeated Li (de)insertion processes, which limit the electrochemical reversibility of Ni and Co through increased polarization. These results expand the understanding of a Ni-rich NMC material under extended cycling, which is vital to the future design of electrode materials.},
doi = {10.1021/acs.jpcc.0c08095},
journal = {Journal of Physical Chemistry. C},
number = 1,
volume = 125,
place = {United States},
year = {Fri Dec 11 00:00:00 EST 2020},
month = {Fri Dec 11 00:00:00 EST 2020}
}
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