Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy

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.

doi:10.1021/acs.jpcc.0c08095

Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy

Journal Article · Fri Dec 11 00:00:00 EST 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c08095· OSTI ID:1772730

Tallman, Killian R. ^[1]; Wheeler, Garrett P. ^[2]; Kern, Christopher J. ^[1]; Stavitski, Eli ^[3]; Tong, Xiao ^[4]; ^[1]; ^[2]; Bock, David C. ^[2]; ^[2]

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)

Ni-rich NMC materials are a particularly promising class of Li-ion cathodes for various applications. LiNi_0.6Mn_0.2Co_0.2O₂ (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.

View Accepted Manuscript (DOE)

Research Organization:: 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 Organization:: Mercedes-Benz Research and Development North America (MBRDNA); New York State Department of Economic Development (DED); New York State Energy Research and Development Authority (NYSERDA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012673; SC0012704

OSTI ID:: 1772730

Report Number(s):: BNL--221150-2021-JAAM

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 1 Vol. 125; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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