Degradation in Ni-Rich LiNi1–x–yMnxCoyO2/Graphite Batteries: Impact of Charge Voltage and Ni Content

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.

doi:10.1021/acs.jpcc.2c08971

Title: Degradation in Ni-Rich LiNi_1–x–yMn_xCo_yO₂/Graphite Batteries: Impact of Charge Voltage and Ni Content

Journal Article · Thu Apr 06 00:00:00 EDT 2023 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.2c08971· OSTI ID:1984421

West, Patrick J. ^[1]; Quilty, Calvin D. ^[1]; Wang, Zhongling ^[1]; Ehrlich, Steven N. ^[2]; Ma, Lu ^[2]; Jaye, Cherno ^[3]; Fischer, Daniel A. ^[3]; Tong, Xiao ^[4]; Kiss, Andrew M. ^[2];

^[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)

Ni-rich LiNi_1–x–yMn_xCoyO₂ (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 LiNi_0.6Mn_0.2Co_0.2O₂ (NMC622) and LiNi_0.8Mn_0.1Co_0.1O₂ (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.

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Research Organization:: 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 Organization:: 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)

Grant/Contract Number:: SC0012704; SC0012673; 75039; 76890

OSTI ID:: 1984421

Report Number(s):: BNL-224470-2023-JAAM

Journal Information:: Journal of Physical Chemistry. C, Vol. 127, Issue 15; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Degradation in Ni-Rich LiNi_1–x–yMn_xCo_yO₂/Graphite Batteries: Impact of Charge Voltage and Ni Content