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Title: The influence of electrochemical cycling protocols on capacity loss in nickel-rich lithium-ion batteries

Abstract

The transition towards electric vehicles and more sustainable transportation is dependent on lithium-ion battery (LIB) performance. Ni-rich layered transition metal oxides, such as NMC811 (LiNi0.8Mn0.1Co0.1O2), are promising cathode candidates for LIBs due to their higher specific capacity and lower cost compared with lower Ni content materials. However, complex degradation mechanisms inhibit their use. In this work, tailored aging protocols are employed to decouple the effect of electrochemical stimuli on the degradation mechanisms in graphite/NMC811 full cells. Using these protocols, impedance measurements, and differential voltage analysis, the primary drivers for capacity fade and impedance rise are shown to be large state of charge changes combined with high upper cut-off voltage. Focused ion beam-scanning electron microscopy highlights that extensive microscale NMC particle cracking, caused by electrode manufacturing and calendering, is present prior to aging and not immediately detrimental to the gravimetric capacity and impedance. Scanning transmission electron microscopy electron energy loss spectroscopy reveals a correlation between impedance rise and the level of transition metal reduction at the surfaces of aged NMC811. The present study provides insight into the leading causes for LIB performance fading, and highlights the defining role played by the evolving properties of the cathode particle surface layer.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. University of Cambridge (United Kingdom); The Faraday Institution, Didcot (United Kingdom)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States). Cell Analysis, Modeling and Prototyping (CAMP) Facility
Sponsoring Org.:
USDOE
OSTI Identifier:
1982223
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 9; Journal Issue: 41; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Energy & Fuels; Materials Science

Citation Formats

Dose, Wesley M., Morzy, Jędrzej K., Mahadevegowda, Amoghavarsha, Ducati, Caterina, Grey, Clare P., and De Volder, Michael F. L. The influence of electrochemical cycling protocols on capacity loss in nickel-rich lithium-ion batteries. United States: N. p., 2021. Web. doi:10.1039/d1ta06324c.
Dose, Wesley M., Morzy, Jędrzej K., Mahadevegowda, Amoghavarsha, Ducati, Caterina, Grey, Clare P., & De Volder, Michael F. L. The influence of electrochemical cycling protocols on capacity loss in nickel-rich lithium-ion batteries. United States. https://doi.org/10.1039/d1ta06324c
Dose, Wesley M., Morzy, Jędrzej K., Mahadevegowda, Amoghavarsha, Ducati, Caterina, Grey, Clare P., and De Volder, Michael F. L. Mon . "The influence of electrochemical cycling protocols on capacity loss in nickel-rich lithium-ion batteries". United States. https://doi.org/10.1039/d1ta06324c. https://www.osti.gov/servlets/purl/1982223.
@article{osti_1982223,
title = {The influence of electrochemical cycling protocols on capacity loss in nickel-rich lithium-ion batteries},
author = {Dose, Wesley M. and Morzy, Jędrzej K. and Mahadevegowda, Amoghavarsha and Ducati, Caterina and Grey, Clare P. and De Volder, Michael F. L.},
abstractNote = {The transition towards electric vehicles and more sustainable transportation is dependent on lithium-ion battery (LIB) performance. Ni-rich layered transition metal oxides, such as NMC811 (LiNi0.8Mn0.1Co0.1O2), are promising cathode candidates for LIBs due to their higher specific capacity and lower cost compared with lower Ni content materials. However, complex degradation mechanisms inhibit their use. In this work, tailored aging protocols are employed to decouple the effect of electrochemical stimuli on the degradation mechanisms in graphite/NMC811 full cells. Using these protocols, impedance measurements, and differential voltage analysis, the primary drivers for capacity fade and impedance rise are shown to be large state of charge changes combined with high upper cut-off voltage. Focused ion beam-scanning electron microscopy highlights that extensive microscale NMC particle cracking, caused by electrode manufacturing and calendering, is present prior to aging and not immediately detrimental to the gravimetric capacity and impedance. Scanning transmission electron microscopy electron energy loss spectroscopy reveals a correlation between impedance rise and the level of transition metal reduction at the surfaces of aged NMC811. The present study provides insight into the leading causes for LIB performance fading, and highlights the defining role played by the evolving properties of the cathode particle surface layer.},
doi = {10.1039/d1ta06324c},
journal = {Journal of Materials Chemistry. A},
number = 41,
volume = 9,
place = {United States},
year = {Mon Oct 11 00:00:00 EDT 2021},
month = {Mon Oct 11 00:00:00 EDT 2021}
}

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