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Quantifying electrochemical degradation in single-crystalline LiNi0.8Mn0.1Co0.1O2–graphite pouch cells through operando X-ray and post-mortem investigations
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Menon, Ashok S., Shah, Nickil, Gott, James A., Fiamegkou, Eleni, Ogley, Matthew J. W., Paez Fajardo, Galo J., Vaenas, Naoum, Ellis, Ieuan, Ravichandran, Nishitha, Cloetens, Peter, Karpov, Dmitry, Warnett, Jay, Malliband, Paul, Walker, David, West, Geoffrey D., Loveridge, Melanie and Piper, Louis F. J. (2023) Quantifying electrochemical degradation in single-crystalline LiNi0.8Mn0.1Co0.1O2–graphite pouch cells through operando X-ray and post-mortem investigations. Working Paper. ChemRxiv.
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WRAP-quantifying-electrochemical-degradation-in-single-crystalline-li-ni0-8mn0-1co0-1o2-graphite-pouch-cells-through-operando-x-ray-and-post-mortem-investigations-2023.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution Non-commercial No Derivatives 4.0. Download (2626Kb) | Preview |
Official URL: http://dx.doi.org/10.26434/chemrxiv-2023-zs9kp-v2
Abstract
Layered nickel-rich lithium transition metal oxides (LiNixMnyCo1−x−yO2; where x ≥ 0.8), with single-crystalline morphology, are promising future high-energy-density Li-ion battery cathodes due to their ability to mitigate particle-cracking-induced degradation. This is due to the absence of grain boundaries in these materials, which prevents the build-up of bulk crystallographic strain during electrochemical cycling. Compared to their polycrystalline counterparts, there is a need to study single-crystalline Ni-rich cathodes using operando X-ray methods in uncompromised machine-manufactured industry-like full cells to understand their bulk degradation mechanisms as a function of different electrochemical cycling protocols. This can help us identify factors to improve their long-term performance. Here, through in-house operando X-ray studies of pilot-line-built LiNi0.8Mn0.1Co0.1O2–Graphite A7 pouch cells, it is shown that their electrochemical capacity fade under harsh conditions (2.5–4.4 V and 40 °C for 100 cycles at C/3 rate) primarily stems from the high-voltage reconstruction of the cathode surface from a layered to a cubic (rock salt) phase that impedes Li+ kinetics and increases cell impedance. Post-mortem electron and X-ray microscopy show that these cathodes can withstand severe anisotropic structural changes and show no cracking when cycled under such conditions. Comparing these results to those from commercial Li-ion cells with surface-modified single-crystalline Ni-rich cathodes, it is identified that cathode surface passivation can mitigate this type of degradation and prolong cycle life. In addition to furthering our understanding of degradation in single-crystalline Ni-rich cathodes, this work also accentuates the need for practically relevant and reproducible fundamental investigations of Li-ion cells and presents a methodology for achieving this.
Item Type: | Working or Discussion Paper (Working Paper) | |||||||||||||||
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Subjects: | Q Science > QD Chemistry T Technology > TK Electrical engineering. Electronics Nuclear engineering |
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Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics Faculty of Science, Engineering and Medicine > Engineering > WMG (Formerly the Warwick Manufacturing Group) |
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Library of Congress Subject Headings (LCSH): | Lithium ion batteries, Cathodes, Metallic oxides | |||||||||||||||
Publisher: | ChemRxiv | |||||||||||||||
Official Date: | 7 December 2023 | |||||||||||||||
Dates: |
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DOI: | 10.26434/chemrxiv-2023-zs9kp-v2 | |||||||||||||||
Institution: | University of Warwick | |||||||||||||||
Status: | Not Peer Reviewed | |||||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | |||||||||||||||
Date of first compliant deposit: | 1 February 2024 | |||||||||||||||
Date of first compliant Open Access: | 1 February 2024 | |||||||||||||||
RIOXX Funder/Project Grant: |
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