DataVXACS Energy LettersPaper
journal article·2023-12-08Open access

Synergistic Degradation Mechanism in Single Crystal Ni-Rich NMC//Graphite Cells

Galo J. Páez Fajardo, Eleni Fiamegkou, James A. Gott, Heng Wang, Israel Temprano, Ieuan D. Seymour, Matthew J. W. Ogley, Ashok S. Menon, Ifan E. L. Stephens, Muhammad Ans, Tien-Lin Lee, Pardeep K. Thakur, Wesley M. Dose, Michaël F. L. De Volder, Clare P. Grey, Louis F. J. Piper

ACS Energy Letters· Volume 8· Issue 12
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Abstract

High Resolution Image Download MS PowerPoint Slide Oxygen loss at high voltages in Ni-rich NMC//graphite Li-ion batteries promotes degradation, but increasing evidence from full cells reveals that the depth of discharge choice can further accelerate aging, i.e., synergistic degradation. In this Letter, we employ cycling protocols to examine the origin of the synergistic degradation for single crystal Ni-rich NMC//graphite pouch cells. In regimes where oxygen loss is not promoted ( V < 4.3 V), a lower cutoff voltage does not affect capacity retention (after 100 cycles), despite significant graphite expansion occurring. In contrast, when NMC surface oxygen loss is induced ( V > 4.3 V), deeper depth of discharge leads to pronounced faster aging. Using a combination of post-mortem analysis and density functional theory, we present a mechanistic description of surface phase densification and evolution as a function of voltage and cycling. The detrimental impact of this mechanism on lithium-ion kinetics is used to explain the observed cycling results.
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Research context

Energy storage

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Technologies Research · Advanced Battery Materials and Technologies

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

WMG, University of Warwick, Coventry CV4 7AL, United Kingdom

The Faraday Institution, Quad One, Harwell Science and Innovation Campus, Didcot OX11 0RA, United Kingdom

Department of Engineering, Institute for Manufacturing, University of Cambridge, 17 Charles Babbage Road, Cambridge CB3 0FS, United Kingdom

Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge CB2 1EW, United Kingdom

Department of Chemistry, University of Aberdeen, Aberdeen AB24 3UE, United Kingdom

Department of Materials, Imperial College London, London SW7 2AZ, United Kingdom

Advanced Centre for Energy and Sustainability (ACES), Department of Chemistry, University of Aberdeen, Aberdeen AB24 3UE, Scotland, United Kingdom

Diamond Light Source, Didcot OX11 0DE, United Kingdom

School of Chemistry, The University of New South Wales, Sydney, NSW 2052, Australia

Funding

Faraday Institution

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