Issue 9, 2021

Quantification of heterogeneous, irreversible lithium plating in extreme fast charging of lithium-ion batteries

Abstract

Realization of extreme fast charging (XFC, ≤15 minutes) of lithium-ion batteries is imperative for the widespread adoption of electric vehicles. However, dramatic capacity fading is associated with XFC, limiting its implementation. To quantitatively elucidate the effects of irreversible lithium plating and other degradation mechanisms on the cell capacity, it is important to understand the links between lithium plating and cell degradation at both the local and global (over the full cell) scales. Here, we study the nature of local lithium plating after hundreds of XFC cycles (charging C-rates ranging from 4C to 9C) in industrially-relevant pouch cells using spatially resolved X-ray diffraction. Our results reveal a spatial correlation at the mm scale between irreversible lithium plating on the anode, inactive lithiated graphite phases, and local state-of-charge of the cathode. In regions of plated lithium, additional lithium is locally and irreversibly trapped as lithiated graphite, contributing to the loss of lithium inventory (LLI) and to a local loss of active anode material. The total LLI in the cell from irreversibly plated lithium is linearly correlated to the capacity loss in the batteries after XFC cycling, with a non-zero offset originating from other parasitic side reactions. Finally, at the global (cell) scale, LLI drives the capacity fade, rather than electrode degradation. We anticipate that the understanding of lithium plating and other degradation mechanisms during XFC gained in this work will help lead to new approaches towards designing high-rate batteries in which irreversible lithium plating is minimized.

Graphical abstract: Quantification of heterogeneous, irreversible lithium plating in extreme fast charging of lithium-ion batteries

Associated articles

Supplementary files

Article information

Article type
Paper
Submitted
23 Apr 2021
Accepted
29 Jul 2021
First published
30 Jul 2021

Energy Environ. Sci., 2021,14, 4979-4988

Quantification of heterogeneous, irreversible lithium plating in extreme fast charging of lithium-ion batteries

P. P. Paul, V. Thampy, C. Cao, H. Steinrück, T. R. Tanim, A. R. Dunlop, E. J. Dufek, S. E. Trask, A. N. Jansen, M. F. Toney and J. Nelson Weker, Energy Environ. Sci., 2021, 14, 4979 DOI: 10.1039/D1EE01216A

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