Coupled electrochemical-thermal-mechanical stress modelling in composite silicon/graphite lithium-ion battery electrodes
Author(s)
Type
Journal Article
Abstract
Silicon is often added to graphite battery electrodes to enhance the electrode-specific capacity, but it undergoes significant volume changes during (de)lithiation, which results in mechanical stress, fracture, and performance degradation. To develop long-lasting and energy-dense batteries, it is critical to understand the non-linear stress behaviour in composite silicon-graphite electrodes. In this study, we developed a coupled electrochemical-thermal-mechanical model of a composite silicon/graphite electrode in PyBaMM (an open-source physics-based modelling platform). The model is experimentally validated against a commercially available LGM50T battery, and the effects of C-rates, depth-of-discharge (DoD), and temperature are investigated. The developed model can reproduce the voltage hysteresis from the silicon and provide insights into the stress response and crack growth/propagation in the two different phases. The stress in the silicon is relatively low at low DoD but rapidly increases at a DoD >~80%, whereas the stress in the graphite increases with decreasing temperature and DoD. At higher C-rates, peak stress in the graphite increases as expected, however, this decreases for silicon due to voltage cut-offs being hit earlier, leading to lower active material utilisation since silicon is mostly active at high DoD. Therefore, this work provides an improved understanding of stress evolution in composite silicon/graphite lithium-ion batteries.
Date Issued
2023-12-01
Date Acceptance
2023-08-02
Citation
Journal of Energy Storage, 2023, 73
ISSN
2352-152X
Publisher
Elsevier BV
Journal / Book Title
Journal of Energy Storage
Volume
73
Copyright Statement
Copyright © Elsevier Ltd. All rights reserved. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0/
Identifier
http://dx.doi.org/10.1016/j.est.2023.108609
Publication Status
Published
Article Number
108609
Date Publish Online
2023-09-04