Journal
JOURNAL OF ENERGY STORAGE
Volume 73, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.est.2023.108609
Keywords
Composite negative electrodes; Silicon/graphite; Stress generation; Particle cracking; Lithium-ion battery; Physics-based model
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In this study, a coupled electrochemical-thermal-mechanical model of composite silicon/graphite electrodes in lithium-ion batteries was developed using an open-source physics-based modelling platform. The model was experimentally validated and the effects of C-rates, depth-of-discharge, and temperature on the stress behavior were investigated. The study provides valuable insights into the stress evolution in composite electrodes, which is crucial for improving the performance and stability of batteries.
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 >similar to 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.
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