Is silicon worth it? Modelling degradation in composite silicon–graphite lithium-ion battery electrodes

The addition of silicon into graphite lithium-ion battery anodes has the potential to increase cell energy density. However, understanding the complex degradation behaviour in these composite systems remains a research challenge. Here, we developed a coupled electrochemical–mechanical model of a composite silicon/graphite electrode, including stress-driven crack formation and solid electrolyte interphase layer growth for each material, validated with experimental degradation data from an LG M50T cell. The model reveals self-limiting loss of silicon due to decreasing stress in the silicon as the silicon activity shifts to a lower state-of-charge. Higher C-rates can lead to lower degradation due to lower phase utilisation as voltage cut-offs are reached earlier. Increasing silicon content can reduce the stress in the silicon by distributing reaction current density over more material. Using this model, we explored whether the extra capacity from silicon is generally 'worth' the faster degradation compared to graphite-only electrodes. The model shows if you use the silicon, you lose it, as the higher initial capacity is rapidly lost with regular high depth-of-discharge events. However, silicon does have value if it enables full graphite utilisation without range anxiety; if high depth-of-discharge events are minimised then graphite's superior longevity can be utilised while exploiting silicon's high specific capacity. The model is integrated into PyBaMM (an open-source physics-based modelling platform); providing the research community and industry with the capability to reproduce our results and further explore the dynamic lifetime behaviour of composite electrodes.