A model for lithium diffusion and stress generation in an intercalation storage particle with phase change

During the cycling of a lithium-ion battery, the active storage materials experience a volume change due to the intercalation process, often causing fracture, loss of contact among the active particles, and finally the degradation of the whole electrode. Here, we present a model for the lithium diffusion and stress generation in a particle of active material having a phase change. In our approach the driving force for diffusion is deduced from basic thermodynamics and statistical physics. The parameters of our model may be obtained from experimental measurements, or from ab-initio density functional theory calculations if the values are experimentally not accessible, as in the evaluation of new, as yet unsynthesized, computer-designed materials. We present results from simulations representing graphite known to experience phase-changes or staging. In some of our simulations, the particles are coupled to a battery simulator to apply conditions experienced in a functioning cell. We find that staging causes a significant increase in particle stress in comparison to when it is absent.