Diffusion-induced stress amplification in phase-transition materials for electrodes of lithium-ion batteries

This work sheds the light on the stress amplification in active material particles of electrodes caused by the localized lithium concentration inhomogeneity due to phase transitions. This is a significant issue usually neglected in the literature, as generally the ideal Fickian diffusion model is used to describe the lithium diffusion, which particularly fails when dealing with phase change materials, resulting in the underestimation of the stress. In turn, this results in the underestimation of the fracture behavior of the electrode and the battery degradation, ultimately. To overcome these limitations, this work proposes a mechanical-transport model where the lithium transport is modeled according to the non-ideal solution theory with an equivalent diffusion coefficient depending on the potential of the host material vs Li/Li+. / Li + . The results show that the proposed model correctly describes the concentration distribution within the particle of phase-change materials (graphite is chosen as a case study), in agreement with the existent experimental measurements. The differences with respect to the traditional Fickian diffusion model is substantial as the stress is up to 85% higher with the proposed model and the concentration distribution can capture the inhomogeneity caused by phase transitions.