A Phase-Field Model Coupled with Large Elasto-Plastic Deformation: Application to Lithiated Silicon Electrodes

A phase-field model, accounting for large elasto-plastic deformation, is developed to study the evolution of phase, morphology and stress in crystalline silicon (Si) electrodes upon lithium (Li) insertion. The Li concentration profiles and deformation geometries are co-evolved by solving a set of coupled phase-field and mechanics equations using the finite element method. The present phase-field model is validated in comparison with a non-linear concentration-dependent diffusion model of lithiation in Si electrodes. It is shown that as the lithiation proceeds, the hoop stress changes from the initial compression to tension in the surface layer of the Si electrode, which may explain the surface cracking observed in experiments. The present phase-field model is generally applicable to high-capacity electrode systems undergoing both phase change and large elasto-plastic deformation. (C) The Author(s) 2014. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution Non-Commercial No Derivativeg 4.0 License (CC BY-NC-ND, http://creativecommons.org/licenses/by-nc-nd/4.0/), which permits non-commercial reuse, distribution, and reproduction in any medium, provided the original work is not changed in any way and is properly cited. For permission for commercial reuse, please email: oa@electrochem.org. All rights reserved.