Chemo-mechanical study of dislocation mediated ion diffusion in lithium-ion battery materials

Authors: Christoph Reimuth, Binbin Lin, Yangyiwei Yang, Peter Stein, Xiandong Zhou and Bai-Xiang Xu

A mechanically coupled diffusion model combined with finite element formulation is developed to study the influence of dislocations on ion diffusion in lithium-ion batteries. The dislocation is modeled by the regularized eigenstrain based on a non-singular continuum dislocation theory. The model is validated with the analytical solution of the stress field of edge dislocations and the solution for the stress-dependent equilibrium concentration around the dislocation. Simulation results on LiMn2O4 demonstrate strong ion enrichment and depletion on the tensile and compressive sides of an edge dislocation, respectively. A stronger influence of the edge dislocation on diffusion is found at a lower state-of-charge, which verifies the experimental observation reported in the literature. The diffusion-induced stress compensates partially the stress field of the edge dislocation and is ascertained to have a state-of-charge dependency. The existence of dislocation does not introduce obvious mobility anisotropy in the bulk material but it results in local mobility heterogeneity around the dislocation. A three-dimensional simulation of the diffusion along the edge dislocation line reveals that the pipe diffusion can be initiated or accelerated on the tensile side of the edge dislocation.

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