Stress-Induced Uphill Diffusion with Interfacial Contact Loss in Solid-State Electrodes

We simulate the mechanical-chemical coupling during delithiation and relaxation of a cathode in a solid-state lithium-ion battery. Contact loss at the interface between the active particle and the solid electrolyte is considered. Uphill diffusion is observed during delithiation and relaxation. This phenomenon is explained by analyzing the total chemical potential and its two components. Contact loss at the interface greatly influences the stress and stress gradient in the active particle. As delithiation continues, the stress and stress gradient grow considerably, and the mechanical part of the total chemical potential becomes dominant over the chemical part of it. In the latter stage of delithiation, the influence of the incomplete interfacial constraint on the stress becomes dominant, while the effect of the concentration gradient becomes negligible. After relaxation, the concentration and stress gradients increase in a particle with contact loss. The influence of the degree of contact loss on the mechanical-chemical coupling is investigated. The overall tensile stress in the active particle increases with decreasing contact loss, causing a sharp decrease in local concentration. We also check the effect of the elastic modulus of the solid electrolyte on the coupling of the active material. A rigid solid electrolyte with a higher elastic modulus more strongly restricts the active particle, leading to a higher tensile stress, a larger stress gradient, and a greater concentration gradient.

Automated summary

The influence of contact loss at the interface on the stress and stress gradient in the active particle during delithiation and relaxation is significant, affecting the mechanical-chemical coupling. In the later stage of delithiation, stress is mainly affected by incomplete interfacial constraint, while the effect of concentration gradient becomes negligible.