Activity-Modulated Localized Recrystallization during Lithium Stripping at the Electrode-Electrolyte Interface

Electrochemical stripping is a fundamental process with wide applications such as discharging of metal electrode and electropolishing. The morphological evolution of metal surface determines the cycling performance of next-generation metal-based batteries. In this work, we computationally characterize the morphological evolution dynamics at the metal-electrolyte interface with a phase-field model. We investigate both plating and stripping kinetics of the metal electrode by incorporating nonidealities of electrolyte solutions into the interfacial reaction kinetics. Intriguingly, at fast stripping, we find an unusual local recrystallization phenomenon in high concentration regions with high activity coefficients in the valley. This recrystallization provides a new approach to mitigate morphological instabilities at electrode-electrolyte interfaces.