Unified Picture on Temperature Dependence of Lithium Dendrite Growth via Phase-Field Simulation

Abstract

Lithium dendrite growth due to uneven electrodeposition may penetrate the separator and solid electrolyte, causing inner short circuit and potential thermal runaway. Despite great electrochemical phase-field simulation efforts devoted to exploring the dendrite growth mechanism under the temperature field, no unified picture has emerged. For example, it remains open how to understand the promotion, inhibition, and dual effects of increased temperature on dendrite growth when using different electrolyte types. Here, by comprehensively considering the temperature-dependent Li + diffusion coefficient, electrochemical reaction coefficient, and initial temperature distribution in phase-field model, we propose that the activation–energy ratio, defined as the ratio of electrochemical reaction activation energy to electrolyte Li + diffusion activation energy, can be used to quantify the effect of temperature on dendrite morphology. Specifically, we establish a mechanism diagram correlating the activation–energy ratio, uniform initial temperature, and maximum dendrite height, which unifies the seemingly contradictory simulation results. Furthermore, results based on nonuniform initial temperature distribution indicate that a positive temperature gradient along the discharging current facilitates uniform Li + deposition and local hotspot should be avoided. These findings provide valuable insights into the temperature-dependent Li dendrite growth and contribute to the practical application of Li metal batteries.