Phase-Field Modeling of Electrolyte Transport Properties and Elasticity Modulus in Suppression of Dendrite Growth in Solid-State-Lithium-Ion-Batteries

Abstract

Dendrite formation in batteries is a critical issue that affects battery performance and lifespan. Solid-state electrolytes have gained attention due to their advantages such as compactness, higher energy density, and enhanced safety. This study investigates dendrite growth in batteries via phase field simulations utilizing a grand potential-based phase field model. The simulations are executed using the MOOSE (Multiphysics Object-Oriented Simulation Environment) framework, a Finite Element Method (FEM) based solver known for its modular approach and proficiency in handling complex multi-physics problems. Initially, the study considers a pure lithium anode and a 1M LiPF6 electrolyte for the liquid case. To explore the benefits of solid electrolytes, a fictitious solid electrolyte with transport properties similar to the liquid electrolyte but having different mechanical properties is considered. The mechanical impact resulting from the volume changes due to lithium deposition is not accounted for in the liquid electrolyte model. However, the solid electrolyte model addresses this by modifying the Butler-Volmer kinetics and incorporating the influence of stresses on the localized lithium deposition. Sensitivity analysis is performed for various parameters in both the liquid and solid electrolytes. The results indicate that dendrite growth is reduced with decreased applied over-potential and interfacial energies. For solid electrolytes, an additional parameter, increased Young’s modulus, contributes to reduced dendrite growth. The evaluation of dendrite growth involves quantifying surface roughness using the root mean square (RMS) approach. The elasticity modulus significantly influences dendrite formation, with higher values in materials like LLZO, and glass Li3PS4 exhibiting lower dendrite growth, while lower values in polymer-based materials like P(VDF-HFP) and PVDF/CAB/PE exhibit higher dendrite growth. The solid electrolyte acts as a crucial mechanical barrier, influencing the dendrite tip growth rate and ensuring uniform electrodeposition throughout the dendritic structure. Furthermore, the work investigates the impact of the cathode on dendrite growth. The contraction of the cathode provides additional space for dendrites to move, leading to reduced compressive stresses and increased dendrite growth. Conversely, higher compressive stresses suppress dendrite growth.