Phase-field simulations of lithium dendrite growth with open-source software

TL;DR

This paper presents a phase-field model implemented in open-source software to simulate lithium dendrite growth, revealing how morphology depends on electrochemical conditions and enabling broader research in lithium metal electrodes.

Contribution

We developed a grand potential based nonlinear phase-field model using open-source software to study lithium dendrite growth, making the methodology accessible for future research.

Findings

Dendrite growth patterns vary with overpotential.

Ion transport and reactions dynamically compete affecting morphology.

Open-source implementation facilitates wider adoption and study.

Abstract

Dendrite growth is a long-standing challenge that has limited the applications of rechargeable lithium metal electrodes. Here, we developed a grand potential based nonlinear phase-field model to study the electrodeposition of lithium as relevant for a lithium metal anode, using open-source software package MOOSE. The dynamic morphological evolution under large/small overpotential is studied in 2-dimensions, revealing important dendrite growth/stable deposition patterns. The corresponding temporal-spatial distributions of ion concentration, overpotential and driving force are studied, which demonstrate an intimate, dynamic competition between ion transport and electrochemical reactions, resulting in vastly different growth patterns. Given the importance of morphological evolution for lithium metal electrodes, wide-spread applications of phase-field models have been limited in part due to in-house or proprietary software. In order to spur growth of this field, we utilize an open-source software package and make all files available to enable future studies to study the many unsolved aspects related to morphology evolution for lithium metal electrodes.