Phase-Field Simulations of Lithium Dendrite Growth with Open-Source Software

Dendrite growth is
a long-standing challenge that has limited the
applications of rechargeable lithium metal electrodes. Here, we have
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 a large/small overpotential is studied in two 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. On the basis
of the understanding from this model, we propose a “compositionally
graded electrolyte” with higher local ion concentration as
a way to potentially suppress dendrite formation. Given the importance
of morphological evolution for lithium metal electrodes, widespread
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 make all files available to enable future studies to study
the many unsolved aspects related to morphology evolution of lithium
metal electrodes.