Three-dimensional experimental-scale phase-field modeling of dendrite formation in rechargeable lithium-metal batteries

Abstract

This work performs three-dimensional phase-field simulations of the electrodeposition process that forms dendrites within metal-anode batteries using an anisotropic representation of lithium crystal surface energy. The model describes the evolution of a phase field, lithium-ion concentration, and electric potential during a battery charge cycle, solving the governing equations using time-marching algorithms with automatic time-step adjustment implemented on an open-source finite element library.

A modified lithium crystal surface anisotropy representation for the phase-field electrodeposition model is proposed and evaluated through numerical tests, showing low sensitivity to numerical parameters. The experimental-scale 3D simulations capture changes in dendritic morphological behaviour through variations in simulated inter-electrode distance. Dendrite shape shifts from smoother, tree-like formations at lower applied voltage to more spike-like, highly branched structures at higher voltage. Simulations show agreement with experimentally-observed lithium dendrite growth rates and morphologies reported in the literature, with comparable morphological parameters including dendrite propagation rates, volume-specific area, and side branching rates. The work provides insight into dendrite formation as a result of competition between lithium cation diffusion and electric migration, with implications for dendrite inhibition strategies in rechargeable lithium-metal batteries.

@article{arguello2023joes,
  title         = {Three-dimensional experimental-scale phase-field modeling of dendrite formation
                  in rechargeable lithium-metal batteries},
  author        = {Arguello, Marcos E. and Labanda, Nicol\'{a}s A. and Calo, Victor M. and Gumulya,
                  Monica and Utikar, Ranjeet and Derksen, Jos},
  year          = 2023,
  month         = jun,
  journal       = {Journal of Energy Storage},
  volume        = 62,
  pages         = 106854,
  doi           = {10.1016/j.est.2023.106854},
  issn          = {2352-152x},
  url           = {https://www.sciencedirect.com/science/article/pii/S2352152X23002517},
  urldate       = {2023-07-03},
  language      = {en}
}