Three-dimensional experimental-scale phase-field modeling of dendrite formation in rechargeable lithium-metal batteries. (June 2023)

• Record Type: Journal Article
• Authors: Arguello, Marcos E.; Labanda, Nicolás A.; Calo, Victor M.; Gumulya, Monica; Utikar, Ranjeet; Derksen, Jos
• Is Part Of: Journal of energy storage. Volume 62(2023)
• Publication Date: 2023-06
• Subjects: Phase-field modeling -- Lithium dendrite -- Inter-electrode distance -- Surface anisotropy -- Metal-anode battery -- Finite element method; Energy storage -- Periodicals; Energy storage -- Research -- Periodicals; 621.3126
• DOI: 10.1016/j.est.2023.106854
• Languages: English
• ISSNs: 2352-152X

Abstract

Abstract: This paper presents a phase-field based numerical study on the 3D formation of dendrites due to electrodeposition in an experimental-scale lithium metal battery. Small-scale 3D simulations were firstly conducted to elucidate the characteristics and resolution requirements of the numerical framework. Using a four-fold anisotropy model to simulate the growth of lithium deposition, the dependency of dendrite morphology on charging conditions ( ϕ b = − 0 . 7 V and ϕ b = − 1 . 4 V ) on a (larger) experimental-scale metal anode was demonstrated. The dendrite shape was found to shift from a smoother, tree-like formation at the lower applied voltage, to a more spike-like, highly branched structure at the higher voltage. The resulting morphological parameters, such as dendrite propagation rates, volume-specific area, and side branching rates, were compared against published experimental data and found to be comparable to the reported ranges for the electrodeposition of spike- or tree-like metal dendrites. This finding supports our previous observation that dendrite formation is connected to the competition between the lithium cation diffusion and electric migration, generating an uneven distribution of Li + on the electrode surface. This observation also gives insight into dendrite inhibition strategies focusing on enhancing the diffusion of lithium ions to achieve a more uniform concentration field on the anode surface. Highlights: Phase-field simulations of dendrite formation in lithium metal batteries. Evaluation of modified lithium crystal surface anisotropy representation. Analysis of 3D experimental-scale simulations. Change of dendritic behavior captured by variation of inter-electrode distance. Simulations' consistency with experimental results reported in the literature.