(Invited) Three-Dimensional Modeling of Dendrite Formation during Rapid Charging

Abstract

Dendrites commonly form during rapid charging of lithium-ion batteries when plating is favored over intercalation. If not mitigated, the potential exists for dendrites to growth through the separator and short the anode and cathode. One metric for diagnosing plating conditions in a computational model is the minimum local potential at the anode, where plating is seen to be thermodynamically favorable below 0.0 V with respect to Li metal.[1, 2] Three-dimensional (3D) models can offer insight to predict the possibility of local lithium plating and can be used as a tool to detect possible global lithium plating onset, so it follows that 3D microstructure models can be used to predict dendrite formation and propagation as well. The volume of fluid (VoF) method, which is commonly used to model the flow of immiscible fluids, can be used to divide the electrolyte region into a liquid phase and a dendrite phase.[3] This strategy is implemented in a 3D microstructure model of a lithium-ion battery to observe the growth of dendrites at the anode during rapid charging. Under onset conditions at the solid/electrolyte interface (SEI), the solid metal phase is deposited at the SEI. Upon growth, the overall electrolyte resistance at the tip of the metal phase is reduced, leading to dendrite growth. The 3D model provides valuable insight into various conditions that may cause plating, if dendrites are formed due to plating, and whether the dendrites formed may proceed to a shorting evenReference T. R. Garrick, J. Gao, X. Yang and B. J. Koch, J Electrochem Soc, 168, 010530 (2021).U. Janakiraman, T. R. Garrick and M. E. Fortier, J Electrochem Soc, 167, 160552 (2020).T. Jang, L. Mishra, S. A. Roberts, B. Planden, A. Subramaniam, M. Uppaluri, D. Linder, M. P. Gururajan, J.-G. Zhang and V. R. Subramanian, J Electrochem Soc, 169, 080516 (2022).