Robust 2D Simulation of Morphological Evolution in Lithium-Metal Batteries
Authors: Jang Taejin , Mishra Lubhani , Shah Krishna , Mittal Prateek , Subramaniam Akshay , Gururajan Mogadalai P. , Roberts Scott A. , Subramanian Venkat R. 
Published: July 2021

The lithium-metal battery is drawing a lot of attention being among the top candidates for the next-generation batteries. This is due to the possibility of achieving high redox potential and specific capacity. While lithium plating is the key to the high specific capacity, the surface morphology deteriorates over cycles due to evolution of dendrites and dead lithium1. This results in capacity loss as well as safety risk due to the possibility of internal short-circuit caused by dendrites piercing through the separator2. Unfortunately, there is still a lack of understanding of the conditions that lead to such undesired interfacial phenomena. To understand and minimize these phenomena, it is crucial to have detailed physics-based 2D model and ability to perform robust simulations. Recently, we have provided well-defined 2D models relevant for lithium metal battery and elucidated the significance of rigorous convergence analysis3.

In the present work, we will discuss the morphological evolution over cycles as predicted by the proposed 2D moving boundary model using experimentally relevant parameters and conditions. One of the goals of this work is to find experimentally relevant conditions that lead to dendritic growth and gain insights into changes in surface morphology as the cell is cycled. The model equations are obtained through rigorous mathematical formulation of the relevant physical phenomena, and lithium seed, which is observed at the early stage of lithium deposition, is considered in the initial geometry for the simulation. The geometrical parameters used are based on experimental measurements reported in the literature4. In addition to the robust simulation with in-house moving boundary model codes, COMSOL Multiphysics, a commonly used commercial solver for battery simulations, is also used and results are compared. In particular, both phase field and moving mesh methods will be compared. Effect of parameters, and the choice of algorithms will be critically analyzed.

Acknowledgments

This research was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US Department of Energy (DoE) through the Advanced Battery Materials Research Program (Battery500 Consortium). Sandia National Laboratories is a multi-mission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC., a wholly owned subsidiary of Honeywell International, Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

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