Numerical Modeling of a Low-Cobalt All-Solid-State Cell with Ceramic Electrolyte Using a Deformable Geometry

Abstract

All-solid-state batteries with a lithium negative electrode and a ceramic electrolyte are key toward high energy density. To ensure a safe, fast, accurate, and cost-effective development of this technology, the experimental methodology must be supported by the numerical modeling approach. This work proposes and describes an electrochemical model of a Li7La3Zr2O12 (LLZO) and Ni-rich NMC-based lithium cell with a deformable lithium negative electrode. Simulations were computed using the finite element method at different operating conditions to demonstrate the scope of the modeling work. Discharge rate tests, deformation tracking, geometric defect investigation, and polarization decomposition are described. Theoretical validation of the mass balance, the stripping rate, the ohmic polarization, and the mesh deformation demonstrated the consistency of the volumetric deformation strategy. We demonstrated in this study a deformable modeling strategy, which was found to be useful for the electrostripping analysis of anodic geometry defects during discharge. Non-uniformity in the lithium stripping rate was found along the anodic interface with defects, and this non-uniformity was accentuated with a higher discharge rate. The cell’s discharge potential was decomposed by considering the equilibrium potential and the polarizations of the main components of the cell. This post-processing was found to be useful for the understanding of the cell’s behavior.