Stochastically Generated Digital Twins of 3D Solid‐State Electrolyte Architecture

Solid‐state lithium batteries (SSBs) have the potential to overcome conventional Li‐ion batteries in performance and safety. SSBs are typically manufactured through casting techniques to produce 3D electrode architectures that increase interfacial surface area and improve cell kinetics. However, these microstructures are often very complex and the exact influence of their geometries on their electrochemical performance can best be determined through numerical simulations. The main obstacle to numerically studying porous electrodes is the difficulty of obtaining high‐quality geometric data. In place of characterizing real samples, a costly and time intensive process, researchers seeking to intelligently design SSB microstructures may choose to run their calculations on stochastically generated digital twins (DTs). Naturally, the quality of these results rests on the fidelity of the DTs with real materials. This work develops a stochastic model and validation suite to produce the highest fidelity computer‐generated microstructures. The DTs generated with this model are compared to several solid‐state electrolyte samples characterized with Focused‐Ion Beam, Scanning Electron Microscopy (FIB‐SEM), and X‐Ray Micro‐Computed Tomography (µCT). An analysis of these microstructures across a series of tape‐casting parameters (including particle size, ceramic volume fraction, and particle roughness) reveals the existence of several geometric relationships that are characteristic of the tape‐casting process.