3D Multiscale Lithium‐Ion Cell Modeling for LiFePO4 Freeze‐Casted Electrode Structures Using Synchrotron X‐Ray and FIB/SEM Tomography

Abstract

AbstractThe performance of batteries and the associated operating areas depend, among other things, on the 3D microstructures of the electrode materials, and thus fundamental research is required in the field of electrode design. A multiscale microstructure‐resolved 3D model is developed that investigates two different LiFePO4 freeze‐casted electrode structures, that is, cellular and lamellar. The microstructure is simulated directly from the X‐ray computed tomography data and the nanostructure is combined with the pseudo‐2D simulation approach, where the morphological parameters and the distribution of the binder, carbon, and LiFePO4 are obtained from ex situ focused ion beam scanning electron microscopy measurements. The discharge performance shows that the lamellar structure exhibits a lower ohmic overvoltage and achieves a higher gravimetric capacity compared to the cellular structure, even though both electrode materials have the same porosity and amount of active material. The simulation reveals that the performance is not only directly influenced by the lithium‐ion transport through the porous structure but also by the current distribution through the active material. Based on these insights, lamellar electrode structures should be considered for next‐generation battery electrodes. The modeling approach can assist in electrode fabrication by identifying defects or suggesting better structural parameters.