Three-dimensional physical modeling of the wet manufacturing process of solid-state battery electrodes

Abstract

Poor design of composite electrodes in Solid-State Batteries (SSBs) is one of the main reasons for their low performance. Although modeling techniques offer great potential in investigating multiple conditions for microstructure optimization, SSB manufacturing remains almost unaddressed in terms of computational studies. We present here a three-dimensional physics-based modeling workflow to investigate the impact of wet manufacturing process parameters on the properties of SSB tape casted composite electrodes based on LiNi0.6Mn0.2Co0.2O2 as the active material and Li6PSCl5 sulfide solid electrolyte. Our proposed workflow models the entire process of wet manufacturing of SSB electrodes, starting with the slurry consisting of active material, carbon additive, binder, solid electrolyte and solvent, and continues through its drying process, and the calendering of the resulting electrodes. Our focus is in particular on the impact of the calendering degree on the microstructure of the electrode. We characterize the resulting microstructures in terms of electronic and ionic conduction properties. We believe that this first-of-its-kind wet manufacturing process model for SSB cathodes is an important step towards the development of systematic modeling approaches that can provide practical optimization of the interfaces between materials in electrodes to improve SSB performance and durability.