Abstract
The rheological properties of the electrode slurry significantly influence the manufacturing process of solid‐state batteries, affecting coating quality and the resulting cathode microstructure. The correlation between slurry attributes and final electrode characteristics is analyzed using particle size and solid content as key metrics. The performed coarse‐grained molecular dynamics simulations of LiNi0.8Mn0.1Co0.1O2 and Li6PS5Cl composite electrodes closely fit experimental viscosity, indicating the model's suitability for predicting slurry behavior. Then the microstructural properties of the dry and calendered electrodes are calibrated with the experiments. The simulation workflow is fitted completely using only two sets of force fields, one for the slurry and the other for the dry state of the electrode. The effective electronic conductivities are contingent on the particle size, without showing significant limitation on cathode rate capabilities. This comprehensive study highlights the intricate interplay between slurry solid content, microstructure design, and manufacturing processes in optimizing solid‐state battery performance. Consistent slurry characteristics are crucial for uniform electrode coating while optimizing particle size and solid content improves electrode porosity. The findings provide valuable insights for enhancing solid‐state battery design and manufacturing processes for the adaptation of already established scaling up technologies.