Experimental and Computational Analysis of Slurry-Based Manufacturing of Solid-State Battery Composite Cathode

The rheological properties of the slurry significantly influence the manufacturing process of solid-state battery cathode electrodes, 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. We perform coarse-grained molecular dynamics simulations of LiNi_0.8Mn_0.1Co_0.1O₂ and Li₆PS₅Cl composite electrodes, with simulated slurries closely fitting experimental viscosities, indicating the model's suitability for predicting slurry behavior. Then the microstructural properties of the dried and calendered electrodes are calibrated with in house experimental data. The simulation workflow is fitted completely using only two sets of force fields, one for the slurry and the other one for the dried state of the electrode. The effective electronic conductivities are contingent on the particle size, without showing significant limitation on cathode power capabilities. This comprehensive study highlights the intricate interplay between slurry solid content, microstructure design, and manufacturing processes in optimizing solid-state battery cell performance. Consistent slurry characteristics are crucial for uniform electrode coating while optimizing particle size and solid content improves electrode porosity. These findings provide valuable insights for enhancing solid-state battery electrode design and slurry-based manufacturing processes for the adaptation of already established scaling up technologies.