Assessment of Core-Shell and Agglomerate Particle Design for All-Solid-State Batteries

All-solid state lithium polymer batteries are promising next-generation batteries with high safety and energy density. Their success depends on an improved design with a tailored cathode manufacturing process. To facilitate a knowledge-driven optimal design of cathode, a model-based analysis on the impact of the cathode particle structure on the electrochemical cell performance is conducted. During production of solid-state cathodes, small active material particles such as lithium-iron phosphate tend to form large agglomerates with inner electrolyte-filled pores which have significant effect on transport properties within a secondary particle. Therefore, a battery cell model with secondary particles and optionally with a core-shell structure is developed and evaluated. Discharge performance is shown to be stronger impacted by changing the electrolyte fraction inside the particle than by changing the size of the electrolyte core within the secondary particle. A core-shell structure has a positive impact on the discharge performance and should be preferred for high power application. In contrast, cells with homogeneous agglomerate particles show better performance at low discharge rates. Thus, they are recommended for high energy and low power applications. The results of this study highlight the potentials of tailored production process for next-generation batteries.