Publication date: 10th April 2024
All-solid state batteries are promising candidates to achieve high energy densities and enable the use of high capacity anodes such as lithium metal or silicon alloys. Over the last years, intensive efforts have been made to improve the ionic conductivity of solid electrolytes and to gain detailed knowledge of the structure and transport behavior in their pristine state. However, for the preparation of cathode composites, processing methods as ball milling are applied to mix the ionic conductors with cathode active materials. While these post-synthesis processing steps are applied very frequently in the preparation of solid-state batteries, little is known about how exactly the processing step influences the properties of the solid electrolyte.
Here, we use an extensive set of experimental methods to fundamentally study the effects of post-synthesis ball milling on the highly conducting chloride-rich argyrodite Li5.5PS4.5Cl1.5. Investigating the crystallinity by X-ray diffraction and neutron pair distribution function shows that ball milling clearly decreases the crystallite size of the ionic conductor. In combination with nuclear magnetic resonance spectroscopy, we observed that the general local structure is maintained with a slight increase of disorder. The reduced crystallite size correlates with a decrease in ionic conductivity in the processed solid electrolytes. Nevertheless, the smaller particles lead to lower tortuosity when fabricating cathode composites, overall affecting performance. Optimization of these processing conditions can play a significant role on the road to highly performing solid state batteries.
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