Roughly Spherical: Tailored PMMA–SiO₂ Composite Supraparticles with Optimized Powder Flowability for Additive Manufacturing

Particulate materials with well-engineered properties are of key importance for many aspects in our daily life. Polymer powders with high flowability, for example, play a crucial role in the emerging field of powder-based additive manufacturing processes. However, the polymer- and composite material selection for these technologies is still limited. Here, we demonstrate the design of spherical polymethyl methacrylate (PMMA) and PMMA–SiO2 composite supraparticle powders with excellent powder flowability and tailored composition for powder-based additive manufacturing. Our process assembles these powders from the bottom up and affords a precise control over surface roughness and internal morphology via the choice of colloidal primary particles. We establish process-structure-property relationships connecting external spray-drying parameters and primary particle sizes with the resulting supraparticle roughness and, subsequently, with the macroscopic powder flowability and powder bed density. In a second step, we demonstrate the control of composition and internal morphology of PMMA–SiO2 composite supraparticles based on different mass mixings and diameter ratios of the two primary particle dispersions. Finally, we successfully apply the prepared supraparticle powders in powder bed additive manufacturing. The optimized flowability of the composite powders allows the production of two-layered square specimens with fusion between the individual layers and a uniform and tunable distribution of nanoscale SiO2 additives without requiring the addition of any flowing aids.