Various
supraparticles have been extensively studied owing to their
excellent catalytic properties that are attributed to their inherent
porous structure; however, their mechanical properties have not garnered
attention owing to their less dense structure. We demonstrate a rational
approach for fabricating assembled supraparticles and, subsequently,
highly dense microspheres. In addition, 3 mol % yttria-stabilized
zirconia (3YSZ) and alumina particles were selected as building blocks
and assembled into higher-order architectures using a droplet-based
template method (spray drying) for validation with proof-of-concept.
Moreover, structural features such as density, size, sphericity, and
morphology of supraparticles were controlled by adjusting the competing
kinetics occurring between the assembly of building blocks and evaporation
of the solvent in the droplets. The preparatory aqueous suspension
and process parameters were optimized as well. A detailed understanding
of the formation mechanism facilitated the yield of tailor-made supraparticles
and, thereafter, highly dense microspheres (approximate relative density
= 99%) with excellent sphericity (>98%) via heat
treatment. The microspheres displayed highest hardness (26.77 GPa)
and superior elastic modulus (210.19 GPa) compared with the mechanical
properties of the 3YSZ samples reported to date. Ultimately, the proposed
supraparticle engineering provided insight for controlling the structural
features and resultant micromechanical properties, which widely extends
the applicability of supraparticle-based functional materials for
practical purposes that require materials with high density and excellent
mechanical properties.