Biological materials achieve directional reinforcement with oriented assemblies of anisotropic building blocks. One such example is the nanocomposite structure of keratinized epithelium on the toe pad of tree frogs, in which hexagonal arrays of (soft) epithelial cells are crossed by densely packed and oriented (hard) keratin nanofibrils. Here, a method is established to fabricate arrays of tree-frog-inspired composite micropatterns composed of polydimethylsiloxane (PDMS) micropillars embedded with polystyrene (PS) nanopillars. Adhesive and frictional studies of these synthetic materials reveal a benefit of the hierarchical and anisotropic design for both adhesion and friction, in particular, at high matrix–fiber interfacial strengths. The presence of PS nanopillars alters the stress distribution at the contact interface of micropillars and therefore enhances the adhesion and friction of the composite micropattern. The results suggest a design principle for bioinspired structural adhesives, especially for wet environments.

When a colloidal suspension droplet evaporates from a solid surface, it leaves a characteristic deposit in the contact region. These deposits are common and important for many applications in printing, coating, or washing. By using superamphiphobic surfaces as a substrate, the contact area can be reduced so that evaporation is almost radially symmetric. While drying, the droplets maintain a nearly perfect spherical shape. Here, we exploit this phenomenon to fabricate supraparticles from bidisperse colloidal aqueous suspensions. The supraparticles have a core-shell morphology. The outer region is predominantly occupied by small colloids forming a close-packed, crystalline structure. Towards the center, the number of large colloids increases and they are packed amorphously. The extent of this stratification decreases with decreasing the evaporation rate. Complementary simulations indicate that evaporation leads to a local increase in density, which in turn exerts stronger inward forces on the larger colloids. Comparison between experiments and simulations suggest that hydrodynamic interactions between the suspended colloids reduce the extent of stratification. Our findings are relevant for the fabrication of supraparticles for applications in the fields of chromatography, catalysis, drug delivery, photonics, and a better understanding of spray drying.

Supraparticles consisting of nano- or microparticles have potential applications as e.g., photonic crystals, drug carriers, or heterogeneous catalysts. To avoid the use of solvent or processing liquid one can make supraparticles by evaporating droplets of aqueous suspensions from super-liquid-repellent surfaces. Herein, a method to adjust the porosity of supraparticles is described; a high porosity is desired, e.g., in catalysis. To prepare highly porous TiO2 supraparticles, polymer nanoparticles are co-dispersed in the suspension. Supraparticles are formed through evaporation of aqueous suspension droplets on superamphiphobic surfaces followed by calcination of the sacrificial polymer particles. The increase of porosity of up to 92%, resulted in enhanced photocatalytic activity while maintaining sufficient mechanical stability.