Tunable distribution of silica nanoparticles in water-borne coatings via strawberry supracolloidal dispersions

Hypothesis: Water-borne coatings are rapidly expanding as sustainable alternatives to organic solvent-borne systems. Inorganic colloids are often added to aqueous polymer dispersions to enhance the performance of water-borne coatings. However, these bimodal dispersions have many interfaces which can result in unstable colloids and undesirable phase separation. The covalent bonding between individual colloids, on a polymer -inorganic core-corona supracolloidal assembly, could reduce or suppress instability and phase separation dur-ing drying of coatings, advancing its mechanical and optical properties. Methods: Aqueous polymer-silica supracolloids with a core-corona strawberry configuration were used to pre-cisely control the silica nanoparticles distribution within the coating. The interaction between polymer and silica particles was fine-tuned to obtain covalently bound or physically adsorbed supracolloids. Coatings were prepared by drying the supracolloidal dispersions at room temperature, and their morphology and mechanical properties were interconnected. Findings: Covalently bound supracolloids provided transparent coatings with a homogeneous 3D percolating silica nanonetwork. Supracolloids having physical adsorption only, resulted in coatings with a stratified silica layer at interfaces. The well-arranged silica nanonetworks strongly improve the storage moduli and water resistance of the coatings. These supracolloidal dispersions offer a new paradigm for preparing water-borne coatings with enhanced mechanical properties and other functionalities, like structural color.