Spontaneous Formation of Double Emulsions at Particle-Laden Interfaces

Abstract: Double emulsions, due to their compartmental structures, are essential in food, agricultural, and pharmaceutical applications. Traditionally, double emulsifications rely on the presence of both oil-soluble and water-soluble surfactants or external stimuli responsive materials and require sequential droplet formation settings or unique fluidic designs. We report on unusual phenomenon where double emulsions are spontaneously formed as soon an aqueous nanoparticle dispersion is placed in contact with an oleic micellar solution. Nanoscale water droplets nucleate in oil in the form of swollen micelles. Nanoparticles form a water-shell encapsulating the saturated oil phase with swollen micelles over time. Remarkably, we find that the gradual surface-activation of nanoparticles is key in self-double emulsification and controlling the emulsion intensity. We build on this new discovery and design a novel system for double emulsion formation. This approach is a scalable self-sequential strategy for preparing core-shell double emulsions that disperses nanoparticles in the opposite phase by employing micelles as transport vehicles. Incorporating nanoparticles into spontaneous emulsification systems opens novel routes for designing emulsion-based materials.