Surface-tension-induced double emulsion drops via phase separation of polymeric fluid confined in micromolds for capsule templates.

We report a simple and rapid route to produce double emulsion drops by utilizing phase separation of the confined fluid in micromolds and surface-tension-induced drop formation. Specifically, we use cross-shaped micromolds containing prepolymer solution that phase-separates into two compartments upon addition of wetting fluid with separation agent (SA). Subsequently, Laplace pressure-driven flow allows it to form double emulsion drops without use of any surfactants and complex formulations of fluids. The size of each compartment in the emulsion drops can be controlled by tuning composition of the prepolymer solution and separation agent, making the double emulsion drops with varying shell thicknesses. The phase separation creates two compartments with different polarity (i.e. water-soluble and water-insoluble), enabling encapsulation of both hydrophilic and/-or hydrophobic cargoes in desired compartments depending on their solubility. In addition, we produce poly(N-isopropylacrylamide) (pNIPAm) hydrogel microcapsules by solidifying middle phase in the double emulsion drops; thus, hydrophilic large cargo loaded priorly in the core can be encapsulated within hydrogel shells. Finally, by taking advantage of hydrophilic-hydrophobic phase transition behavior of pNIPAm, we achieve encapsulation of small cargo via post-loading approach; the encapsulated cargo can be released by tuning temperature.