Microfluidic macroemulsion stabilization through in situ interfacial coacervation of associative nanoplatelets and polyelectrolytes

[Display omitted] •Monodisperse macroemulsions were produced through electrostatic attraction-driven in situ interfacial coacervation.•Interfacial coacervation led to formation of a mechanically robust membrane, thus solidifying emulsion interfaces.•Our interfacial engineering technology will overcome the conventional challenge of stabilizing macroemulsions. Since macroemulsions tend to break down to lower free energy, they hardly retain their initial drop state. Therefore, studies are being conducted to overcome this based on advanced interface engineering techniques, but it is still challenging. Herein we hypothesize that the stability of giant droplets can be secured without chemical bonding through the interfacial coacervation of polyelectrolyte and associative nanoplatelets. We synthesized associative silica nanoplates (ASNPs) via polypeptide-templated silicification and consecutive wettability adjustment. To produce monodisperse macrodroplets, the inner fluid containing partially positively charged ASNPs and the outer fluid dissolving negatively charged polyacrylic acid (PAA) were coflowed through a capillary-based microfluidic channel. Dynamic interfacial tension and interfacial rheology measurements revealed that the migration of ASNPs and PAA from each phase to the interface led to the formation of a complex bilayered thin membrane with an enhanced interfacial modulus. In addition, we demonstrated that adjusting the surface properties of ASNPs by coupling a fluorochemical enabled the production of monodisperse fluorocarbon-in-oil-in-water double macroemulsions. These results highlighted the applicability of our microfluidics-based interfacial coacervation technology in the development of complex fluid products with visual differentiation and drug encapsulation.