ABSTRACT
HYPOTHESIS: Anisotropic particles with a high aspect ratio led to favorable interfacial adhesion, thus enabling Pickering emulsion stabilization. Herein, we hypothesized that pearl necklace-shaped colloid particles would play a key role in stabilizing water-in-silicone oil (W/S) emulsions by taking advantage of their enhanced interfacial attachment energy. EXPERIMENTS: We fabricated hydrophobically modified silica nanolaces (SiNLs) by depositing silica onto bacterial cellulose nanofibril templates and subsequently grafting alkyl chains with tuned amounts and chain lengths onto the nanograins comprising the SiNLs. FINDINGS: The SiNLs, of which nanograin has the same dimension and surface chemistry as the silica nanospheres (SiNSs), showed more favorable wettability than SiNSs at the W/S interface, which was supported by the approximately 50 times higher attachment energy theoretically calculated using the hit-and-miss Monte Carlo method. The SiNLs with longer alkyl chains from C6 to C18 more effectively assembled at the W/S interface to produce a fibrillary interfacial membrane with a 10 times higher interfacial modulus, preventing water droplets from coalescing and improving the sedimentation stability and bulk viscoelasticity. These results demonstrate that the SiNLs acted as a promising colloidal surfactant for W/S Pickering emulsion stabilization, thereby allowing the exploration of diverse pharmaceutical and cosmetic formulations.
ABSTRACT
HYPOTHESIS: 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. EXPERIMENTS: 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. FINDINGS: 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.
