Ultrastable Water-in-Oil High Internal Phase Emulsions Featuring Interfacial and Biphasic Network Stabilization

In this work, we present gel-in-gel water-in-oil (W/O) high internal phase emulsions (HIPEs) that feature high stability by structuring both phases of the emulsion. Compared to significant advances made in oil-in-water (O/W) HIPEs, W/O HIPEs are extremely unstable and difficult to generate without introducing high concentrations of surfactants. Another main challenge is the low viscosity of both water and oil phases which promotes the instability of W/O HIPEs. Here, we demonstrate ultrastable W/O HIPEs that feature biphasic structuring, in which hydrogels are dispersed in oleogels, and self-forming, low-concentration interfacial Pickering crystals provide added stability. These W/O HIPEs exhibit high tolerance toward pH shock and destabilizing environments. In addition, this novel ultrastable gel-in-gel W/O HIPE is sustainable and made solely with natural ingredients without the addition of any synthetic stabilizers. By applying phase structuring within the HIPEs through the addition of various carrageenans and beeswax as structurants, we can increase the emulsion's stability and viscoelastic rheological properties. The performance of these gel-in-gel W/O HIPEs holds promise for a wide range of applications. As a proof of concept, we demonstrated herein the application as a gelled delivery system that enables the co-delivery of hydrophilic and hydrophobic materials at maximized loads, demonstrating high resistance to gastrointestinal pHs and a controlled-release profile.