Synergistic Interactions of Plant Protein Microgels and Cellulose Nanocrystals at the Interface and Their Inhibition of the Gastric Digestion of Pickering Emulsions

It is possible that Pickering emulsions can optimize the transport of nutraceuticals, pharmaceuticals, and other bioactive compounds in human physiology. So-called ultrastable Pickering emulsions are often destabilized in the gastric digestion regime if the particles are proteinaceous in nature. The present study seeks to test how the interfacial structure can be engineered via synergistic particle-particle interactions to impact the gastric coalescence of Pickering emulsions. In this study, we designed plant-based protein-particle-stabilized oil-in-water emulsions (PPM-E, with 20 wt % sunflower oil) via pea protein microgels (PPM at 1 wt %). The PPM hydrodynamic diameter is ∼250 nm. In vitro gastric digestion of PPM-E confirmed droplet coalescence within 30 min of pepsin addition. Supposedly surface-active cellulose nanocrystals (CNCs, 1-3 wt %) were added to PPM-E at pH 3.0 to determine if they could act as a barrier to interfacial pepsinolysis due to the CNC and PPM being oppositely charged at this gastric pH value. A combination of confocal microscopy, zeta potential, and Langmuir trough measurements suggested that CNCs and PPMs might form a combined layer at the O/W interface, owing to the electrostatic attraction between them. CNCs at >2 wt % inhibited the pepsinolyis of the adsorbed PPM film and thus droplet coalescence. However, increasing concentrations of CNC also increased the bulk viscosity of the PPM-E and eventually caused gelation of the emulsions, which would also delay their gastric breakdown. In conclusion, tuning the bulk and interfacial structure of Pickering emulsions via synergistic interactions between two types of particles could be an effective strategy to modify the enzymatic breakdown of such emulsions, which would have important applications in pharmaceuticals, foods, and other soft-matter applications.