We report on high-internal-phase,
oil-in-water Pickering emulsions
that are stable against coalescence during storage. Viscous, edible
oil (sunflower) was emulsified by combining naturally derived cellulose
nanocrystals (CNCs) and a food-grade, biobased cationic surfactant
obtained from lauric acid and L-arginine (ethyl lauroyl arginate,
LAE). The interactions between CNC and LAE were elucidated by isothermal
titration calorimetry (ITC) and supplementary techniques. LAE adsorption
on CNC surfaces and its effect on nanoparticle electrostatic stabilization,
aggregation state, and emulsifying ability was studied and related
to the properties of resultant oil-in-water emulsions. Pickering systems
with tunable droplet diameter and stability against oil coalescence
during long-term storage were controllably achieved depending on LAE
loading. The underlying stabilization mechanism was found to depend
on the type of complex formed, the LAE structures adsorbed on the
cellulose nanoparticles (as unimer or as adsorbed admicelles), the
presence of free LAE in the aqueous phase, and the equivalent alkane
number of the oil phase (sunflower and dodecane oils were compared).
The results extend the potential of CNC in the formulation of high-quality
and edible Pickering emulsions. The functional properties imparted
by LAE, a highly effective molecule against food pathogens and spoilage
organisms, open new opportunities in food, cosmetics, and pharmaceutical
applications, where the presence of CNC plays a critical role in achieving
synergistic effects with LAE.