Heteroaggregation effects on Pickering stabilization using oppositely charged cellulose nanocrystal and nanochitin

Pickering emulsions are stabilized using complexes of cellulose nanocrystals (CNC) and nanochitin (NCh). The colloidal behavior and heteroaggregation in aqueous media are studied in relation to complex formation and net charge. The complexes are remarkably effective in stabilizing oil-in-water Pickering emulsions under conditions of slightly net positive or negative charges, as determined by the CNC/NCh mass ratio. Close to charge neutrality (CNC/NCh ~5), large heteroaggregates form, resulting in unstable emulsions. By contrast, under net cationic conditions, interfacial arrest of the complexes leads to non-deformable emulsion droplets with high stability (no creaming for 9 months). At given CNC/NCh concentrations, emulsions with up to 50% oil fraction are produced. This study shows how to control emulsion properties beyond consideration of the typical formulation variables, for instance, through adjusting CNC/NCh ratio or charge stoichiometry. We highlight the possibilities that are available for emulsion stabilization by using a combination of polysaccharide nanoparticles.