Formation of oleogels based on emulsions stabilized with cellulose nanocrystals and sodium caseinate

Hypothesis: In the preparation of oleogels based on Pickering-emulsions, the choice of the preparation route is critical to withstand drying under ambient conditions, as it conditions the composition of the interfacial layer at the oil-water interface. Experiments: Hexadecane and olive oil oleogels were prepared using an emulsion-template approach from oil-in-water emulsions formulated with cellulose nanocrystals (CNC) and sodium caseinate (CAS) added in different orders (CNC/CAS together; first CAS then CNC; first CNC then CAS). The oleogels were formed from preconcentrated emulsions by drying at ambient temperature. The structure of the gels was characterised by confocal laser scanning microscopy, and the gels were assessed in terms of viscoelastic properties and redispersibility. Findings: The properties of oleogels were controlled by 1) the composition of the surface layer at oil water interface; 2) the amount and type of non-adsorbed stabilizer; and 3) the composition and viscosity of oils (hexadecane vs. olive oil). For the oleogels prepared from starting emulsions stabilized with CNC with subsequent addition of CAS, and free CAS present in aqueous phase, the elastic component was prevalent. Overall, the dominating species at the oil-water interface controlled the emulsion behaviour and stability, as well as viscoelastic behaviour of the resulting oleogels and their redispersibility. (c) 2021 The Authors. Published by Elsevier Inc. This is an open access article under the CC BY license (http:// creativecommons.org/licenses/by/4.0/).