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We report the fabrication of multiple emulsions where both the enclosed and the external water phases are structured using a combination of two non-gelling biopolymers. Emulsions (with gelled inner water droplets and gelled water continuous phase) were created using a simple ‘one-step’ process where the oil phase (triglyceride oil and polyglycerol polyricinoleate) and the water phase (containing a combination of locust bean gum and carrageenan) were emulsified at an elevated temperature (70 °C) followed by cooling to room temperature. The temperature triggered gelling of the synergistic biopolymer combination led to the formation of structured emulsions on cooling. Flowable to self-standing emulsion gels could be prepared by changing the total concentration of polymers (and the ratios of the individual polymers) as confirmed from low amplitude oscillatory shear rheology and creep recovery measurements. The cryo-scanning electron microscopy images of freeze-fractured emulsion samples revealed the presence of gelled inner water droplets. Further, when subjected to heating and cooling cycles, emulsions displayed reversible rheological changes which could be tuned by simply changing the total polymer concentration and the proportions of individual polymers. Such biopolymer-based structured emulsions with interesting microstructure and rheological properties could find potential applications in bio-related fields like food structuring.

Physical trapping of a hydrophobic liquid oil in a matrix of water-soluble biopolymers was achieved using a facile two-step process by first formulating a surfactant-free oil-in-water emulsion stabilized by biopolymers (a protein and a polysaccharide) followed by complete removal of the water phase (by either high- or low-temperature drying of the emulsion) resulting in structured solid systems containing a high concentration of liquid oil (above 97 wt %). The microstructure of these systems was revealed by confocal and cryo-scanning electron microscopy, and the effect of biopolymer concentrations on the consistency of emulsions as well as the dried product was evaluated using a combination of small-amplitude oscillatory shear rheometry and large deformation fracture studies. The oleogel prepared by shearing the dried product showed a high gel strength as well as a certain degree of thixotropic recovery even at high temperatures. Moreover, the reversibility of the process was demonstrated by shearing the dried product in the presence of water to obtain reconstituted emulsions with rheological properties comparable to those of the fresh emulsion.

The preparation and characterization of oleogels structured by using a combination of a surface-active and a non-surface-active polysaccharide through an emulsion-templated approach is reported. Specifically, the oleogels were prepared by first formulating a concentrated oil-in-water emulsion, stabilized with a combination of cellulose derivatives and xanthan gum, followed by the selective evaporation of the continuous water phase to drive the network formation, resulting in an oleogel with a unique microstructure and interesting rheological properties, including a high gel strength, G′>4000 Pa, shear sensitivity, good thixotropic recovery, and good thermostability.