Among available structuring agents that have been used to provide solid properties to liquid oils, protein is a more recent candidate. Due to their nutritional value and high consumer acceptance, proteins are of special interest for the preparation of edible oleogels as an alternative for solid fats. Whereas the field of protein oleogelation is still rather new and just starts unfolding, several preparation methods have been demonstrated to be suitable for protein oleogel preparation. However, there is limited knowledge regarding the link between microstructural properties of the gels and macroscopic rheological properties, and the potential of such protein-based oleogels as a fat replacer in food products. In this review, we therefore provide an overview of various protein oleogel preparation methods and the resulting gel microstructures. Based on the different structures, we discuss how the rheological properties can be modified for the different types of protein oleogels. Finally, we consider the suitability of the different preparation methods regarding potential applications on industrial scale, and provide a short summary of the current state of knowledge regarding the behavior of protein oleogels as a fat replacer in food products.

Particle size distribution and particle size ratio have an important effect on rheological properties of model chocolate samples, but also other factors like particle shape, surface roughness and hydrophilicity should be taken into account.

Capillary suspensions feature networks of particles connected by liquid bridges, which are obtained by adding a small amount of a second immiscible liquid to a suspension. It is possible to link the network formation as well as the rheological behaviour of capillary suspensions to the intermolecular interactions of their constituents. Through a combination of experimental and numerical methods, we present a novel approach, based on Hansen solubility parameters computed from Molecular Dynamics (MD) simulations, to rationalize and predict the rheological behaviour of capillary suspensions. We investigated the formation of capillary suspensions for various combinations of bulk and secondary liquids mixed with hydrophilic silica particles. The predictions were confirmed experimentally by rheological analysis, interfacial tension measurements and microscopy (CLSM) imaging. Numerical and experimental results show that the Hansen solubility parameters theory allows to predict the formation of capillary suspensions, whose strength exponentially decays with decreasing intermolecular interactions between the secondary liquids and the dispersed particles. High immiscibility between the bulk and secondary liquid strengthens the gel up to a critical immiscibility point, above which the strength of the gel remains mostly affected by the affinity between the secondary liquids and the dispersed particles. Furthermore, we find that hydrogen-bonding and polar interactions control the formation of capillary suspensions. This simple approach can guide the selection of adequate solvents and immiscible secondary liquids, allowing an easy formulation of new particulate-based gels.