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The structuring of vegetable oils without the use of saturated and trans fatty acids is essential for the food industry, which nowadays faces the challenge of incorporating healthy edible oils in food products. Through the molecular self-assembly of monoglycerides (MGs) we can structure highly unsaturated edible oils, developing oleogels with physical and functional properties that closely mimic those provided by saturated and trans fats. Unfortunately, MG oleogels are metastable and the polymorphic changes that occur during storage result in a deleterious effect of the oleogel's functional properties and, eventually, in oil phase separation. This chapter discusses the basic principles in the use of phase diagrams for the development of MG oleogels and their relationship with the oleogel's rheology. In the same way, this chapter presents results about the synergistic interactions of MGs with lecithin and with ethylcellulose during the development of oleogels. The oleogels formulated with MG–lecithin and MG–ethylcellulose mixtures have excellent rheological and oil-binding properties, with the additional plus of having longer term stability for oil phase separation than the MG oleogels. These results open new alternatives to diversify the use of MG oleogels in food products.

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