Structural Build-Up and Stability of Hybrid Monoglyceride–Triglyceride Oleogels

Oleogelation is an alternative oil structuring route to formulate (semi-)solid fats with a reduced amount of saturated fats. Monoglycerides have been identified as effective gelators; however, their application potential can be limited due to challenges regarding mechanical strength and long-term stability. Therefore, the formulation of hybrid fat blends is a promising way to improve the functionality of oleogels. This research focuses on the interaction between mono- and triglycerides (MAGs and TAGs) in hybrid oleogels. A total gelator concentration of 10% (<i>w</i>/<i>w</i>) with changing MAGs-TAGs ratios (increase by 25% on a molar basis; M0-T100, M25-T75, M50-T50, M75-T25, M100-T0) was used. First, the oleogels were produced without shear to unravel the crystallization behavior (DSC, SAXS, WAXS). Next, the oleogels were crystallized with shear to assess the interactions between MAGs and TAGs on macroscale properties (rigidity, oil binding capacity) during storage of 1 day, 1 week, and 4 weeks. A clear distinction could be made between the MAG crystals and TAG crystals in the blends M50-T50 and M75-T25 based on WAXS, SAXS, and phase contrast microscopy. This indicates that both gelators crystallize separately. During the follow-up study of the dynamically produced samples, a synergistic effect was found for Dy-M50-T50 and Dy-M75-T25; however, it was not maintained upon storage. The initial rigidity of 2.4 × 10⁴ Pa and 2.0 × 10⁴ Pa decreased to 1.5 × 10⁴ Pa and 1.0 × 10⁴ Pa for Dy-M50-T50 and Dy-M75-T25, respectively.