Abstract
Oleogels must replicate the rheological behavior of saturated fats at processing and consumption temperatures to maintain their physical stability and sensory acceptance. Thus, multicomponent oleogels present a promising approach since oleogelators can exhibit structuring and melting at different temperatures. The aim of the study was to produce a mixture of ultra-chain-long esters capable of structuring and modulating rheological behavior in response to temperature exposure. Therefore, enzymatic transesterification between sorbitol and fully hydrogenated crambe oil (FHCO) was performed to produce a mixture of ultra-long-chain sorbitan esters (SB) for efficient structuring of sunflower oil. SB generated in a reaction medium consisting exclusively of ethanol (60 °C, 200 rpm, 1:1 molar ratio) was selected for its high sorbitol consumption (~95%). While SB oleogels exhibited higher gel strength at 5 °C, at 25 °C, FHCO oleogels were stiffer, showing the gradual melting of SB oleogels evaluated by temperature-dependent rheological analyses and thermal properties. Oleogelation inhibited hydroperoxide formation compared to sunflower oil over 30 days. Results highlight the potential of multicomponent oleogels based on ultralong-chain esters for healthier and more stable high-lipid products. Modulating rheological thermoresponsiveness ensures physical stability under refrigeration while providing a texture similar to saturated fats during spreading and swallowing.