Luo, PingBayés-García, LauraCalvet Pallàs, Maria TeresaLi, XuanZhang, Lu2026-02-192026-01-221438-2377https://hdl.handle.net/2445/227075Although oleogels are promising substitutes for saturated fats, their widespread adoption is hindered by multiple factors, among which an insufficient understanding of their crystallization behavior remains a key barrier. This work presents the first systematic analysis of the crystallization behavior in thermo-reversible linseed oil (LO)-based oleogels. The investigation combines in situ X-ray diffraction with thermal and microscopic analyses across a wide temperature range (-80 °C to 80 °C). We compared three natural waxes, sunflower wax (SFW), candelilla wax (CDW), and rice bran wax (RBW), along with two behenate-based glycerides, glyceryl behenate (GB) and fully hydrogenated high erucic acid rapeseed oil (FHR), as gelators for structuring LO. While LO itself exhibited both sub-α and β′ polymorphs, wax-based oleogels predominantly stabilized the β′ form. In contrast, oleogels with FHR or GB showed coexisting α/β′ and α/sub-α forms, respectively. Additionally, a β′ to β transformation was observed upon further heating in FHR-containing oleogels. Although most oleogels exhibited higher oil-binding capacity (OBC) at 5 °C than at 25–35 °C, the GB-containing oleogel achieved the highest OBC at 35 °C. These findings highlight the essential role of gelator polymorphism and crystal morphology in tailoring oleogel properties, guiding the rational design of functional oleogels for specific applications.26 p.application/pdfeng(c) Springer Verlag, 2026Cristal·lografiaPolimorfisme (Cristal·lografia)CrystallographyPolymorphism (Crystallography)info:eu-repo/semantics/article7659772026-02-19info:eu-repo/semantics/embargoedAccess