Lamellar periodicity population redistribution and elasticity in sunflower wax-based oleogels

The elasticity of sunflower wax (SFW)-based oleogels arises from the hierarchical organisation of their crystalline network. This study examines how cooling-rate-controlled crystallisation regulates elasticity through redistribution of coexisting lamellar periodicity populations. Small-angle X-ray diffraction reveals long- and slightly shorter-period lamellar components, while wide-angle X-ray diffraction confirms unchanged molecular packing, indicating no polymorphic transitions. The population of the slightly shorter-period component varies systematically with cooling rate. Peak broadening suggests differences in internal crystalline state, including accumulated strain and crystallite size, which may influence stiffness. In-situ time-resolved synchrotron measurements show that early-stage crystallisation kinetics affect subsequent structural heterogeneity. Shear-induced homogenisation reduces the shorter-period population and increases elasticity. Overall, mechanical properties are primarily associated with lamellar periodicity redistribution rather than changes in molecular packing, providing a structural basis for texture design in wax-structured edible oil systems.