Rheological characterization of solid lipids with domain structure

Authors
A. Todorova, D. Cholakova, N. Denkov, S. Tcholakova
Journal
Colloids Surf. A
Year
2026
Volume
742
Pages
140415
A. Todorova, D. Cholakova, N. Denkov, S. Tcholakova
Colloids Surf. A 2026
742
140415
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Abstract

Phase behavior of lipids is of primary importance for the manufacturing and applications of foods, cosmetics and pharmaceuticals, as well as for the functions of biological membranes. Upon cooling, the molten bulk lipids crystallize into ordered domains which determine their rheological properties. While storage and loss moduli are typically used to describe these properties, their direct connection to the underlying molecular rearrangement remains poorly understood. In the current study, we performed a detailed rheological characterization of the rotator phases (intermediate phases between fully ordered crystalline and completely disordered liquid phases) formed in bulk linear alkanes. Large series of stress-relaxation and creep-recovery experiments were performed and interpreted, using generalized Kelvin-Voigt model with one spring, connected in series with three combined elements of a spring and a dashpot. We determined the elasticities and viscosities of all these rheological elements, along with the respective three relaxation times of the combined elements. These relaxation times are governed by different molecular processes in the sheared samples and differ by three orders of magnitude: t1 ≈ 0.45 s and t2 ≈ 8–9 s are related to local molecular rearrangements at the domain boundaries, while t3 ≈ 140–200 s most probably describes the rearrangement of disordered lipid molecules entrapped between the ordered domains. The storage and loss moduli, calculated from the constants of the generalized Kelvin-Voigt model, were in a very good agreement with those measured directly in amplitude sweep and temperature ramps oscillatory tests, thus supporting the self-consistency of data interpretation. The methodology presented here is applicable to other polycrystalline lipid materials with 2D or 3D domain structures, providing a valuable framework for interpreting their rheological behavior.