Designing of multifunctional soft and smart materials from natural sources is a useful strategy for producing safer chemicals having potential applications in biomedical research and pharmaceutical industries. Herein, eight glycolipids with variation in unsaturation of hydrophobic tail and polar headgroup size were designed. The effect of unsaturation in the tail group and headgroup size on gelation ability, and mechanical and thermal stability of glycolipid hydro/organogels was studied to understand structure and property relationship. Glycolipids are functional amphiphilic molecules having potential applications in the field of drug delivery and metal removal. The encapsulation capacity and kinetic release behavior of hydrophobic/hydrophilic bioactives like curcumin/riboflavin from the hydrophobic/hydrophilic pockets of glycolipids hydro/organogels was examined. A significant observation was that the glucamine moiety of the glycolipid headgroup plays a vital role in removal of Cr and Cu from oil/water biphasic systems. Typical functions of the glycolipid hydrogels are metal chelation and enzyme-triggered release behavior, enabled them as promising material for Cr, Cu removal from edible oils and controlled release of water soluble/insoluble bioactives.

Oleogelation is emerging as one of the most exigent oil structuring technique. The main objective of this study was to formulate and characterize rice bran/ sunflower wax-based oleogels using eight refined food grade oils such as sunflower oil, mustard oil, soybean oil, sesame oil, groundnut oil, rice bran oil, palm oil, and coconut oil. Stability and properties of these oleogels with respect to oil unsaturation and wax composition were explored. Sunflower wax exhibited excellent gelation ability even at 1%-1.5% (w/v) concentration compared to rice bran wax (8%-10% w/v). As the oleogelator concentration increased, peak melting temperature also increased with increase in strength of oleogels as per rheological studies. X-ray diffraction and morphological studies revealed that oleogel microstructure has major influence of wax composition only. Sunflower wax oleogels unveiled rapid crystal formation with maximum oil binding capacity of 99.46% in highly unsaturated sunflower oil with maximum polyunsaturated fatty acid content. Further, the applicability of this wax based oleogels as solid fat substitute in marketed butter products was also scrutinized. The lowest value of solid fat content (SFC) in oleogel was 0.20% at 25 C, resembling closely with the marketed butter products. With increase in oil unsaturation, oleogels displayed remarkable reduction in SFC. Depending upon prerequisite, oleogel properties can be modulated by tuning wax type and oil unsaturation. In conclusion, this wax-based oleogel can be used as solid fat substitute in food products with extensive applications in other fields too.

Designing of supramolecular hydro-/organogels having desired properties, biocompatibility, and stimuli responsiveness is a challenging task. Herein, the gelation ability of amphiphilic glycolipid-based gelators in a wide range of solvents is explored. The structure–function relationship was established by varying the chain length and polar headgroup size of amphiphilic gelators. The prepared hydro-/organogels were characterized by employing several techniques such as differential scanning calorimetry (DSC), rheology, field emission scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), etc. The thermal stability of hydro-/organogels increased with an increase in chain length. Rheological analysis depicted that variation in chain length and headgroup size of amphiphilic gelators significantly affected the gel strength and stability. The self-assembled morphology of hydro-/organogel samples revealed the compact entangled fibrillar network structures. After comparing the energy-minimized molecular length with the d-spacing value obtained by XRD, interdigitated bilayer packing in the gel network was established. The bioactive encapsulation and enzymatic release study of hydro-/organogels portrayed their potential application in the biomedical field. To our delight, glycolipid 16M (C16 chain length) formed a molecular hydrogel with injectable and thixotropic behaviors. High critical strain value, thixotropy, injectability, thermoreversibility, and faster bioactive release for the 16M-W hydrogel proved crucial to predict its future applications. Overall, glycolipid amphiphiles designed by upholding proper hydrophilic–lipophilic balance can form multifunctional supramolecular hydrogels with excellent implementation in the drug delivery system.