Spent coffee grounds, the main by-product of the coffee-brewing process, were valorized as a renewable source of lipids for the synthesis of novel wax esters and as an alternative and sustainable oil-structuring agent for the production of oleogels. The lipase-catalyzed reactions were implemented using fatty alcohols both under solvent-free conditions and with limonene as an environmentally friendly solvent. Wax esters were evaluated for their ability to formulate olive oil oleogels through the determination of the physical properties of oleogels. Results showed that high conversion yields were achieved when cetyl and behenyl alcohols were applied under solvent-free conditions, achieving a maximum yield of 90.3% and 91.7%, respectively. In the presence of limonene, the highest conversion yields were 88.9% and 94.5% upon the use of cetyl and behenyl alcohols, respectively. The behenyl wax esters exhibited greater oil-structuring properties, regardless of whether they were derived from solvent or solvent-free conditions. Rheological curves showed that the produced oleogels exhibited a strong gel strength, which was enhanced as the wax ester concentration increased. Frequency sweep curves confirmed the formation of a stable three-dimensional oleogel network and revealed the low dependence of the storage modulus on frequency. Overall, this study demonstrated that producing wax esters from renewable lipid sources has the potential to serve as an effective circular economy paradigm for creating novel oleogels with a broad range of applications.
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