Hydrophobic deep eutectic solvents (DES) have recently been used as green alternatives to conventional solvents in several applications. In addition to their tunable melting temperature, the viscosity of DES can be optimized by selecting the constituents and molar ratio. This study examined the viscosity of 14 eutectic systems formed by natural substances over a wide range of temperatures and compositions. The eutectic systems in this study were classified as ideal or non-ideal based on their solid-liquid equilibria (SLE) data found in the literature. The eutectic systems containing constituents with cyclohexyl rings were considerably more viscous than those containing linear or phenyl constituents. Moreover, the viscosity of non-ideal eutectic systems was higher than that of ideal eutectic systems because of the strong intermolecular interactions in the liquid solution. At temperatures considerably lower than the melting temperature of the pure constituents, non-ideal and ideal eutectic systems with cyclohexyl constituents exhibited considerably high viscosity, justifying the kinetic limitations in crystallization observed in these systems. Overall, understanding the correlation between the molecular structure of constituents, SLE, and the viscosity of the eutectic systems will help in designing new, low-viscosity DES.
Keywords: glass transition; hydrophobic deep eutectic solvents; monocarboxylic acids; solid–liquid equilibria; terpenes.