Deep eutectic solvents (DESs) are an emerging class of green solvents with a wide spectrum of potential applications whose properties may be further tailored through the addition of water. Here, we study, through molecular dynamics, the influence of water on the properties of a betaine-glycerol-water (B:G:W) DES (1:2:ζ; ζ = 0 to 100), aiming at getting insight into the structural and dynamic crossover between a DES and an aqueous solution. The density, shear viscosity, and diffusion coefficients are found to exhibit a non-linear dependence of ζ, similar to that observed for the solvation layers' composition. Each Gly and Bet are replaced, respectively, by ∼3 and ∼5 water molecules, with the highest rates of depletion being found for Gly around Bet and Gly around Gly. Above ζ = 7 (70 mol %; 29.5 wt %), a major structural transformation occurs, with the complete disruption of the second Bet-Gly solvation layer and the formation of a new second layer at a shorter distance, accompanied by a sudden change in the rate of increase of the components' diffusion. Nonetheless, opposite to other DES, our results indicate a smooth crossover between a DES and an aqueous solution.

This work investigated a green approach to obtain and stabilize Lavandula stoechas L. volatile organic compounds with sensory aroma characteristics by using alternative solvents, namely supercritical carbon dioxide (scCO2) and deep eutectic solvents (DES). The CO2 extracts were dispersed in different DES mixtures (betaine:ethylene glycol (1:3), betaine:glycerol (1:2), and glycerol:glucose (4:1)) and their stability was monitored during 6 months of storage at room temperature by monitoring the headspace (HS) profile. The CO2 extract was used as the control. It was initially determined that there was a dominant presence of oxygenated monoterpenes (67.33-77.50%) in the extracts. During storage, significant changes occurred in the samples' HS, such as the decrease in terpene hydrocarbons which also affected the presence of oxygenated terpenes, which increased in certain cases. Moreover, the highest formation of new components was recorded in the control which could be an indicator of decreased stability. The DESs-CO2 were more stable than the CO2 control and among them, betaine:ethylene glycol stood out as the most adequate systems for maintaining the stability of L. stoechas HS components. For the visual estimation of similarities and dissimilarities among the samples, chemometric pattern recognition approaches were applied including the hierarchical cluster analysis, principal component analysis, and sum of ranking differences.

A new methodology for the selective extraction of antioxidants from mate tea leaves (and decaffeinated mate tea leaves), using different natural deep eutectic systems (NADES), is reported in this paper. A fractionated extraction was carried out and the optimization of the extraction conditions such as solid/liquid ratio, temperature, time, stirring and the use of ultrasound assisted extraction (UAE) technology was performed. The results demonstrate that a sequential extraction using, in a first step, an hydrophobic system Men:Lau (2:1) and, in a second step, an hydrophilic lactic acid-based NADES, leads to two distinct extracts: the first one rich in pigments and the second one rich in polyphenols. NADES systems were able to extract 30% more of the polyphenolic components of the mate tea leaves matrices, when compared with traditional solvents/techniques. Moreover, it has been shown that the incorporation of the extract in the NADES, compared to the same extract in aqueous medium was beneficial for the stabilization of the antioxidants. It maintains their functionality at least for three months, reaching 41% more versus the extracts obtained by traditional solvents/techniques. The absence of caffeine in the extracts did not shown to have any effects on the stability results.

Defatted raspberry seeds were used as an alternative source of antioxidants and ellagic acid (EA) extracted using Natural deep eutectic solvents (NADES). In the preliminary study, the best NADES combination (citric acid-betaine) and the most influential variables (temperature, time, and NADES/plant ratio) were selected for the further optimization process. All samples were analyzed in terms of total polyphenol, EA content, and antioxidant activity. Two sets of optimal conditions were generated by response surface methodology. The first set (Opt1) was designed for higher conversion of ellagitannins to EA while the latter set (Opt2) for higher EA content/100 g extract. Opt1 and Opt2 had higher values for all investigated responses compared to 80% ethanolic extract but had a lower conversion rate of ellagitannins to EA compared to acidified methanol extract. The third set of parameters (Opt3) selected beyond the initial experimental domain was used to obtain a sample with the highest EA content/100 g extract. Due to their nature, NADES extracts are ready to use and could have various technological roles in products since they are antioxidants, acidifiers, and colorants. NADES raspberry extracts exhibited higher anti-proliferative activity compared to ethanolic extracts in terms of EC50 values. However, the main contributor of anti-cancer activity in NADES raspberry extracts were individual NADES compounds and/or their newly formed NADES structure.