https://hdl.handle.net/10259/4330 Thu, 28 May 2026 16:29:50 GMT 2026-05-28T16:29:50Z https://hdl.handle.net/10259/11717 Molecular layering and CO₂ selectivity in graphene-supported natural deep eutectic solvent films: An in-silico investigation Rozas Azcona, Sara; Aguilar Cuesta, Nuria; Marcos Villa, Pedro A.; Bol Arreba, Alfredo; Aparicio Martínez, Santiago A multiscale computational study was conducted to investigate graphene-supported thin films composed of a natural deep eutectic solvent (NADES) formed by menthol and decanoic acid (MENTH:DA), with a focus on applications in sustainable CO₂ capture. Density functional theory (DFT) and molecular dynamics (MD) simulations were employed to elucidate interfacial structuring, molecular interactions, and gas adsorption behavior. DFT results indicated a strong interaction between decanoic acid and the graphene surface (− 35.88 kJ/mol), characterized by a parallel orientation that maximizes van der Waals interactions. In contrast, menthol displayed weaker adsorption energies (− 5.15 kJ/mol) and a predominantly perpendicular orientation. MD simulations revealed the formation of distinct adsorption layers, with decanoic acid enriched in the first layer and menthol in the second, while the NADES hydrogen-bonding network remained largely intact. CO₂ exhibited preferential adsorption over flue gas components (N₂, H₂O, O₂), with substantial accumulation in both the first and second interfacial layers. Approximately 50% of the CO₂ content from flue gas mixtures was retained within the structured region. Adsorption performance was found to be largely independent of temperature (303− 323K) and NADES film thickness (20–50 Å). These results provide fundamental insight into NADES–graphene interactions and highlight the potential of type V, naturally derived deep eutectic solvents as selective and environmentally benign materials for CO₂ separation technologie Thu, 01 Jan 2026 00:00:00 GMT https://hdl.handle.net/10259/11717 2026-01-01T00:00:00Z https://hdl.handle.net/10259/11439 Molecular mechanisms of β-cyclodextrin solubilization in natural deep eutectic solvents: A quantum chemical investigation Huerta Sainz, Sergio de la; Escobedo Monge, María Antonieta; Escobedo-Monge, Marlene Fabiola; Bol Arreba, Alfredo; Marcos Villa, Pedro A.; Atilhan, Mert; Aparicio Martínez, Santiago Cyclodextrins, particularly β-cyclodextrin (β-CD), exhibit remarkable host-guest complexation capabilities due to their unique toroidal structures. Natural deep eutectic solvents (NADES), biocompatible mixtures of readily available components, represent sustainable alternatives to conventional solvents with tunable physicochemical properties. This work investigates the molecular interplay between β-CD and NADES, focusing on their potential to create sustainable, multifunctional materials. Two configurations were explored: (i) β-CD dissolved in NADES and (ii) β-CD acting as a NADES component. Using density functional theory simulations, the study examined intermolecular forces, confinement effects, and molecular topology to characterize host–guest interactions between atomistic models of selected NADES (menthol + thymol and menthol + decanoic acid) and β-CD complexes. Energetic and kinetic analyses provided insights into the driving forces and timescales of complexation processes. The findings contribute to a mechanistic understanding of NADES–CD systems, enabling rational selection of solvent compositions and cyclodextrin forms for optimized guest encapsulation and targeted functionalities. Sun, 01 Feb 2026 00:00:00 GMT https://hdl.handle.net/10259/11439 2026-02-01T00:00:00Z https://hdl.handle.net/10259/11438 Nature's tool kit: Designing biocompatible and affordable NADES for sustainable extraction of plant bioactives Huerta Sainz, Sergio de la; Escobedo Monge, María Antonieta; Marcos Villa, Pedro A.; Esteban-Ollo, José Antonio; Montejo-Gil, Laura; Conde-Rioll, María; Atilhan, Mert; Bol Arreba, Alfredo; Aparicio Martínez, Santiago Conventional extraction of valuable plant compounds often relies on hazardous volatile organic solvents (VOCs), posing environmental and health risks. This study explores a sustainable alternative using Natural Deep Eutectic Solvents (NADES) designed in-silico through the Conductor-like Screening Model for Realistic Solvents methodology (COSMO-RS) for efficient extraction of target plant metabolites. A library of NADES with varying compositions was designed using COSMO-RS to predict their physicochemical properties and affinity for target natural compounds, selecting the most promising candidates in terms of versatility, cost-effectiveness and biocompatibility. To complete the study, a predictive Artificial Intelligence based method (Decision Trees) was developed for reverse design of NADES for target bioactive compounds from energetic and structural molecular descriptors. From a compendium of 58 plant metabolites of interest and 66 natural compounds as NADES components, nearly 3000 solubility in silico tests were conducted and a total of 12 NADES were selected. Three solubility models were created, and a clear dependance of the target compound properties was observed. Sat, 01 Mar 2025 00:00:00 GMT https://hdl.handle.net/10259/11438 2025-03-01T00:00:00Z https://hdl.handle.net/10259/11437 Beyond the blend: Unveiling the thermophysical fingerprints of hydrated choline chloride deep eutectic systems with bio-derived and synthetic hydrogen bond donors Alcalde García, Rafael T.; Huerta Sainz, Sergio de la; Diez Cabanes, Valentin; Escobedo Monge, María Antonieta; Trenzado, José Luis; Atilhan, Mert; Bol Arreba, Alfredo; Aparicio Martínez, Santiago This study presents a comprehensive thermophysical characterization of hydrated deep eutectic solvents (DESs) composed of choline chloride (ChCl) and four hydrogen bond donors (HBDs): citric acid, malic acid, fructose, and ethylene glycol in equimolar ratios. By introducing 2, 10, and 22 wt% water—spanning key hydration regimes where DESs structure is progressively altered—we systematically quantify the effects of hydration on density, viscosity, electrical conductivity, thermal conductivity, and refractive index over a wide temperature range. Results demonstrate that water addition leads to a dramatic reduction in viscosity, particularly for bio-derived HBDs, enhancing processability and enabling practical applications. The ChCl:citric acid DESs maintains high structural cohesion upon hydration, reflected in persistent cooperative dynamics and high activation energy, whereas the synthetic ethylene glycol system exhibits predictable, tunable behavior, ideal for engineered fluid systems. Electrical conductivity increases non-linearly with water content, accompanied by a transition from fragile to strong liquid behavior. Derived parameters—molecular volume, thermal expansion coefficient, and excess molar volumes—reveal non-ideal mixing behavior and structural reorganization. Our findings define structure–property correlations critical for optimizing DESs formulations, offering a foundation for application-specific solvent engineering in energy, electrochemistry, and separation technologies. Sat, 01 Nov 2025 00:00:00 GMT https://hdl.handle.net/10259/11437 2025-11-01T00:00:00Z