2026-05-28T15:33:30Zhttps://riubu.ubu.es/oai/request

oai:riubu.ubu.es:10259/117172026-05-27T00:05:17Zcom_10259_9476com_10259.4_106com_10259_2604col_10259_9477

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 CO2 capture Flue gas Deep eutectic solvents Thin films Graphene Quantum chemistry Molecular dynamics Química cuántica Quantum chemistry 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 This work was funded by the European Union (873005-WORLD-H2020-MSCA-RISE-2019). We also acknowledge SCAYLE (Supercomputación Castilla y León, Spain) and COMPUTAEX (Supercomputación Extremadura, Spain) for providing supercomputing facilities. The statements made herein are solely the responsibility of the authors 2026-05-26T06:24:44Z 2026-05-26T06:24:44Z 2026-01 info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion 2452-2627 https://hdl.handle.net/10259/11717 10.1016/j.flatc.2026.100995 eng FlatChem. 2026, V. 55, 100995 https://doi.org/10.1016/j.flatc.2026.100995 Attribution-NonCommercial-NoDerivatives 4.0 Internacional http://creativecommons.org/licenses/by-nc-nd/4.0/ info:eu-repo/semantics/openAccess application/pdf Elsevier