Felycia Edi-Soetaredjo, Marwa Slama, Lotfi Sellaoui, Houcine Ghalla, Mounir Ben El Hadj Rhouma, Suryadi Ismadji, Barbara Ernst, Adrian Bonilla-Petriciolet, Abdelmottaleb Ben Lamine
The adsorption of amoxicillin (AMX) and doripenem (DRPNM) on copper benzene-1,3,5-tricarboxylate (HKUST-1) in single and binary systems is analyzed in this paper. The experimental results showed that the adsorption capacities of this MOF for the removal of these pharmaceuticals reduced from single to binary solutions. A monolayer adsorption model and its extended competitive version were successfully applied to analyze the adsorption data. The modeling results showed that the reduction of AMX and DRPNM adsorption capacities was explained by a competitive effect of these adsorbates generating an antagonistic behavior for both molecules where the same adsorption site was involved during their removal. The statistical physics model was also utilized to estimate the AMX and DRPNM adsorption orientation on the HKUST-1 surface. Adsorption energies were calculated confirming an exothermic removal process for both molecules and DFT simulations allowed to determine the role of hydrogen bonding in the adsorption mechanism. It was concluded that the interactions for the adsorption of DRPNM on this MOF were higher than those for AMX removal. Particularly, the oxygens linked to the cupper ions on MOFs structure played a crucial role during the adsorption mechanisms of these organic compounds. Overall, this paper presents a combination between experiment results and two different theoretical approaches to provide a new explanation of the mechanism of adsorption of two relevant antibiotics on HKUST-1 MOF. © 2023 Elsevier B.V.
Department of Chemical Engineering, Widya Mandala Surabaya Catholic University, Kalijudan 37, Surabaya, 60114, Indonesia; Collaborative Research Center for Zero Waste and Sustainability, Jl. Kalijudan 37, East Java, Surabaya, 60114, Indonesia; Université de Monastir, Institut Préparatoire aux Études des Ingénieurs de Monastir, Laboratoire d’Études des Milieux Ionisés et Réactifs (EMIR), Monastir, 5000, Tunisia; CRMN, Centre for Research on Microelectronics and Nanotechnology of Sousse, NANOMISENE, LR16CRMN01, Code Postal 4054, Sousse, Tunisia; Laboratory of Quantum and Statistical Physics, LR18ES18, Monastir University, Faculty of Sciences of Monastir, Tunisia; Université de Strasbourg, CNRS, IPHC, UMR 7178, Laboratoire de Reconnaissance et Procédés de Séparation Moléculaire (RePSeM), ECPM 25 rue Becquerel, Strasbourg, F-67000, France; Instituto Tecnológico de Aguascalientes, Aguascalientes, 20256, Mexico