Water contamination with dyes and pharmaceuticals is a major threat to ecological and human well-being. This study highlights the importance of using molecular simulations in designing and predicting the performance of novel adsorbents for wastewater treatment. The research explores the potential of biodegradable polymers like Pectin (PE) and oxidized Chitosan (OCN) in functionalizing a metal-organic framework (MOF) known as UO-66 (Zr) (UO). By incorporating these functional groups, the study aims to improve the adsorption efficiency of UO towards rhodamine B (RHOB, a dye pollutant) and Losartan (LOSA, a pharmaceutical pollutant). Firstly, density functional theory (DFT) calculations were employed to inspect the structures of both pollutants and the modified adsorbents. Subsequently, the research investigated the adsorbents’ various physicochemical characteristics, including fractional free volume, glass transition temperature, and mechanical properties. Finally, molecular dynamics (MD) and Monte Carlo (MC) simulations were accomplished to evaluate the adsorption behaviour of the pollutants on various UO forms (pristine, PE-functionalized, and OCN-functionalized). The study found that all adsorbents showed strong adsorption capabilities, with adsorption energies ranging from −3500 to −4500 kcal/mol for RHOB and −1500 to −2600 kcal/mol for LOSA. Moreover, The drug rejection rate of RHOB for neat is 50 % but increases to 80 % and 90 % with the addition of PE and OCN, respectively, showing their synergistic effect. Similarly, the accumulation rate rises from 6 Å (NH2/UO) to 10 Å (OCN/UO) and 11 Å (PE/UO). For LOSA, the drug rejection rate improves from 30 % to 60 %, while the accumulation rate increases from 4 Å to 8 Å with PE and OCN functionalization. The results demonstrated that functionalizing UO with the chosen biodegradable polymers enhanced its adsorption capacity for both pollutants compared to the pristine form. Notably, the developed adsorbent exhibited a higher affinity towards RHOB dye compared to LOSA pharmaceutical.
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