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Τετάρτη 21 Δεκεμβρίου 2016

Co-modified MCM-41 as an effective adsorbent for levofloxacin removal from aqueous solution: optimization of process parameters, isotherm, and thermodynamic studies

Abstract

Antibiotics are emerging contaminants due to their potential risks to human health and ecosystems. Poor biodegradability makes it necessary to develop effective physical-chemical methods to eliminate these contaminants from water. The cobalt-modified MCM-41 was prepared by a one-pot hydrothermal method and characterized by SAXRD, N2 adsorption-desorption, SEM, UV–Vis DR, and FTIR spectroscopy. The results revealed that the prepared 3% Co-MCM-41 possessed mesoporous structure with BET surface areas at around 898.5 m2g−1. The adsorption performance of 3% Co-MCM-41 toward levofloxacin (LVF) was investigated by batch experiments. The adsorption of LVF on 3% Co-MCM-41 was very fast and reached equilibrium within 2 h. The adsorption kinetics followed the pseudo-second-order kinetic model with the second-order rate constants in the range of 0.00198–0.00391 g mg−1 min−1. The adsorption isotherms could be well represented by the Langmuir, Freundlich, and Dubinin-Radushkevich (D-R) isotherm equations. Nevertheless, D-R isotherm provided the best fit based on the coefficient of determination and average relative error values. The mean free energy of adsorption (E) calculated from D-R model was about 11 kJ mol−1, indicating that the adsorption was mainly governed by a chemisorption process. Moreover, the adsorption capacity was investigated as a function of pH, adsorbent dosage, LVF concentration, and temperature with help of respond surface methodology (RSM). A quadratic model was established, and an optimal condition was obtained as follows: pH 8.5, adsorbent dosage of 1 g L−1, initial LVF concentration of 119.8 mg L−1, and temperature of 31.6 °C. Under the optimal condition, the adsorption capacity of 3% Co-MCM-41 to LVF could reach about 108.1 mg g−1. The solution pH, adsorbent dosage, LVF concentration, and a combination of adsorbent dose and LVF concentration were significant factors affecting the adsorption process. The adsorption thermodynamic functions were also determined. The negative ΔH 0 (−33.50 kJ mol−1) and ΔS 0 (−43.57 J mol−1 K−1) suggested that the adsorption was an exothermic process accompanied by decreasing disorder. This study may indicate that 3% Co-MCM-41 is a promising adsorbent for removing emerging pollutants of LVF from water.



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