Process Optimization for Catalytic Oxidation of Dibenzothiophene over UiO-66-NH2 by Using a Response Surface Methodology.

Abstract

This research investigates the catalytic performance of a metal–organic framework (MOF) with a functionalized ligand—UiO-66-NH2—in the oxidative desulfurization of dibenzothiophene (DBT) in n-dodecane as a model fuel mixture (MFM). The solvothermally prepared catalyst was characterized by XRD, FTIR, 1H NMR, SEM, TGA, and MP-AES analyses. A response surface methodology was employed for the experiment design and variable optimization using central composite design (CCD). The effects of reaction conditions on DBT removal efficiency, including temperature (X1), oxidant agent over sulfur (O/S) mass ratio (X2), and catalyst over sulfur (C/S) mass ratio (X3), were assessed. Optimal process conditions for sulfur removal were obtained when the temperature, O/S mass ratio, and C/S mass ratio were 72.6 °C, 1.62 mg/mg, and 12.1 mg/mg, respectively. Under these conditions, 89.7% of DBT was removed from the reaction mixture with a composite desirability score of 0.938. From the results, the temperature has the most significant effect on the oxidative desulfurization reaction. The model F values gave evidence that the quadratic model was well-fitted. The reusability of the MOF catalyst in the ODS reaction was tested and demonstrated a gradual loss of activity over four runs.