Oxidative desulfurization process of model fuel under molecular oxygen by polyoxometalate loaded in hybrid material CNTs@MOF-199 as catalyst

Abstract

Fuel desulfurization as a crucial subject has aroused people's attention with the environmental problems becoming more and more important. Oxidative desulfurization (ODS) is one of the most promising methods due to its high efficiency, low cost, easy operation and mild reaction condition. With the loading of polyoxometalate (POM), a hybrid material (CNTs@MOF-199) supported catalysts (CNTs@MOF-199-POM) are designed and prepared using one-pot procedure. The novel catalysts are investigated by FT-IR, XRD, XPS, SEM and BET. Factors affecting the desulfurization, such as catalyst dosage, loading amount of POM, reaction temperature, agitation rate and reaction time, are evaluated, and the optimum reaction conditions are determined. The test results indicate that the catalyst CNTs@MOF-199-Mo16V2 possesses superior catalytic activity, with a desulfurization efficiency of up to 98.30%. In addition, CNTs@MOF-199-Mo16V2 exhibits an excellent reusability, and the catalytic efficiency is only slightly reduced after recycling for 7 times. Besides, the kinetic studies indicate that the desulfurization process belongs to apparent first-order kinetic reaction. And the apparent activation energy is 12.89 kJ/mol.