Yan Gao,Ziyan Lv,Ruimin Gao,Gai Zhang,Ying Zheng,Jianshe Zhao
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-Mo 16 V 2 possesses superior catalytic activity, with a desulfurization efficiency of up to 98.30%. In addition, CNTs@MOF-199-Mo 16 V 2 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.
Yan Gao,Zhe Liu,Guangfa Hu,Ruimin Gao,Jianshe Zhao
The supported catalysts of Mo 16 V 2 loaded with CNTs@MOF-199 are produced via three means including microwave method (CNTs@MOF-199-Mo 16 V 2 (M)), one-pot method (CNTs@MOF-199-Mo 16 V 2 (O)) and impregnation method (CNTs@MOF-199-Mo 16 V 2 (I)), respectively. The structure of the target materials is characterized by means of several analysis methods, and the effect of catalyst on removal of thiophene is investigated with the molecular oxygen as oxidant and the dimethyl formamide (DMF) as extraction solvent . The reaction conditions including catalyst dosage, reaction temperature, oxygen quantity and stirring speed are investigated. The experiment result shows that the catalyst synthesized by one-pot method has the best performance, and the efficiency can reach 100% under the optimum conditions. On the basis of kinetic study , thiophene oxidation shows the kinetic characteristic of a first order reaction, and then rate constant and activation energy were obtained. In addition, response surface design (RSD) is designed and applied to verify the optimum reaction conditions.
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