Heteropolyacids supported on macroporous materials POM@MOF-199@LZSM-5: Highly catalytic performance in oxidative desulfurization of fuel oil with oxygen

• Published in: Fuel (Guildford) Vol. 221; pp. 1 - 11
• Main Authors: Li, Si-Wen, Gao, Rui-Min, Zhang, Wei, Zhang, Yuan, Zhao, Jian-she
• Format: Journal Article
• Language: English
• Published: Kidlington Elsevier Ltd 01.06.2018; Elsevier BV
• Subjects: Catalysis; Catalysts; Desulfurization; Desulfurizing; Diffraction; Fourier transforms; Fuel oils; Infrared spectroscopy; Keggin-type POM; Macropore LZSM-5; Metal-organic frameworks; Optimization; Organic compounds; Oxidation; Oxidative desulfurization; Petroleum; Photoelectron spectroscopy; Porous materials; Response surface method; Response surface methodology; Reusability; Scanning electron microscopy; Transmission electron microscopy; X ray photoelectron spectroscopy; X-ray diffraction; Oxidative desulfurization; Macropore LZSM-5; Keggin-type POM; Reusability; Response surface method
• ISSN: 0016-2361; 1873-7153
• DOI: 10.1016/j.fuel.2017.12.093

[Display omitted] •Keggin heteropolyacid was successfully supported in the macroporous LZSM-5.•The macroporous LZSM-5 favors to the diffusion of the DBT reactant molecules.•Catalytic behavior of samples for oxidation of DBT was investigated.•The response surface method was used to optimize the DBT removal process.•The catalyst can be easily recovered and reused. A highly active catalyst Keggin type POM-based inorganic-organic compound POM@MOF-199@LZSM-5(PMZ) has been prepared and applied in the catalytic oxidative desulfurization system. Structure and properties of catalyst were characterized by X-ray diffraction (XRD), Fourier transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), N2 adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM) and so on. The catalyst gave high desulfurization activity in the removal of DBT using O2 as the oxidant. Under the optimal conditions, the conversion rate reached 100% only in 120 min. The kinetic studies revealed that the oxidative desulfurization can present a pseudo first-order kinetic process and the apparent activation energy was 30.5 kJ/mol. The response surface method also used to optimize the process of oxidative desulfurization. There was little change for the oxidative desulfurization efficiency after 10 recycle times. This enhanced catalytic performance could be attributed to the more filled active species, POM, in the larger porous materials and the good protection measures of dual-function porous material supports.