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| Heteropoly Acid Grafted-MOFs Functionalized Magnetic Composite Material for Catalytic Oxidative Desulfurization |
| Author Name | Affiliation | E-mail | | ZHANG Han | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | WANG Jun-Er | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | DONG Hao | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | YANG Ni-Ni | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | PAN Lin-Yun | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | SHEN Hao-Yu | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | hyshen@nit.zju.edu.cn | | HU Mei-Qin | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | | | CHENG Jin-Jin | Zhejiang University Ningbo Institute of Technology, Ningbo, Zhejiang 315100, China | |
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| Abstract: Carboxylated magnetic microsphere Fe3O4-COOH was firstly synthesized by solvothermal method. MIL-101(Cr) functionalized magnetic composite Fe3O4-COOH@MIL-101(Cr) was obtained next by one-pot method. Phosphotungstic acid was finally grafted on the Fe3O4-COOH@MIL-101(Cr) by ultrasonic impregnation method to obtain HPW@Fe3O4-COOH@MIL-101(Cr). Its composition and morphology were characterized by Fourier transform infrared spectrum (FT-IR), X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), Vibrating sample magnetometer (VSM), transmission electron microscopy (TEM) and scanning electron microscopy (SEM). It was used as catalyst with hydrogen peroxide as oxidant to catalyze the oxidation of n-octane simulated oil sample with dibenzothiophene as sulfur source. The effects of ultrasonic reaction time, oxidant dosage, reaction temperature, dosage of the phase transfer agent and the catalyst amount on the desulfurization rate were investigated by using single factor method. The presumed mechanism was discussed. The results showed that the optimized catalytic degradation rate reached when the reaction time was at 60℃, 5 mins, nH2O2/nS of 4, usage amount of the phase transfer agent CTAB at 0.2%(w/w), with the catalyst amount of 8 g·L-1. The catalytic degradation rate reached 73.15%. After used for 5 times, the catalytic degradation rate decreased by 7.8%, indicating that the material has good catalytic desulfurization performance and can be reused. Primary mechanism study showed that the active center for the catalytic desulfurization might be the heteropoly acid anion of the HPW@Fe3O4-COOH@MIL-101(Cr), in which the Fe3O4-COOH@MIL-101(Cr) may act as a supporter and cooperative absorbent. |
| Keywords: heteropoly acid MOFs functionalized magnetic composite material oxidative desulfurization phase transfer agent |
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| ZHANG Han,WANG Jun-Er,DONG Hao,YANG Ni-Ni,PAN Lin-Yun,SHEN Hao-Yu,HU Mei-Qin,CHENG Jin-Jin.Heteropoly Acid Grafted-MOFs Functionalized Magnetic Composite Material for Catalytic Oxidative Desulfurization[J].Chinese Journal of Inorganic Chemistry,2020,36(8):1475-1484. |
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