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Homogeneous Oxidative Desulfurization Catalyzed by the Recoverable Reaction-controlled Phase Transfer Catalyst based on Trilacunary Keggin Polyoxometallate

Abstract

A phosphotungstic reaction-controlled phase transfer catalyst [C7H7(CH3)3N]9PW9O34 (Q9PW9) with trilacunary Keggin structure was successfully synthesized and characterized by powder X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR) and Thermo-gravimetry analysis (TG). This catalyst showed high activity for removing the most refractory sulfur compounds such as dibenzothiophene (DBT), benzothiophene (BT) , thiophene (TH) and 4,6-dimethyldibenzothiophene (4,6-DMDBT) in oxidative desulfurization process. Nearly 100 % DBT removal rate was achieved under optimal conditions which were temperature: 60 ◦C; catalyst dosage: 0.2015g; O/S molar ratio: 10; pre-immersion time of catalyst in H2O2: 10 min. And the catalyst could be easily separated from the oxidative desulfurization system at the end of the reaction when H2O2 was consumed. The IR and TG analysis to the recycled catlayst indicated that the structure of the polyoxometalate anion could be retained intactly after reuse. Catalyst Q9PW9 could be recycled for three consecutive ODS cycles with only a slight decrease of desulfurization efficiency. Moreover, very positive desulfurization result was achieved in the oxidative desulfurization for actual diesel catalyzed by Q9PW9. Finally, according to the discussion of the experimental and analytical data, a mechanism was proposed for the oxidation process of DBT.

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Publication details

The article was received on 01 Jan 2019, accepted on 10 Apr 2019 and first published on 10 Apr 2019


Article type: Paper
DOI: 10.1039/C9NJ00002J
Citation: New J. Chem., 2019, Accepted Manuscript

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    Homogeneous Oxidative Desulfurization Catalyzed by the Recoverable Reaction-controlled Phase Transfer Catalyst based on Trilacunary Keggin Polyoxometallate

    J. Ding, Y. Zhang and R. Wang, New J. Chem., 2019, Accepted Manuscript , DOI: 10.1039/C9NJ00002J

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