Highly efficient deep desulfurization of fuels by meso/macroporous H3PW12O40/TiO2 at room temperature

[Display omitted] •A new kind of meso/macroporous structured HPW/TiO2 catalyst was prepared by monodispersed polystyrene spheres and quaternary ammonium bromide.•Quaternary ammonium bromide with longer alkyl chains length (STAB) was found to be the best mesostructure-directing agent in the synthesis...

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Veröffentlicht in:Materials research bulletin 2018-09, Vol.105, p.210-219
Hauptverfasser: Yue, Du, Jiaheng, Lei, Lina, Zhou, ran, Guo Zhen, Xiaodi, Du, Junsheng, Li
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Sprache:eng
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Zusammenfassung:[Display omitted] •A new kind of meso/macroporous structured HPW/TiO2 catalyst was prepared by monodispersed polystyrene spheres and quaternary ammonium bromide.•Quaternary ammonium bromide with longer alkyl chains length (STAB) was found to be the best mesostructure-directing agent in the synthesis of meso/macroporous HPW/TiO2 catalyst.•The influence of dosage of macroporous templates (monodispersed polystyrene spheres) and alkyl chains length of quaternary ammonium bromide on the textural of meso/macroporous HPW/TiO2 catalyst were investigated.•With proper PS spheres and quaternary ammonium bromide usage, disordered macropores arranged periodicity and led relatively larger pore size and pore volume.•The meso/macroporous HPW/TiO2 materials exhibited enhanced excellent desulfurization performance of thiophenic sulfur in model fuel than other samples. Dibenzothiophene can be completely removed within 2 h at 30 °C. This paper described the synthesis of meso/macroporous phosphotungstic acid (HPW) /TiO2 catalyst with quaternary ammonium bromide and monodispersed polystyrene spheres (PS) as dual-template. The synthetic parameters, such as concentration of the templates and the alky chain length of quaternary ammonium bromide was studied carefully and optimized to generate catalyst with regulated porous features. The chemical properties of the catalyst was also investigated, X-ray diffraction (XRD) and Fourier transform infrared (FT-IR) measurements confirmed the Keggin-type HPW were highly dispersed on the TiO2 framework. The optimal meso/macroporous HPW/TiO2 catalyst exhibited excellent catalytic activity in the oxidation of refractory sulphur compounds such as benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT). DBT was removed within 2 h at 30 °C under selected reaction conditions and the apparent activation energy for DBT oxidation was calculated to be 45.7 kJ/mol. The high ODS reaction rate of catalyst could be attributed to the combination of unique meso/macroporous architecture allowing for efficient mass transport of reactants and products in pore channel and its high surface area, large mesoporous size, and pore volume enabling sufficient exposure of catalytic active sites. Moreover, the meso/macroporous HPW/TiO2 catalyst also exhibited excellent reusability with no obviously degradation even after eight cycles.
ISSN:0025-5408
1873-4227
DOI:10.1016/j.materresbull.2018.04.048