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Iron and molybdenum mixed oxide supported on Al-PILC for the catalytic oxidative desulfurization of dibenzothiophene in simulated diesel fuel

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Abstract

In this work, three novel catalysts were prepared by 2.5, 5.0, and 10.0 wt.% facile impregnation with an iron and molybdenum mixed oxide (Fe/Mo) on an aluminum pillared clay (Al-PILC) support. These materials were characterized by scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS), X-ray diffraction (XRD), temperature programed reduction (TPR), and nitrogen (N2) physisorption at 77 K. Characterizations indicated that the metal particles were dispersed on the surface of the three catalysts, and the interlayer d001 spacing of the pillared material remained unchanged after the impregnation process. The catalytic tests showed good results for DBT oxidation using the synthesized catalysts, with high turnover frequency (TOF) values, particularly for the material with 5.0 wt.% Fe/Mo. Theoretical calculations were carried out at the density functional theory (DFT) level, to investigate how the DBT molecules were adsorbed onto the surface of the mixed oxide. The lowest energy proposal was obtained when both Fe and Mo were present at the active sites, indicating a possible synergistic effect of the metals on catalyst activity. Reuse tests indicated that the catalysts could be employed effectively for up to 3 cycles in a row, then a decrease in activity occurred and the active sites needed to be regenerated.

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Funding

This work was supported by the National Counsel of Technological and Scientific Development (CNPQ) and the Higher Education Co-ordination Agency (CAPES).

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Correspondence to Aline Auxiliadora Tireli or Iara do Rosário Guimarães.

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Tireli, A.A., do Rosário Guimarães, I., Mello Mattos de Castro, G. et al. Iron and molybdenum mixed oxide supported on Al-PILC for the catalytic oxidative desulfurization of dibenzothiophene in simulated diesel fuel. Environ Sci Pollut Res (2020). https://doi.org/10.1007/s11356-020-07961-8

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Keywords

  • Mixed oxide
  • DBT
  • Oxidation
  • Pillared clay
  • DFT calculations