Abstract
Supported ionic liquid (IL) catalysts [Cnmim]3PMo12O40/Am TiO2 (amorphous TiO2) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization (ECODS) system. Characterizations such as FTIR, DRS, wide-angle XRD, N2 adsorption–desorption and XPS were applied to analyze the morphology and Keggin structure of the catalysts. In ECODS with hydrogen peroxide as the oxidant, it was found that ILs with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene. The desulfurization could reach 100% under optimal conditions, and GC–MS analysis was employed to detect the oxidized product after the reaction. Factors affecting the desulfurization efficiencies were discussed, and a possible mechanism was proposed. In addition, cyclic experiments were also conducted to investigate the recyclability of the supported catalyst. The catalytic activity of [C16mim]3PMo12O40/Am TiO2 only dropped from 100% to 92.9% after ten cycles, demonstrating the good recycling performance of the catalyst and its potential industrial application.
Highlights
Nowadays, environmental problems due to the annually increasing emission of sulfur oxides (SOx) have aroused worldwide attention (Piccinino et al 2017; Zeng et al 2017)
In extraction coupled catalytic oxidative desulfurization (ECODS) with hydrogen peroxide as the oxidant, it was found that ionic liquid (IL) with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene
The exact sulfur compound of model oil after the reaction was determined by Gas chromatography–mass spectrometry (GC–MS) with a flame ionization detector (FID), using n-tetradecane as an internal standard
Summary
Environmental problems due to the annually increasing emission of sulfur oxides (SOx) have aroused worldwide attention (Piccinino et al 2017; Zeng et al 2017). The dispersion and catalytic activity of the catalyst are significantly affected by the characteristics of the carrier during the sulfur removal process. These include hydrophilic or hydrophobic properties, hole parameters, structure and composition. It is well known that polyoxometalates have good catalytic activity (Yao et al 2016; Zhang et al 2016; Gao et al 2018) According to structure, they can be categorized as Keggin, Dawson, Anderson, Waugh or Silverton types and so on (Alsalme et al 2016). In this work, supported IL catalysts [Cnmim]3PMo12O40/Am TiO2 (n = 4, 8, 16) with Keggin structure were prepared and investigated in ECODS. [C16mim]3PMo12O40/Am TiO2 has the optimal desulfurization rate and recycling performance in heterogeneous reaction
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