Abstract
A core-shell Cu-benzene-1,3,5-tricarboxylic acid (Cu-BTC)@TiO2 was successfully synthesized for photocatalysis-assisted adsorptive desulfurization to improve adsorptive desulfurization (ADS) performance. Under ultraviolet (UV) light irradiation, the TiO2 shell on the surface of Cu-BTC achieved photocatalytic oxidation of thiophenic S-compounds, and the Cu-BTC core adsorbed the oxidation products (sulfoxides and sulfones). The photocatalyst and adsorbent were combined using a distinct core-shell structure. The morphology and structure of the fabricated Cu-BTC@TiO2 microspheres were verified by scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive x-ray spectroscopy, X-ray powder diffraction, nitrogen adsorption-desorption and X-ray photoelectron spectroscopy analyses. A potential formation mechanism of Cu-BTC@TiO2 is proposed based on complementary experiments. The sulfur removal efficiency of the microspheres was evaluated by selective adsorption of benzothiophene (BT) and dibenzothiophene (DBT) from a model fuel with a sulfur concentration of 1000 ppmw. Within a reaction time of 20 min, the BT and DBT conversion reached 86% and 95%, respectively, and achieved ADS capacities of 63.76 and 59.39 mg/g, respectively. The BT conversion and DBT conversion obtained using Cu-BTC@TiO2 was 6.5 and 4.6 times higher, respectively, than that obtained using Cu-BTC. A desulfurization mechanism was proposed, the interaction between thiophenic sulfur compounds and Cu-BTC@TiO2 microspheres was discussed, and the kinetic behavior was analyzed.
Highlights
Sulfur compounds in fuel oils present a major air pollution problem because of the sulfur oxide content (SOx, x = 2, 3) in the exhausted gasses
Field-emission scanning electron microscopy (FESEM), and HRTEM images revealed the jagged surface of the microspheres, which suggested the formation of an external layer by the adhesion of small TiO2 particles
Brunauer Emmett Teller (BET) showed that Cu-BTC and Cu-BTC@TiO2 obtained large increases in surface area and significant reductions in the average pore diameter
Summary
Sulfur compounds in fuel oils present a major air pollution problem because of the sulfur oxide content (SOx, x = 2, 3) in the exhausted gasses. These oxides contribute to acid rain and acid smog, and they are harmful to human health [1]. DBT alkyl derivatives such as 4,6-dimethyldibenzothiophene (4,6-DMDBT) under normal operating conditions [3,4,5] Oxidation of these compounds can occur under even the most mildly reactive conditions [6], but the organosulfur compounds, oxidation products and solvent seems to be separated not
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