摘 要: | In order to study their synergistic catalytic effects in toluene degradation, CuMn_2O_4/HTS-1(HTS-1 was a titanium silicon molecular sieve), Cu_(0.7)Mn_2Y_(0.3)O_x/HTS-1 and Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1 catalysts were prepared by the impregnation method.The textural properties, redox properties and acidity of the catalysts were characterized by X-ray diffractometer(XRD),transmission electron microscopy(TEM), scanning electron microscopy(SEM), H_2 temperature-programmed reduction(H_2-TPR), X-ray photoelectron spectroscopy(XPS),frustrated total internal reflection(FT-IR), ammonium temperature-programmed desorption(NH_3-TPD) and pyridine adsorption internal reflection(Py-IR) measurements.The potential roles of Lewis acid sites(activating dioxygen) were discussed, and the experimental results indicated that the most efficient route for toluene degradation over Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1(toluene conversion rate of 90%(T99) = 295℃) was ascribed to regulation of the synergistic effects of redox properties(activating molecular toluene) and Lewis acid sites(activating dioxygen).The Mars–Van–Krevelen(MVK) model was adopted to describe the reaction process of toluene oxidation, which gave an in-depth view into the toluene degradation over CuMn_2O_4/HTS-1, Cu_(0.7)Mn_2Y_(0.3)O_x/HTS-1 and Cu_(0.7)Mn_2Ce_(0.3)O_x/HTS-1.In addition, the synergistic effects between redox properties and Lewis acid sites were studied in detail.
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