Catalytic Combustion of Methane over High Copper-Loading ZSM-5 Catalysts

来源 :Journal of Natural Gas Chemistry | 被引量 : 0次 | 上传用户:luckymanjxj
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Two series of Cu/ZSM-5 catalysts,loading from 5 to 20 wt% CuO,were prepared by the deposition-precipitation and impregnation methods,respectively.The catalysts prepared by the impreg- nation method showed better catalytic performances than those prepared by the deposition-precipitation method and the increase of copper loading favored methane conversion.20Cu(I)/ZSM-5 had the highest activity with T_(90%)of 746 K,and for 20Cu(D)/ZSM-5,T_(90%)was as high as 804 K.The characteriza- tion of X-ray diffraction(XRD),temperature-programmed reduction(TPR),temperature-programmed desorption(TPD),and X-ray photoelectron spectroscopy(XPS)revealed that the dispersion of cop- per species could be improved by using the deposition-precipitation method instead of the impregnation method,but the fraction of surface CuO,corresponding to active sites for methane oxidation,was larger on 20Cu(I)/ZSM-5 than 20Cu(D)/ZSM-5.The results of Pyridine-Fourier transform infrared spectrum (Py-FT-IR)showed that a majority of Lewis acidity and a minority of Brφnsted acidity were present on Cu/ZSM-5 catalysts.20Cu(I)/ZSM-5 presented more Lewis acid sites.The number of Lewis acid sites changed significantly with preadsorption of oxygen.Adsorption of methane and oxygen on acid sites was observed.The properties of Cu/ZSM-5 catalysts were correlated with the activity for methane oxidation. Two series of Cu / ZSM-5 catalysts, loading from 5 to 20 wt% CuO, were prepared by the deposition-precipitation and impregnation methods, respectively. These catalysts prepared by the imprega- nation method showed better catalytic performances than those prepared by the deposition-precipitation method and the increase of copper loading favored methane conversion. 20Cu (I) / ZSM-5 had the highest activity with T_ (90%) of 746 K, and for 20 Cu (D) / ZSM- %) was as high as 804 K. The characteriza- tion of X-ray diffraction (XRD), temperature-programmed reduction (TPR), temperature- programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS) revealed that the dispersion of cop-per species could be improved by using the deposition-precipitation method instead of the impregnation method, but the fraction of surface CuO, corresponding to active sites for methane oxidation, was larger on 20 Cu (I) / ZSM-5 than 20 Cu (D) /ZSM-5.The results of Pyridine-Fourier transform infrared spectrum (Py-FT-IR) showed that a major ity of Lewis acidity and a minority of Brφnsted acidity were present on Cu / ZSM-5 catalysts.20Cu (I) / ZSM-5 presented more Lewis acid sites. The number of Lewis acid sites changed significantly with preadsorption of oxygen. Adsorption of methane and oxygen on acid sites was observed. The properties of Cu / ZSM-5 catalysts were correlated with the activity for methane oxidation.
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