By calcinating commercial silica gel at 1500℃or adding Na2C2O4 and then calcinating at 850℃,α cristobalite was formed.On the basis of the vibration spectroscopy of silica support,Na W Mn/SiO2 catalyst was character...By calcinating commercial silica gel at 1500℃or adding Na2C2O4 and then calcinating at 850℃,α cristobalite was formed.On the basis of the vibration spectroscopy of silica support,Na W Mn/SiO2 catalyst was characterized by Raman spectroscopy.The results show that the structure of support and the interaction among metal components have significant effect on the dispersion and the structure of metal sites,and the tetrahedrally coordinated formed on α cristobalite surface is the most possible site of methane activation with high C2 selectivity.展开更多
The effects of operating parameters on oxidative coupling of methane （OCM） over Na-W-Mn/SiO2 catalyst have been studied at elevated pressures of 0.2, 0.3 and 0.4 MPa under low gaseous hourly space velocity （GHSV） ...The effects of operating parameters on oxidative coupling of methane （OCM） over Na-W-Mn/SiO2 catalyst have been studied at elevated pressures of 0.2, 0.3 and 0.4 MPa under low gaseous hourly space velocity （GHSV） and low temperature conditions. Experimental results show that when the operating pressure is increased, C2＋ yield slightly decreases, while the maximum ratio of ethylene to ethane remains unchanged. Moreover, it has been found empirically that increase of pressure does not affect the catalyst behavior permanently, the catalyst recovers its original low pressure performance without hysteresis behavior by reducing the pressure. Under the investigated conditions, when oxygen is completely consumed, the increase of GHSV leads to improvement in C2 selectivity, while C3＋ and COx selectivities decrease slightly. The C2＋ selectivity increases by increase of nitrogen diluent in the feed, but the C3＋ hydrocarbons selectivities decrease with increase of nitrogen since it is possible that further dilution at high pressure may reduce the probability of collision between CH3 and C2＋ hydrocarbons. During the stability test at high pressure, the catalyst performance remains unchanged throughout the 20 h running. The fresh and used catalysts were characterized using XRD, SEM and N2 adsorption-desorption methods. It was found that the phase transformation of the support from α-cristobalite to tridymite and quartz does not have obvious effect on catalyst performance at high pressure.展开更多
Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the be...Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the best catalytic performance among all samples. In addition, the effects of different addition sequences of Na, W, Mn, Zr, S and P on the catalytic performance were studied. The absence of Na before the addition of Mn and Zr in the catalysts preparation depressed the formation of the active phases of Mn2O3 and ZrO2 and decreased the activities of the catalysts significantly.展开更多
文摘By calcinating commercial silica gel at 1500℃or adding Na2C2O4 and then calcinating at 850℃,α cristobalite was formed.On the basis of the vibration spectroscopy of silica support,Na W Mn/SiO2 catalyst was characterized by Raman spectroscopy.The results show that the structure of support and the interaction among metal components have significant effect on the dispersion and the structure of metal sites,and the tetrahedrally coordinated formed on α cristobalite surface is the most possible site of methane activation with high C2 selectivity.
文摘The effects of operating parameters on oxidative coupling of methane （OCM） over Na-W-Mn/SiO2 catalyst have been studied at elevated pressures of 0.2, 0.3 and 0.4 MPa under low gaseous hourly space velocity （GHSV） and low temperature conditions. Experimental results show that when the operating pressure is increased, C2＋ yield slightly decreases, while the maximum ratio of ethylene to ethane remains unchanged. Moreover, it has been found empirically that increase of pressure does not affect the catalyst behavior permanently, the catalyst recovers its original low pressure performance without hysteresis behavior by reducing the pressure. Under the investigated conditions, when oxygen is completely consumed, the increase of GHSV leads to improvement in C2 selectivity, while C3＋ and COx selectivities decrease slightly. The C2＋ selectivity increases by increase of nitrogen diluent in the feed, but the C3＋ hydrocarbons selectivities decrease with increase of nitrogen since it is possible that further dilution at high pressure may reduce the probability of collision between CH3 and C2＋ hydrocarbons. During the stability test at high pressure, the catalyst performance remains unchanged throughout the 20 h running. The fresh and used catalysts were characterized using XRD, SEM and N2 adsorption-desorption methods. It was found that the phase transformation of the support from α-cristobalite to tridymite and quartz does not have obvious effect on catalyst performance at high pressure.
基金supported by the financial support from National Natural Science Foundation of China (20676116)
文摘Na-W-Mn-Zr-S-P/SiO2 catalysts for oxidative coupling of methane （OCM） were prepared by incipient wetness impregnation, sol-gel and mixture slurry methods. The catalyst prepared by mixture slurry method showed the best catalytic performance among all samples. In addition, the effects of different addition sequences of Na, W, Mn, Zr, S and P on the catalytic performance were studied. The absence of Na before the addition of Mn and Zr in the catalysts preparation depressed the formation of the active phases of Mn2O3 and ZrO2 and decreased the activities of the catalysts significantly.
