A series of Ce-promoted Mn-Na2WO4/SiO2 catalysts were prepared by incipient wetness impregnation method, and their catalytic performance for oxidative coupling of methane （OCM） was investigated at atmospheric pressu...A series of Ce-promoted Mn-Na2WO4/SiO2 catalysts were prepared by incipient wetness impregnation method, and their catalytic performance for oxidative coupling of methane （OCM） was investigated at atmospheric pressure in a micro-quartz-tube reactor. The catalysts were characterized by X-ray diffraction （XRD）, temperature program reduction （TPR） and BET surface area. Ce promoter increased surface area and Na2WO4 species dispersion, which enriched the amount of the surface species. In addition, Ce promoter increased the Na/W species reduction, but the reduction peak shifted to higher temperature. Stability test of 5wt%Ce catalyst indicated suitable performance and stability. The selectivity and yield of C^2＋ hydrocarbons after 50 h operation reached 65.5% and 19.6%, respectively, at 840 ℃ over 5wt%Ce-2wt%Mn5wt%Na2WO4/SiO2 catalyst.展开更多
In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation meth...In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.展开更多
In the preparation of this precursor tetraethlortho silicate (TEOS), sodium tungstate, ethyl alcohol, HCl and RECl3(RE=Eu,Tb) were mixed and then heated at 800 ℃ for 2 h, leading to a luminescent compound. The struct...In the preparation of this precursor tetraethlortho silicate (TEOS), sodium tungstate, ethyl alcohol, HCl and RECl3(RE=Eu,Tb) were mixed and then heated at 800 ℃ for 2 h, leading to a luminescent compound. The structure of the materials was characterized by TG-DTA and IR analysis, and the results indicate that the materials were in SiO2 network structure. Three-dimensional fluorescence spectra was used to characterize the luminescent properties of the materials. The luminescence property of doped and un-doped Eu3+or Tb3+ and Na2WO4 in silica materials were prepared and measured. The results show that good energy transfer from WO2-4 to Eu3+ ion, sensitized the luminescence intensity of Eu3+ remarkably. Tb3+ ion incorporated silica materials expressed the inverse energy transition from Tb3+ to WO2-4, however, we got the materials with homogeneous green blue fluorescent light. Finally, the energy transfer of WO2-4 and Eu3+, WO2-4 and Tb3+ were explained by energy levels diagram.展开更多
文摘A series of Ce-promoted Mn-Na2WO4/SiO2 catalysts were prepared by incipient wetness impregnation method, and their catalytic performance for oxidative coupling of methane （OCM） was investigated at atmospheric pressure in a micro-quartz-tube reactor. The catalysts were characterized by X-ray diffraction （XRD）, temperature program reduction （TPR） and BET surface area. Ce promoter increased surface area and Na2WO4 species dispersion, which enriched the amount of the surface species. In addition, Ce promoter increased the Na/W species reduction, but the reduction peak shifted to higher temperature. Stability test of 5wt%Ce catalyst indicated suitable performance and stability. The selectivity and yield of C^2＋ hydrocarbons after 50 h operation reached 65.5% and 19.6%, respectively, at 840 ℃ over 5wt%Ce-2wt%Mn5wt%Na2WO4/SiO2 catalyst.
基金support from the Ministry of Science and Technology (Nos.2012BAC20B10)the National Natural Science Foundation of China (Nos. 21321061 and 20976109)
文摘In this work,the influence of CO2 on the structural variation and catalytic performance of Na2WO4/Mn/Si O2 for oxidative coupling of methane to ethylene was investigated. The catalyst was prepared by impregnation method and characterized by XRD,Raman and XPS techniques. Appropriate amount of CO2 in the reactant gases enhanced the formation of surface tetrahedral Na2WO4 species and promoted the migration of O in MOx,Na,W from the catalyst bulk to surface,which were favorable for oxidative coupling of methane. When the molar ratio of CH4/O2/CO2 was 3/1/2,enriched surface tetrahedral Na2WO4 species and high surface concentration of O in MOx,Na,W were detected,and then high CH4 conversion of 33.1% and high C2H4 selectivity of 56.2% were obtained. With further increase of CO2 in the reagent gases,the content of active surface tetrahedral Na2WO4 species and surface concentration of O in MOx,Na,W decreased,while that of inactive species（Mn WO4 and Mn2O3） increased dramatically,leading to low CH4 conversion and low C2H4 selectivity. It could be speculated that Na2WO4 crystal was transformed into Mn WO4 crystal with excessive CO2 added under the reaction conditions. Pretreatment of Na2WO4/Mn/Si O2 catalyst by moderate amount of CO2 before OCM also promoted the formation of Na2WO4 species.
基金Project supported by State Natural Science Foundation (20161001)Natural Science Foundation of Inner Mongolia Autonomous Region Science Commission (200508010206)
文摘In the preparation of this precursor tetraethlortho silicate (TEOS), sodium tungstate, ethyl alcohol, HCl and RECl3(RE=Eu,Tb) were mixed and then heated at 800 ℃ for 2 h, leading to a luminescent compound. The structure of the materials was characterized by TG-DTA and IR analysis, and the results indicate that the materials were in SiO2 network structure. Three-dimensional fluorescence spectra was used to characterize the luminescent properties of the materials. The luminescence property of doped and un-doped Eu3+or Tb3+ and Na2WO4 in silica materials were prepared and measured. The results show that good energy transfer from WO2-4 to Eu3+ ion, sensitized the luminescence intensity of Eu3+ remarkably. Tb3+ ion incorporated silica materials expressed the inverse energy transition from Tb3+ to WO2-4, however, we got the materials with homogeneous green blue fluorescent light. Finally, the energy transfer of WO2-4 and Eu3+, WO2-4 and Tb3+ were explained by energy levels diagram.
