Partial oxidation of methane to formaldehyde and methanol was studied at atmospheric pressure in the temperature range of 700-750 °C using heteropolycompound catalysts （NH4）6HSiMo11FeO40, （NH4）4PMo11FeO39, an...Partial oxidation of methane to formaldehyde and methanol was studied at atmospheric pressure in the temperature range of 700-750 °C using heteropolycompound catalysts （NH4）6HSiMo11FeO40, （NH4）4PMo11FeO39, and H4PMo11VO40, which were prepared and characterized by various analysis techniques such as infrared, visible UV, XRD and DTA. O2 or N2O was used as the oxidizing agent, and the principal products of the reaction were CH3OH, CH2O, CO, CO2, and water. The conversion and the selectivity of products depend strongly on the reaction temperature, the nature of oxidizing agent, and the composition of catalyst.展开更多
A series of NH_4Cs_(1.5)Fe_(0.08)H_xPVMo_(11)As_aO_y heteropolycompoundcatalysts for the selective oxidation of isobutane, having Keggin structure, were synthesized byusing co-precipitation method. The catalysts were ...A series of NH_4Cs_(1.5)Fe_(0.08)H_xPVMo_(11)As_aO_y heteropolycompoundcatalysts for the selective oxidation of isobutane, having Keggin structure, were synthesized byusing co-precipitation method. The catalysts were characterized by FT-IR, H_2-TPR, TG-DTA, SEM andXRD. Effects of the As content, reaction time, reaction temperature and molar ratio of isobutane tooxygen in feedstock on the activity and selectivity of the catalyst were investigated. Theactivation energy of the catalysts was measured by kinetics researches. Results showed theintroduction of Cs^+ into the catalysts shortened the stable period of them and enhanced theircatalytic activity for the selective oxidation of isobutane. The highest conversion of isobutane andthe total selectivity to liquid products were 18.6% and 81.2%, respectively, which were obtained at380℃ with a space velocity of 975 h^(-1) over the NH_4Cs_(1.5)Fe_(0.08)H_xPVMo_(11) As_(0.3)O_yheteropolycompound catalyst. It is confirmed that completely oxidized products were controlled well.展开更多
Cesium heteropolysalts Cs3PMo12O40 and HCs3PVMo11O40 were synthesized by modifying the preparation conditions in order to get materials with a much higher surface area than the original Keggin-type heteropolyacids(H3P...Cesium heteropolysalts Cs3PMo12O40 and HCs3PVMo11O40 were synthesized by modifying the preparation conditions in order to get materials with a much higher surface area than the original Keggin-type heteropolyacids(H3PMo12O40 and H4PVMo11O40).These solids were used as carriers for the dispersion of H4PVMo11O40 heteropolyacid by the incipient wetness impregnation technique.The textural and structural properties of supports and catalysts were examined by scanning electron microscopy,N2 adsorption-desorption isotherms and Raman spectroscopy.The supported catalysts were studied before and after red/ox pretreatments by X-ray photoelectron spectroscopy,which showed that both the surface composition and oxidized to reduced species ratio depend on the used carrier.The catalytic performances of these novel supported catalysts in the selective oxidation of isobutane to methacrylic acid and methacrolein were studied.The best catalytic properties were obtained when H4PVMo11O40 was supported on HCs3PVMo11O40.The isobutane conversion and yield of the desired oxygenates increased along the unsupported H4PVMo11O40【H4PVMo11O40/Cs3PMo12O40【H4PVMo11O40/HCs3PVMo11O40 series.展开更多
文摘Partial oxidation of methane to formaldehyde and methanol was studied at atmospheric pressure in the temperature range of 700-750 °C using heteropolycompound catalysts （NH4）6HSiMo11FeO40, （NH4）4PMo11FeO39, and H4PMo11VO40, which were prepared and characterized by various analysis techniques such as infrared, visible UV, XRD and DTA. O2 or N2O was used as the oxidizing agent, and the principal products of the reaction were CH3OH, CH2O, CO, CO2, and water. The conversion and the selectivity of products depend strongly on the reaction temperature, the nature of oxidizing agent, and the composition of catalyst.
基金Supported by Scientific Research Fund of Hunnan Provincial Education Department (03C515) Hunan Provincial Natural Science Foundation of China (04jj6003)
文摘A series of NH_4Cs_(1.5)Fe_(0.08)H_xPVMo_(11)As_aO_y heteropolycompoundcatalysts for the selective oxidation of isobutane, having Keggin structure, were synthesized byusing co-precipitation method. The catalysts were characterized by FT-IR, H_2-TPR, TG-DTA, SEM andXRD. Effects of the As content, reaction time, reaction temperature and molar ratio of isobutane tooxygen in feedstock on the activity and selectivity of the catalyst were investigated. Theactivation energy of the catalysts was measured by kinetics researches. Results showed theintroduction of Cs^+ into the catalysts shortened the stable period of them and enhanced theircatalytic activity for the selective oxidation of isobutane. The highest conversion of isobutane andthe total selectivity to liquid products were 18.6% and 81.2%, respectively, which were obtained at380℃ with a space velocity of 975 h^(-1) over the NH_4Cs_(1.5)Fe_(0.08)H_xPVMo_(11) As_(0.3)O_yheteropolycompound catalyst. It is confirmed that completely oxidized products were controlled well.
文摘Cesium heteropolysalts Cs3PMo12O40 and HCs3PVMo11O40 were synthesized by modifying the preparation conditions in order to get materials with a much higher surface area than the original Keggin-type heteropolyacids(H3PMo12O40 and H4PVMo11O40).These solids were used as carriers for the dispersion of H4PVMo11O40 heteropolyacid by the incipient wetness impregnation technique.The textural and structural properties of supports and catalysts were examined by scanning electron microscopy,N2 adsorption-desorption isotherms and Raman spectroscopy.The supported catalysts were studied before and after red/ox pretreatments by X-ray photoelectron spectroscopy,which showed that both the surface composition and oxidized to reduced species ratio depend on the used carrier.The catalytic performances of these novel supported catalysts in the selective oxidation of isobutane to methacrylic acid and methacrolein were studied.The best catalytic properties were obtained when H4PVMo11O40 was supported on HCs3PVMo11O40.The isobutane conversion and yield of the desired oxygenates increased along the unsupported H4PVMo11O40【H4PVMo11O40/Cs3PMo12O40【H4PVMo11O40/HCs3PVMo11O40 series.
