The effects of metal atomic ratio, water content, oxygen content, and calcination temperature on the catalytic performances of MoVTeNbO mixed oxide catalyst system for the selective oxidation of propane to acrylic aci...The effects of metal atomic ratio, water content, oxygen content, and calcination temperature on the catalytic performances of MoVTeNbO mixed oxide catalyst system for the selective oxidation of propane to acrylic acid have been investigated and discussed. Among the catalysts studied, it was found that the MoVTeNbO catalyst calcined at a temperature of 600 ℃ showed the best performance in terms of propane conversion and selectivity for acrylic acid under an atmosphere of nitrogen. An effective MoVTeNbO oxide catalyst for propane selective oxidation to acrylic acid was obtained with a combination of a preferred metal atomic ratio （Mo1V0.31Te0.23Nb0.12）. The optimum reaction condition for the selective oxidation of propane was the molar ratio of C3H8 ：O2 ： H2O ： N2 = 4.4： 12.8 ： 15.3 ： 36.9. Under such conditions, the conversion of propane and the maximum yield of acrylic acid reached about 50% and 21%, respectively.展开更多
Ammonium salts, （NH4）6HPMo11MO40 （M = Ni, Co, Fe）, have been investigated for the oxidation of propane, with molecular oxygen, at temperature ranging between 380 ℃ and 420 ℃ after in-situ pre-treatment performed...Ammonium salts, （NH4）6HPMo11MO40 （M = Ni, Co, Fe）, have been investigated for the oxidation of propane, with molecular oxygen, at temperature ranging between 380 ℃ and 420 ℃ after in-situ pre-treatment performed at two heating rate of 5 or 9 ℃/min. They were characterized by BET method, XRD, 31p NMR, UV-Vis and IR techniques. The catalysts were found active in the propane oxidation and selective to propene or acrolein, in particular for samples pre-treated with the heating rate of 9 ℃/min.展开更多
Selective oxidation of propane by lattice oxygen of vanadium-phosphorus oxide(VPO) catalysts was investigated with a pulse reactor in which the oxidation of propane and there-oxidation of catalyst were implemented alt...Selective oxidation of propane by lattice oxygen of vanadium-phosphorus oxide(VPO) catalysts was investigated with a pulse reactor in which the oxidation of propane and there-oxidation of catalyst were implemented alternately in the presence of water vapor. The principalproducts are acrylic acid (AA), acetic acid (HAc), and carbon oxides. In addition, small amounts ofC_1 and C_2 hydrocarbons were also found, molar ratio of AA to HAc is 1.4-2.2. The active oxygenspecies are those adsorbed on catalyst surface firmly and/or bound to catalyst lattice, i.e. latticeoxygen; the selective oxidation of propane on VPO catalysts can be carried out in a circulatingfluidized bed (CFB) riser reactor. For propane oxidation over VPO catalysts, the effects of reactiontemperature in a pulse reactor were found almost the same as in a steady-state flow reactor. Thatis, as the reaction temperature increases, propane conversion and the amount of C_1+C_2 hydrocarbonsin the product increase steadily, while selectivity to acrylic acid and to acetic acid increaseprior to 350℃ then begin to drop at temperatures higher than 350℃, and yields of acrylic acid andof acetic acid attained maximum at about 400℃. The maximum yields of acrylic acid and of aceticacid for a single-pass are 7.50% and 4.59% respectively, with 38.2% propane conversion. When theamount of propane pulsed decreases or the amount of catalyst loaded increases, the conversionincreases but the selectivity decreases. Increasing the flow rate of carrier gases causes theconversion pass through a minimum but selectivity and yields pass through a maximum. In a fixed bedreactor, it is hard to obtain high selectivity at a high reaction conversion due to the furtherdegradation of acrylic acid and acetic acid even though propane was oxidized by the lattice oxygen.The catalytic performance can be improved in the presence of excess propane. Propylene can beoxidized by lattice oxygen of VPO catalyst at 250℃, nevertheless, selectivity to AA and to HAc areeven lower, much more acetic 展开更多
A Pt/WO3/TiO2 catalyst for propane oxidation was prepared by a stepwise wet impregnation method, and was aged at 800°C for 5 hr. Compared to the sulfate-derived titania supported catalyst, the introduction of tun...A Pt/WO3/TiO2 catalyst for propane oxidation was prepared by a stepwise wet impregnation method, and was aged at 800°C for 5 hr. Compared to the sulfate-derived titania supported catalyst, the introduction of tungsten oxide as stable Br nsted acid sites led to the formation of more metallic platinum active sites at the Pt/WO3 interface. The dissociation of surface intermediates for propane oxidation was promoted on the WO3-modified catalyst. This, as well as the inhibition effects of tungsten oxide on the sintering of anatase and the phase transformation to rutile, resulting in a high activity and thermal stability for the Pt/WO3/TiO2 catalyst.展开更多
The pure phase of praseodymium orthovanadate (PrVO\-4) has been prepared by the citrate method. The active site of PrVO\-4 was studied by ESR, NO_TPD, O\-2_TPD and 18 O\-2_isotope exchange methods. The results of ESR ...The pure phase of praseodymium orthovanadate (PrVO\-4) has been prepared by the citrate method. The active site of PrVO\-4 was studied by ESR, NO_TPD, O\-2_TPD and 18 O\-2_isotope exchange methods. The results of ESR and NO_TPD confirmed the presence of V 4+ in the catalyst. 18 O\-2_isotope exchange was through a single exchange procedure. From the result of O\-2+TPD and the kinetic study of 18 O\-2_isotope exchange, one can reach a conclusion that the V 4+ species associated with oxygen vacancies are the site for O\-2 activation. The adsorbed O\-2 or O\+- are the active oxygen species in propane oxidative dehydrogenation.展开更多
文摘The effects of metal atomic ratio, water content, oxygen content, and calcination temperature on the catalytic performances of MoVTeNbO mixed oxide catalyst system for the selective oxidation of propane to acrylic acid have been investigated and discussed. Among the catalysts studied, it was found that the MoVTeNbO catalyst calcined at a temperature of 600 ℃ showed the best performance in terms of propane conversion and selectivity for acrylic acid under an atmosphere of nitrogen. An effective MoVTeNbO oxide catalyst for propane selective oxidation to acrylic acid was obtained with a combination of a preferred metal atomic ratio （Mo1V0.31Te0.23Nb0.12）. The optimum reaction condition for the selective oxidation of propane was the molar ratio of C3H8 ：O2 ： H2O ： N2 = 4.4： 12.8 ： 15.3 ： 36.9. Under such conditions, the conversion of propane and the maximum yield of acrylic acid reached about 50% and 21%, respectively.
文摘Ammonium salts, （NH4）6HPMo11MO40 （M = Ni, Co, Fe）, have been investigated for the oxidation of propane, with molecular oxygen, at temperature ranging between 380 ℃ and 420 ℃ after in-situ pre-treatment performed at two heating rate of 5 or 9 ℃/min. They were characterized by BET method, XRD, 31p NMR, UV-Vis and IR techniques. The catalysts were found active in the propane oxidation and selective to propene or acrolein, in particular for samples pre-treated with the heating rate of 9 ℃/min.
基金The work is supported by The Department of Education of Heilongjiang Province.
文摘Selective oxidation of propane by lattice oxygen of vanadium-phosphorus oxide(VPO) catalysts was investigated with a pulse reactor in which the oxidation of propane and there-oxidation of catalyst were implemented alternately in the presence of water vapor. The principalproducts are acrylic acid (AA), acetic acid (HAc), and carbon oxides. In addition, small amounts ofC_1 and C_2 hydrocarbons were also found, molar ratio of AA to HAc is 1.4-2.2. The active oxygenspecies are those adsorbed on catalyst surface firmly and/or bound to catalyst lattice, i.e. latticeoxygen; the selective oxidation of propane on VPO catalysts can be carried out in a circulatingfluidized bed (CFB) riser reactor. For propane oxidation over VPO catalysts, the effects of reactiontemperature in a pulse reactor were found almost the same as in a steady-state flow reactor. Thatis, as the reaction temperature increases, propane conversion and the amount of C_1+C_2 hydrocarbonsin the product increase steadily, while selectivity to acrylic acid and to acetic acid increaseprior to 350℃ then begin to drop at temperatures higher than 350℃, and yields of acrylic acid andof acetic acid attained maximum at about 400℃. The maximum yields of acrylic acid and of aceticacid for a single-pass are 7.50% and 4.59% respectively, with 38.2% propane conversion. When theamount of propane pulsed decreases or the amount of catalyst loaded increases, the conversionincreases but the selectivity decreases. Increasing the flow rate of carrier gases causes theconversion pass through a minimum but selectivity and yields pass through a maximum. In a fixed bedreactor, it is hard to obtain high selectivity at a high reaction conversion due to the furtherdegradation of acrylic acid and acetic acid even though propane was oxidized by the lattice oxygen.The catalytic performance can be improved in the presence of excess propane. Propylene can beoxidized by lattice oxygen of VPO catalyst at 250℃, nevertheless, selectivity to AA and to HAc areeven lower, much more acetic
基金supported by the Ministry of Science and Technology of China (No. 2009AA06Z313,2009AA064803)
文摘A Pt/WO3/TiO2 catalyst for propane oxidation was prepared by a stepwise wet impregnation method, and was aged at 800°C for 5 hr. Compared to the sulfate-derived titania supported catalyst, the introduction of tungsten oxide as stable Br nsted acid sites led to the formation of more metallic platinum active sites at the Pt/WO3 interface. The dissociation of surface intermediates for propane oxidation was promoted on the WO3-modified catalyst. This, as well as the inhibition effects of tungsten oxide on the sintering of anatase and the phase transformation to rutile, resulting in a high activity and thermal stability for the Pt/WO3/TiO2 catalyst.
文摘The pure phase of praseodymium orthovanadate (PrVO\-4) has been prepared by the citrate method. The active site of PrVO\-4 was studied by ESR, NO_TPD, O\-2_TPD and 18 O\-2_isotope exchange methods. The results of ESR and NO_TPD confirmed the presence of V 4+ in the catalyst. 18 O\-2_isotope exchange was through a single exchange procedure. From the result of O\-2+TPD and the kinetic study of 18 O\-2_isotope exchange, one can reach a conclusion that the V 4+ species associated with oxygen vacancies are the site for O\-2 activation. The adsorbed O\-2 or O\+- are the active oxygen species in propane oxidative dehydrogenation.
