MoVNbTe catalyst has been found to be the most active and selective catalyst in the ammoxidation of propane to ACN, the selective oxidation of propane to acrylic acid and in the oxidative dehydrogenation of ethane to ...MoVNbTe catalyst has been found to be the most active and selective catalyst in the ammoxidation of propane to ACN, the selective oxidation of propane to acrylic acid and in the oxidative dehydrogenation of ethane to ethylene. However, in our previous work, when 0.5 mL of MoVNbTe catalyst prepared using slurry method was tested in the propane ammoxidation to ACN, it only shows 1% conversion of propane with about 55% selectivity to CAN, thus giving only 0.6% yields to ACN. The poor catalyst activity is attributed to insufficient formation of crystalline phases essential for the propane activation process. In an attempt to improve the physicochemical properties of this catalyst, several preparation methods have been used, namely hydrothermal, reflux, changing the solvent and changing the calcinations temperature. The modified catalysts have been characterized using X-Ray Diffraction （XRD） and N2 physisorption （BET）. The MoVNbTe catalyst prepared by hydrothermal method shows a remarkable improvement in the formation of crystalline phases.展开更多
A random walk Monte Carlo （RWMC） simulation model of catalytic particle was established on the basis of the structures of bismuth molybdate catalysts and mechanisms of catalytic reactions with propylene selective ox...A random walk Monte Carlo （RWMC） simulation model of catalytic particle was established on the basis of the structures of bismuth molybdate catalysts and mechanisms of catalytic reactions with propylene selective oxidation and ammoxidation. The simulation results show that rationality of the RWMC model is proved on the basis of pulse experimental data. One of the most remarkable factors affecting catalytic behavior is the transfer of bulk lattice oxygen, which decides the rate of ammonia-consuming and propylene-consuming. The selectivity of main products reaches the maximum after the reduction of catalysts to a certain degree. It is inferred that catalytic performance improves greatly if the ratio of capacity for dehydrogenation from adsorbed propylene molecule on catalytically active site of molybdenum metal-imido group （Mo=NH） to that on catalytically active site of molybdenum metal-oxo group （Mo=O） becomes much higher.展开更多
VSb3W-Al2O3 catalysts for propane ammoxidation were prepared by the conventional slurry method and new slurry method,namely,the reduction-oxidation slurry method.The effect of preparation methods on the physicochemica...VSb3W-Al2O3 catalysts for propane ammoxidation were prepared by the conventional slurry method and new slurry method,namely,the reduction-oxidation slurry method.The effect of preparation methods on the physicochemical properties of VSb3W-Al2O3 catalysts were studied by N2 adsorption,XRD,XPS and Raman spectroscopy,and their catalytic performance for the ammoxidation of propane to acrylonitrile were tested.Compared with the VSb3W-Al2O3 catalyst prepared by the conventional slurry method,the VSb3W-Al2O3 catalyst prepared by the reduction-oxidation slurry method exhibited better propane conversion and acrylonitrile selectivity.This is due to that the reduction-oxidation treatment was advantageous for obtaining low valence state vanadium and high valence state antimony to form more rutile SbVO4,which is a vital active phase for propane ammoxidation.展开更多
文摘MoVNbTe catalyst has been found to be the most active and selective catalyst in the ammoxidation of propane to ACN, the selective oxidation of propane to acrylic acid and in the oxidative dehydrogenation of ethane to ethylene. However, in our previous work, when 0.5 mL of MoVNbTe catalyst prepared using slurry method was tested in the propane ammoxidation to ACN, it only shows 1% conversion of propane with about 55% selectivity to CAN, thus giving only 0.6% yields to ACN. The poor catalyst activity is attributed to insufficient formation of crystalline phases essential for the propane activation process. In an attempt to improve the physicochemical properties of this catalyst, several preparation methods have been used, namely hydrothermal, reflux, changing the solvent and changing the calcinations temperature. The modified catalysts have been characterized using X-Ray Diffraction （XRD） and N2 physisorption （BET）. The MoVNbTe catalyst prepared by hydrothermal method shows a remarkable improvement in the formation of crystalline phases.
基金国家自然科学基金，the Fundamental Research Foundation of SINOPEC
文摘A random walk Monte Carlo （RWMC） simulation model of catalytic particle was established on the basis of the structures of bismuth molybdate catalysts and mechanisms of catalytic reactions with propylene selective oxidation and ammoxidation. The simulation results show that rationality of the RWMC model is proved on the basis of pulse experimental data. One of the most remarkable factors affecting catalytic behavior is the transfer of bulk lattice oxygen, which decides the rate of ammonia-consuming and propylene-consuming. The selectivity of main products reaches the maximum after the reduction of catalysts to a certain degree. It is inferred that catalytic performance improves greatly if the ratio of capacity for dehydrogenation from adsorbed propylene molecule on catalytically active site of molybdenum metal-imido group （Mo=NH） to that on catalytically active site of molybdenum metal-oxo group （Mo=O） becomes much higher.
基金support from the National Basic Research Program of China (No.2010CB732300)China Petroleum & Chemical Corporation (No.204061)
文摘VSb3W-Al2O3 catalysts for propane ammoxidation were prepared by the conventional slurry method and new slurry method,namely,the reduction-oxidation slurry method.The effect of preparation methods on the physicochemical properties of VSb3W-Al2O3 catalysts were studied by N2 adsorption,XRD,XPS and Raman spectroscopy,and their catalytic performance for the ammoxidation of propane to acrylonitrile were tested.Compared with the VSb3W-Al2O3 catalyst prepared by the conventional slurry method,the VSb3W-Al2O3 catalyst prepared by the reduction-oxidation slurry method exhibited better propane conversion and acrylonitrile selectivity.This is due to that the reduction-oxidation treatment was advantageous for obtaining low valence state vanadium and high valence state antimony to form more rutile SbVO4,which is a vital active phase for propane ammoxidation.
