Bismuth-promoted （1% and 3%） vanadyl pyrophosphate catalysts were prepared by refluxing Bi（NO3）4.5H2O and VOPO4.2H2O in isobutanol. The incorporation of Bi into the catalysts lattice increased the surface area and...Bismuth-promoted （1% and 3%） vanadyl pyrophosphate catalysts were prepared by refluxing Bi（NO3）4.5H2O and VOPO4.2H2O in isobutanol. The incorporation of Bi into the catalysts lattice increased the surface area and lowered the overall V oxidation state. Profiles of temperature programmed reduction （TPR） in H2 show a significant shift of the maxima of major reduction peaks to lower temperatures for the Bi-promoted catalysts. A new peak was also observed at the low temperature region for the catalyst with 3% of Bi dopant. The addition of Bi also increased the total amount of oxygen removed from the catalysts. The reduction pattern and reactivity information provide fundamental insight into the catalytic properties of the catalysts. Bi-promoted catalysts were found to be highly active （71% and 81% conversion for 1% and 3% Bi promoted catalysts, respectively, at 703 K）, as compared to the unpromoted material （47% conversion）. The higher activity of the Bi-promoted catalysts is due to that these catalysts possess highly active and labile lattice oxygen. The better catalytic performance can also be attributed to the larger surface area.展开更多
Three Bi-doped vanadyl pyrophosphate catalysts were prepared via dihydrate route （VPD method）, which consisted of different preparation methods including mechanosynthesis, mechanochemical treatment, and the conventi...Three Bi-doped vanadyl pyrophosphate catalysts were prepared via dihydrate route （VPD method）, which consisted of different preparation methods including mechanosynthesis, mechanochemical treatment, and the conventional reflux method. The catalysts produced by the above three methods were characterized by x-ray diffraction （XRD）, scanning electron microscopy （SEM）, and temperature programmed reduction （TPR）. Catalytic evaluation for the partial oxidation of n-butane to maleic anhydride （MA） was also carried out. The XRD patterns of all the Bi-doped catalysts showed the main peaks of pyrophosphate phase. Lower intensity peaks were observed for the mechanochemically treated Bi-doped catalyst （VPDBiMill） with two additional small peaks corresponding to the presence of a small amount of V5＋ phase. The TPR profiles showed that the highest amount of active oxygen species, i.e, V4＋–O- pair, responsible for n-butane activation, was removed from VPDBiMill. Furthermore, from the catalytic test results, the graph of selectivity to MA as a function of the conversion of n-butane demonstrated that VPDBiMill was the most selective catalyst. This suggests that the mechanochemical treatment of vanadium phosphate catalyst （VPDBiMill） is a potential method to improve the catalytic properties for the partial oxidation of n-butane to maleic anhydride.展开更多
A series of vanadyl pyrophosphate catalyst （VPO） modified by different additives have been prepared with the aim to study the performance for selective conversion of n-butane to maleic anhydride（MA）. The addition ...A series of vanadyl pyrophosphate catalyst （VPO） modified by different additives have been prepared with the aim to study the performance for selective conversion of n-butane to maleic anhydride（MA）. The addition of various promoters improved the catalytic performance remarkably on both activity and selectivity. The correlation of activity and selectivity of the catalysts with their structure has been discussed. The increase in BET surface areas and surface redox sites leads to an enhanced activity. However, good selectivity can only be obtained on those surfaces with suitable surface acid sites.展开更多
文摘Bismuth-promoted （1% and 3%） vanadyl pyrophosphate catalysts were prepared by refluxing Bi（NO3）4.5H2O and VOPO4.2H2O in isobutanol. The incorporation of Bi into the catalysts lattice increased the surface area and lowered the overall V oxidation state. Profiles of temperature programmed reduction （TPR） in H2 show a significant shift of the maxima of major reduction peaks to lower temperatures for the Bi-promoted catalysts. A new peak was also observed at the low temperature region for the catalyst with 3% of Bi dopant. The addition of Bi also increased the total amount of oxygen removed from the catalysts. The reduction pattern and reactivity information provide fundamental insight into the catalytic properties of the catalysts. Bi-promoted catalysts were found to be highly active （71% and 81% conversion for 1% and 3% Bi promoted catalysts, respectively, at 703 K）, as compared to the unpromoted material （47% conversion）. The higher activity of the Bi-promoted catalysts is due to that these catalysts possess highly active and labile lattice oxygen. The better catalytic performance can also be attributed to the larger surface area.
文摘Three Bi-doped vanadyl pyrophosphate catalysts were prepared via dihydrate route （VPD method）, which consisted of different preparation methods including mechanosynthesis, mechanochemical treatment, and the conventional reflux method. The catalysts produced by the above three methods were characterized by x-ray diffraction （XRD）, scanning electron microscopy （SEM）, and temperature programmed reduction （TPR）. Catalytic evaluation for the partial oxidation of n-butane to maleic anhydride （MA） was also carried out. The XRD patterns of all the Bi-doped catalysts showed the main peaks of pyrophosphate phase. Lower intensity peaks were observed for the mechanochemically treated Bi-doped catalyst （VPDBiMill） with two additional small peaks corresponding to the presence of a small amount of V5＋ phase. The TPR profiles showed that the highest amount of active oxygen species, i.e, V4＋–O- pair, responsible for n-butane activation, was removed from VPDBiMill. Furthermore, from the catalytic test results, the graph of selectivity to MA as a function of the conversion of n-butane demonstrated that VPDBiMill was the most selective catalyst. This suggests that the mechanochemical treatment of vanadium phosphate catalyst （VPDBiMill） is a potential method to improve the catalytic properties for the partial oxidation of n-butane to maleic anhydride.
基金Partially Supported by National Education Commission of China.
文摘A series of vanadyl pyrophosphate catalyst （VPO） modified by different additives have been prepared with the aim to study the performance for selective conversion of n-butane to maleic anhydride（MA）. The addition of various promoters improved the catalytic performance remarkably on both activity and selectivity. The correlation of activity and selectivity of the catalysts with their structure has been discussed. The increase in BET surface areas and surface redox sites leads to an enhanced activity. However, good selectivity can only be obtained on those surfaces with suitable surface acid sites.
