The vapor-phase synthesis of 3-methylindole over Ag/SiO2 doped with ZnO was investigated. The catalysts were characterized by XRD, H2- TPR, NH3-TPD and TG techniques. The results indicated that ZnO promoter greatly en...The vapor-phase synthesis of 3-methylindole over Ag/SiO2 doped with ZnO was investigated. The catalysts were characterized by XRD, H2- TPR, NH3-TPD and TG techniques. The results indicated that ZnO promoter greatly enhanced the initial activity of the catalyst but disfavored its stability. H2-TPR and XRD results showed that the reduction peak of Ag2O shifted to higher temperature and the intensity of silver diffraction peaks was much weaker after the addition of ZnO promoter to Ag/SiO2. This indicated that there existed the interaction between Ag2O and SiO2-ZnO which promoted the silver particles dispersing on the support and inhibited the sintering of silver during the reaction. NH3-TPD and TG results revealed that the acid amounts of the catalyst and coking increased after adding ZnO to Ag/SiO2, which resulted in the deactivation of Ag/SiO2-ZnO catalyst rapidly.展开更多
The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition beha...The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.展开更多
The surface species of CO hydrogenation on CeO2-Co/SiO2 catalyst were investigated using the techniques of temperature programmed reaction and transient response method. The results indicated that the formation of H2O...The surface species of CO hydrogenation on CeO2-Co/SiO2 catalyst were investigated using the techniques of temperature programmed reaction and transient response method. The results indicated that the formation of H2O and CO2 was the competitive reaction for the surface oxygen species, CH4 was produced via the hydrogenation of carbon species step by step, and C2 products were formed by the polymerization of surface-active carbon species （-CH2-）. Hydrogen assisted the dissociation of CO. The hydrogenation of surface carbon species was the rate-limiting step in the hydrogenation of CO over CeO2-Co/SiO2 catalyst. The investigation of total pressure, gas hourly space velocity （GHSV）, and product distribution using nitrogen-rich synthesis gas as feedstock over a laboratory scale fixed-bed reactor indicated that total pressure and GHSV had a significant effect on the catalytic performance of CeO2-Co/SiO2 catalyst. The removal of heat and control of the reaction temperature were extremely critical steps, which required lower GHSV and appropriate CO conversion to avoid the deactivation of the catalyst. The feedstock of nitrogen-rich synthesis gas was favorable to increase the conversion of CO, but there was a shift of product distribution toward the light hydrocarbon. The nitrogen-rich synthesis gas was feasible for F-T synthesis for the utilization of remote natural gas.展开更多
ZnO/SiO\-2 and ZnO\|SiO\-2 catalysts were prepared by the impregnation and sol\|gel method, respectively. The characterization of the catalysts by XPS and FTIR indicated that much "free" zinc oxide and unrea...ZnO/SiO\-2 and ZnO\|SiO\-2 catalysts were prepared by the impregnation and sol\|gel method, respectively. The characterization of the catalysts by XPS and FTIR indicated that much "free" zinc oxide and unreacted Si\_OH existed on the surface of ZnO/SiO\-2 sample. As for ZnO\|SiO\-2 sol\|gel catalyst, the corresponding phenomena were not observed. The prepared samples were also used as the catalysts for decomposition of 2\|butanol. A high selectivity for dehydrogenation was observed over the supported catalyst. However, a high selectivity for dehydration was shown over the ZnO\|SiO\-2 sol\|gel catalyst. The opposite selectivity for dehydration or dehydrogenation observed over the two kinds of catalysts may be just because of the different surface structures of the catalysts.展开更多
Core–shell nanoparticles containing plasmonic metals（Ag or Au） have been frequently reported to enhance performance of photo-electrochemical（PEC） devices. However, the stability of these particles in water-splitt...Core–shell nanoparticles containing plasmonic metals（Ag or Au） have been frequently reported to enhance performance of photo-electrochemical（PEC） devices. However, the stability of these particles in water-splitting conditions is usually not addressed. In this study we demonstrate that Ag@SiOcore–shell particles are instable in the acidic conditions in which WO-based PEC cells typically operate, Ag in the core being prone to oxidation, even if the SiOshell has a thickness in the order of 10 nm. This is evident from in situ voltammetry studies of several anode composites. Similar to the results of the PEC experiments, the Ag@SiOcore–shell particles are instable in slurry-based, Pt/ZnO induced photocatalytic water-splitting. This was evidenced by in situ photodeposition of Ag nanoparticles on the Pt-loaded ZnO catalyst, observed in TEM micrographs obtained after reaction. We explain the instability of Ag@SiOby OH-radical induced oxidation of Ag, yielding dissolved Ag+. Our results imply that a decrease in shell permeability for OH-radicals is necessary to obtain stable, Ag-based plasmonic entities in photo-electrochemical and photocatalytic water splitting.展开更多
The Ag/SiO2 nanoparticles had been successfully synthesized. The Ag/SiO2 nano- particles can be an excellent catalyst for the synthesis of ultraviolet absorber benzotriazole by catalytic hydrogenation. The synthesis r...The Ag/SiO2 nanoparticles had been successfully synthesized. The Ag/SiO2 nano- particles can be an excellent catalyst for the synthesis of ultraviolet absorber benzotriazole by catalytic hydrogenation. The synthesis route is very efficient with less pollution and excellent yields. It is also easy to industrialized production.展开更多
Cu/ZnO/Al_(2)O_(3) catalysts with Cu/Zn/Al ratios of 6/3/1 were precipitated and aged by conventional and microwave heating methods and tested in the slurry phase reactor for methanol synthesis.The effect of technolog...Cu/ZnO/Al_(2)O_(3) catalysts with Cu/Zn/Al ratios of 6/3/1 were precipitated and aged by conventional and microwave heating methods and tested in the slurry phase reactor for methanol synthesis.The effect of technological condition of precipitation and aging process under microwave irradiation on the catalytic performance was investigated to optimize the preparing condition of Cu/ZnO/Al_(2)O_(3) catalyst.The results showed that the microwave irradiation during precipitation process could improve the activity of the catalyst,but had little effect on the stability.While the microwave irradiation during aging process has a great benefit to both the activity and stability of the catalyst,the catalyst aged at 80℃ for 1 h under microwave irradiation possessed higher methanol space time yield(STY)and more stable catalytic activity.The activity and stability of the catalyst was further enhanced when microwave irradiation was used in both precipitation and aging processes;the optimized condition for the catalyst precursor preparation was precipitation at 60℃ and aging at 80℃ under microwave irradiation.展开更多
基金supported by the Innovative Research Team in University of Liaoning (No. 2008T106)
文摘The vapor-phase synthesis of 3-methylindole over Ag/SiO2 doped with ZnO was investigated. The catalysts were characterized by XRD, H2- TPR, NH3-TPD and TG techniques. The results indicated that ZnO promoter greatly enhanced the initial activity of the catalyst but disfavored its stability. H2-TPR and XRD results showed that the reduction peak of Ag2O shifted to higher temperature and the intensity of silver diffraction peaks was much weaker after the addition of ZnO promoter to Ag/SiO2. This indicated that there existed the interaction between Ag2O and SiO2-ZnO which promoted the silver particles dispersing on the support and inhibited the sintering of silver during the reaction. NH3-TPD and TG results revealed that the acid amounts of the catalyst and coking increased after adding ZnO to Ag/SiO2, which resulted in the deactivation of Ag/SiO2-ZnO catalyst rapidly.
基金supported by the National Natural Science Foundation of China(No.51576039)
文摘The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.
基金the National Key Project for Basic Research of China(973 Project)(No.2005CB221402)the China National Petroleum Corporation.
文摘The surface species of CO hydrogenation on CeO2-Co/SiO2 catalyst were investigated using the techniques of temperature programmed reaction and transient response method. The results indicated that the formation of H2O and CO2 was the competitive reaction for the surface oxygen species, CH4 was produced via the hydrogenation of carbon species step by step, and C2 products were formed by the polymerization of surface-active carbon species （-CH2-）. Hydrogen assisted the dissociation of CO. The hydrogenation of surface carbon species was the rate-limiting step in the hydrogenation of CO over CeO2-Co/SiO2 catalyst. The investigation of total pressure, gas hourly space velocity （GHSV）, and product distribution using nitrogen-rich synthesis gas as feedstock over a laboratory scale fixed-bed reactor indicated that total pressure and GHSV had a significant effect on the catalytic performance of CeO2-Co/SiO2 catalyst. The removal of heat and control of the reaction temperature were extremely critical steps, which required lower GHSV and appropriate CO conversion to avoid the deactivation of the catalyst. The feedstock of nitrogen-rich synthesis gas was favorable to increase the conversion of CO, but there was a shift of product distribution toward the light hydrocarbon. The nitrogen-rich synthesis gas was feasible for F-T synthesis for the utilization of remote natural gas.
文摘ZnO/SiO\-2 and ZnO\|SiO\-2 catalysts were prepared by the impregnation and sol\|gel method, respectively. The characterization of the catalysts by XPS and FTIR indicated that much "free" zinc oxide and unreacted Si\_OH existed on the surface of ZnO/SiO\-2 sample. As for ZnO\|SiO\-2 sol\|gel catalyst, the corresponding phenomena were not observed. The prepared samples were also used as the catalysts for decomposition of 2\|butanol. A high selectivity for dehydrogenation was observed over the supported catalyst. However, a high selectivity for dehydration was shown over the ZnO\|SiO\-2 sol\|gel catalyst. The opposite selectivity for dehydration or dehydrogenation observed over the two kinds of catalysts may be just because of the different surface structures of the catalysts.
基金part of the research programme of the Foundation for Fundamental Research on Matter(FOM,project 10TBSC07-1),which is part of the Netherlands Organisation for Scientific Research(NWO)
文摘Core–shell nanoparticles containing plasmonic metals（Ag or Au） have been frequently reported to enhance performance of photo-electrochemical（PEC） devices. However, the stability of these particles in water-splitting conditions is usually not addressed. In this study we demonstrate that Ag@SiOcore–shell particles are instable in the acidic conditions in which WO-based PEC cells typically operate, Ag in the core being prone to oxidation, even if the SiOshell has a thickness in the order of 10 nm. This is evident from in situ voltammetry studies of several anode composites. Similar to the results of the PEC experiments, the Ag@SiOcore–shell particles are instable in slurry-based, Pt/ZnO induced photocatalytic water-splitting. This was evidenced by in situ photodeposition of Ag nanoparticles on the Pt-loaded ZnO catalyst, observed in TEM micrographs obtained after reaction. We explain the instability of Ag@SiOby OH-radical induced oxidation of Ag, yielding dissolved Ag+. Our results imply that a decrease in shell permeability for OH-radicals is necessary to obtain stable, Ag-based plasmonic entities in photo-electrochemical and photocatalytic water splitting.
基金supported by research fund of Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province (No. AE201127)
文摘The Ag/SiO2 nanoparticles had been successfully synthesized. The Ag/SiO2 nano- particles can be an excellent catalyst for the synthesis of ultraviolet absorber benzotriazole by catalytic hydrogenation. The synthesis route is very efficient with less pollution and excellent yields. It is also easy to industrialized production.
基金supported by the National Basic Research Program of China(Grant No.2005CB221204).
文摘Cu/ZnO/Al_(2)O_(3) catalysts with Cu/Zn/Al ratios of 6/3/1 were precipitated and aged by conventional and microwave heating methods and tested in the slurry phase reactor for methanol synthesis.The effect of technological condition of precipitation and aging process under microwave irradiation on the catalytic performance was investigated to optimize the preparing condition of Cu/ZnO/Al_(2)O_(3) catalyst.The results showed that the microwave irradiation during precipitation process could improve the activity of the catalyst,but had little effect on the stability.While the microwave irradiation during aging process has a great benefit to both the activity and stability of the catalyst,the catalyst aged at 80℃ for 1 h under microwave irradiation possessed higher methanol space time yield(STY)and more stable catalytic activity.The activity and stability of the catalyst was further enhanced when microwave irradiation was used in both precipitation and aging processes;the optimized condition for the catalyst precursor preparation was precipitation at 60℃ and aging at 80℃ under microwave irradiation.
