In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were charac...In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were characterized by SEM,NH3-TPD and N2adsorption-desorption isotherms to indicate their intrinsic characteristics.Furthermore,in order to understand the mechanism of deactivation,the resulted green oil was characterized using FTIR and SIM DIS.FTIR results confirmed the presence of more unsaturated constituents and then,more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO,which in turn,could block the pores mouths.Besides the limited hydrogen transfer,N2 adsorption-desorption isotherms results supported that the lowest pore diameters of Al2O3/SMFs close to the surface led to fast deactivation,compared with the other catalysts,especially at higher temperatures.展开更多
The effects of manganese oxide or ceria promoters on the performance of Na2WO4/SiO2 catalysts for oxidative coupling of methane (OCM) are reported. The OCM reaction was performed in a continuous-flow microreactor at...The effects of manganese oxide or ceria promoters on the performance of Na2WO4/SiO2 catalysts for oxidative coupling of methane (OCM) are reported. The OCM reaction was performed in a continuous-flow microreactor at 800℃, atmospheric pressure and under GHSV = 13200 ml·gCat^-1·h^-1.Catalysts were characterized by in situ conductivity measurement, FT-IR spectroscopy, XRD, SEM and temperature programmed reduction analysis. Manganese oxide promoted Na2WO4/SiO2 is considered as one of the active and selective catalysts for OCM reaction. Ceria with high oxygen storage capacity is selected as a proper oxygen activator, providing a higher concentration of the oxy-anion species which is suitable for OCM reaction and compared with manganese oxide. Electrical conductivity of the catalysts was measured in OCM reaction under oxidizing atmosphere, i.e. in the absence of methane. It was found that the trimetallic catalysts, i.e. the catalysts having sodium, tungsten and Mn or Ce species, exhibited similar crystalline structures and morphologies, which lead to suitable bulk properties for the formation of an active and selective catalyst. However, tungsten had significant effect on the texture and redox properties of the catalysts. It was also shown that the crystalline structure of the bimetallic (Na+Mn or Ce)/SiO2 samples was quite different. This reveals that the metal oxides have significant effect on the extent of crystallization, taking place in the course of interaction of sodium with silica support. Similar conductivities and catalytic performances of (Na2WO4+Mn or Ce)/SiO2 catalysts propose that the ability of Na2WO4/SiO2 for utilizing oxy-anions formed in presence of different metal oxides is limited.展开更多
Series of mixed metal oxides were synthesized by gel-combustion method and their catalytic activities for soot oxidation were investigated. The catalysts were M-Ce-Zr (M = Mn, Cu, Fe, K, Ba, Sr), and χK-20Mn-Ce-Zr...Series of mixed metal oxides were synthesized by gel-combustion method and their catalytic activities for soot oxidation were investigated. The catalysts were M-Ce-Zr (M = Mn, Cu, Fe, K, Ba, Sr), and χK-20Mn-Ce-Zr (χ= 0, 5, 10, 20), they were characterized by XRD, SEM, TPR and BET surface area techniques. The results of soot temperature programmed oxidation (TPO) in an O2 oxidizing atmosphere indicate that K-Ce-Zr has the highest catalytic activity for soot oxidation under loose contact condition, due to enhancement of the soot and catalyst contacts. On the other hand, under a tight contact condition, Mn-Ce-Zr and Cu-Ce-Zr nano-composites have high activities for soot oxidation and lower the soot TPO peak temperatures by about 280 and 270℃, respectively, as compared to non-catalytic soot oxidation. Furthermore, the addition of up to 10 wt.% potassium oxides into Mn-Ce-Zr increases its catalytic activity and further reduces the soot TPO peak temperature by about 40℃ under loose contact condition.展开更多
A series of organic compounds were successfully immobilized on an N-doped graphene quantum dot (N-GQD) to prepare a multifunctional organocatalyst for coupling reaction between CO_(2)and propylene oxide (PO).The simul...A series of organic compounds were successfully immobilized on an N-doped graphene quantum dot (N-GQD) to prepare a multifunctional organocatalyst for coupling reaction between CO_(2)and propylene oxide (PO).The simultaneous presence of halide ions in conjunction with acidic-and basic-functional groups on the surface of the nanoparticles makes them highly active for the production of propylene carbonate (PC).The effects of variables such as catalyst loading,reaction temperature,and structure of substituents are discussed.The proposed catalysts were characterized by different techniques,including Fourier transform infrared spectroscopy (FTIR),field emission scanning electron microscopy/energy dispersive X-ray microanalysis (FESEM/EDX),thermogravimetric analysis (TGA),elemental analysis,atomic force microscopy (AFM),and ultraviolet–visible (UV-Vis) spectroscopy.Under optimal reaction conditions,3-bromopropionic acid (BPA) immobilized on N-GQD showed a remarkable activity,affording the highest yield of 98%at 140℃ and 106Pa without any co-catalyst or solvent.These new metal-free catalysts have the advantage of easy separation and reuse several times.Based on the experimental data,a plausible reaction mechanism is suggested,where the hydrogen bonding donors and halogen ion can activate the epoxide,and amine functional groups play a vital role in CO_(2)adsorption.展开更多
文摘In the present study,CNFs,ZnO and Al2O3 were deposited on the SMFs panels to investigate the deactivation mechanism of Pd-based catalysts in selective acetylene hydrogenation reaction.The examined supports were characterized by SEM,NH3-TPD and N2adsorption-desorption isotherms to indicate their intrinsic characteristics.Furthermore,in order to understand the mechanism of deactivation,the resulted green oil was characterized using FTIR and SIM DIS.FTIR results confirmed the presence of more unsaturated constituents and then,more branched hydrocarbons formed upon the reaction over alumina-supported catalyst in comparison with the ones supported on CNFs and ZnO,which in turn,could block the pores mouths.Besides the limited hydrogen transfer,N2 adsorption-desorption isotherms results supported that the lowest pore diameters of Al2O3/SMFs close to the surface led to fast deactivation,compared with the other catalysts,especially at higher temperatures.
文摘The effects of manganese oxide or ceria promoters on the performance of Na2WO4/SiO2 catalysts for oxidative coupling of methane (OCM) are reported. The OCM reaction was performed in a continuous-flow microreactor at 800℃, atmospheric pressure and under GHSV = 13200 ml·gCat^-1·h^-1.Catalysts were characterized by in situ conductivity measurement, FT-IR spectroscopy, XRD, SEM and temperature programmed reduction analysis. Manganese oxide promoted Na2WO4/SiO2 is considered as one of the active and selective catalysts for OCM reaction. Ceria with high oxygen storage capacity is selected as a proper oxygen activator, providing a higher concentration of the oxy-anion species which is suitable for OCM reaction and compared with manganese oxide. Electrical conductivity of the catalysts was measured in OCM reaction under oxidizing atmosphere, i.e. in the absence of methane. It was found that the trimetallic catalysts, i.e. the catalysts having sodium, tungsten and Mn or Ce species, exhibited similar crystalline structures and morphologies, which lead to suitable bulk properties for the formation of an active and selective catalyst. However, tungsten had significant effect on the texture and redox properties of the catalysts. It was also shown that the crystalline structure of the bimetallic (Na+Mn or Ce)/SiO2 samples was quite different. This reveals that the metal oxides have significant effect on the extent of crystallization, taking place in the course of interaction of sodium with silica support. Similar conductivities and catalytic performances of (Na2WO4+Mn or Ce)/SiO2 catalysts propose that the ability of Na2WO4/SiO2 for utilizing oxy-anions formed in presence of different metal oxides is limited.
文摘Series of mixed metal oxides were synthesized by gel-combustion method and their catalytic activities for soot oxidation were investigated. The catalysts were M-Ce-Zr (M = Mn, Cu, Fe, K, Ba, Sr), and χK-20Mn-Ce-Zr (χ= 0, 5, 10, 20), they were characterized by XRD, SEM, TPR and BET surface area techniques. The results of soot temperature programmed oxidation (TPO) in an O2 oxidizing atmosphere indicate that K-Ce-Zr has the highest catalytic activity for soot oxidation under loose contact condition, due to enhancement of the soot and catalyst contacts. On the other hand, under a tight contact condition, Mn-Ce-Zr and Cu-Ce-Zr nano-composites have high activities for soot oxidation and lower the soot TPO peak temperatures by about 280 and 270℃, respectively, as compared to non-catalytic soot oxidation. Furthermore, the addition of up to 10 wt.% potassium oxides into Mn-Ce-Zr increases its catalytic activity and further reduces the soot TPO peak temperature by about 40℃ under loose contact condition.
基金supported by Iran National Science Foundation(No.97015707)。
文摘A series of organic compounds were successfully immobilized on an N-doped graphene quantum dot (N-GQD) to prepare a multifunctional organocatalyst for coupling reaction between CO_(2)and propylene oxide (PO).The simultaneous presence of halide ions in conjunction with acidic-and basic-functional groups on the surface of the nanoparticles makes them highly active for the production of propylene carbonate (PC).The effects of variables such as catalyst loading,reaction temperature,and structure of substituents are discussed.The proposed catalysts were characterized by different techniques,including Fourier transform infrared spectroscopy (FTIR),field emission scanning electron microscopy/energy dispersive X-ray microanalysis (FESEM/EDX),thermogravimetric analysis (TGA),elemental analysis,atomic force microscopy (AFM),and ultraviolet–visible (UV-Vis) spectroscopy.Under optimal reaction conditions,3-bromopropionic acid (BPA) immobilized on N-GQD showed a remarkable activity,affording the highest yield of 98%at 140℃ and 106Pa without any co-catalyst or solvent.These new metal-free catalysts have the advantage of easy separation and reuse several times.Based on the experimental data,a plausible reaction mechanism is suggested,where the hydrogen bonding donors and halogen ion can activate the epoxide,and amine functional groups play a vital role in CO_(2)adsorption.