A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observe...A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observed by scanning electron microscope (SEM) and transmission electron microscope (TEM).Mesopores could be detected by N2 adsorption-desorption isotherms which further confirmed the 3DOM structural characteristics of catalyst.Moreover,Keggin-type HPW was highly dispersed in the Al2O3 framework,which suggested by powder X-ray diffraction (XRD) and Fourier transform infrared spectra (FT-IR) results.The oxidation desulfurization (ODS) performance of 3DOM H3PW12O40/Al2O3 of refractory sulphur compounds was evaluated in the presence of hydrogen peroxide.It oxidized 98.5% of dibenzothiophene (DBT) into corresponding sulfone within 3 h,which exhibited superior ODS performance than corresponding mesoporous and microporous H3PW12O40/Al2O3 catalyst.The enhancement of ODS efficiency is related to the improvement of mass transfer of DBT in the pore channel resulting from the interconnected 3DOM structure.Furthermore,the as-prepared catalyst still demonstrates outstanding cycle performance after 6 runs,which could be easily recovered from the model fuel.展开更多
Nanostructured -y-A12O3 with high surface area and mesoporous structure was synthesized by sol-gel method and employed as catalyst support for nickel catalysts in methane reforming with carbon dioxide. The prepared sa...Nanostructured -y-A12O3 with high surface area and mesoporous structure was synthesized by sol-gel method and employed as catalyst support for nickel catalysts in methane reforming with carbon dioxide. The prepared samples were characterized by XRD, N2 adsorption-desorption, TPR, TPO, TPH, NH3-TPD and SEM techniques. The BET analysis showed a high surface area of 204 m2.g-1 and a narrow pore-size distribution centered at a diameter of 5.5 nm for catalyst support. The BET results revealed that addition of lanthanum oxide to aluminum oxide decreased the specific surface area. In addition, TPR results showed that addition of lanthanum oxide increased the reducibility of nickel catalyst. The catalytic evaluation results showed an increase in methane conversion with increasing lanthanum oxide to 3 mol% and further increase in lanthanum content decreased the catalytic activity. TPO analysis revealed that the coke deposition decreased with increasing lanthanum oxide to 3 mol%. SEM and TPH analyses confirmed the formation of whisker type carbon over the spent catalysts. Addition of steam and Oxide to drv reformin feed increased the methane conversion and led to carbon free ooeration in combined orocesses.展开更多
This work describes the environmentally friendly technology for oxidation of ammonia （NH3） to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation （SCO） over a nanosized Pt- Rh/γ...This work describes the environmentally friendly technology for oxidation of ammonia （NH3） to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation （SCO） over a nanosized Pt- Rh/γ-A12O3 catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid （H2PtC16） and rhodium （Ⅲ） nitrate （Rh（NO3）3） with γ-A12O3 in a tubular fixed-bed flow quartz reactor （TFBR）. The characterization of catalysts were thoroughly measured using transmission electron microscopy （TEM）, three- dimensional excitation-emission fluorescent matrix （EEFM） spectroscopy, UV-Vis absorption, dynamic light- scattering （DLS）, zeta potential meter, and cyclic voltam- metry （CV）. The results demonstrated that at a temperature of 673K and an oxygen content of4%, approximately 99% of the NH3 was removed by catalytic oxidation over the nanosized Pt-Rh/γ-A12O3 catalyst. N2 was the main product in NH3-SCO process. Further, it reveals that the oxidation of NH3 was proceeds by the over-oxidation of NH3 into NO, which was conversely reacted with the NH3 to yield N2. Therefore, the application ofnanosized Pt-Rh/γ-A12O3 catalyst can significantly enhance the catalytic activity toward NH3 oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-A12O3 catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.展开更多
基金Funded by the National Natural Science Foundation of China(No.21476177)。
文摘A series of heteropoly acid (HPA) based Al2O3 catalysts with three-dimensional ordered (3DOM) structure were synthesized by colloidal crystal template method.Interconnected macropores (250 nm) could be clearly observed by scanning electron microscope (SEM) and transmission electron microscope (TEM).Mesopores could be detected by N2 adsorption-desorption isotherms which further confirmed the 3DOM structural characteristics of catalyst.Moreover,Keggin-type HPW was highly dispersed in the Al2O3 framework,which suggested by powder X-ray diffraction (XRD) and Fourier transform infrared spectra (FT-IR) results.The oxidation desulfurization (ODS) performance of 3DOM H3PW12O40/Al2O3 of refractory sulphur compounds was evaluated in the presence of hydrogen peroxide.It oxidized 98.5% of dibenzothiophene (DBT) into corresponding sulfone within 3 h,which exhibited superior ODS performance than corresponding mesoporous and microporous H3PW12O40/Al2O3 catalyst.The enhancement of ODS efficiency is related to the improvement of mass transfer of DBT in the pore channel resulting from the interconnected 3DOM structure.Furthermore,the as-prepared catalyst still demonstrates outstanding cycle performance after 6 runs,which could be easily recovered from the model fuel.
基金supported by University of Kashan(Grant No.158426/29)
文摘Nanostructured -y-A12O3 with high surface area and mesoporous structure was synthesized by sol-gel method and employed as catalyst support for nickel catalysts in methane reforming with carbon dioxide. The prepared samples were characterized by XRD, N2 adsorption-desorption, TPR, TPO, TPH, NH3-TPD and SEM techniques. The BET analysis showed a high surface area of 204 m2.g-1 and a narrow pore-size distribution centered at a diameter of 5.5 nm for catalyst support. The BET results revealed that addition of lanthanum oxide to aluminum oxide decreased the specific surface area. In addition, TPR results showed that addition of lanthanum oxide increased the reducibility of nickel catalyst. The catalytic evaluation results showed an increase in methane conversion with increasing lanthanum oxide to 3 mol% and further increase in lanthanum content decreased the catalytic activity. TPO analysis revealed that the coke deposition decreased with increasing lanthanum oxide to 3 mol%. SEM and TPH analyses confirmed the formation of whisker type carbon over the spent catalysts. Addition of steam and Oxide to drv reformin feed increased the methane conversion and led to carbon free ooeration in combined orocesses.
文摘This work describes the environmentally friendly technology for oxidation of ammonia （NH3） to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation （SCO） over a nanosized Pt- Rh/γ-A12O3 catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid （H2PtC16） and rhodium （Ⅲ） nitrate （Rh（NO3）3） with γ-A12O3 in a tubular fixed-bed flow quartz reactor （TFBR）. The characterization of catalysts were thoroughly measured using transmission electron microscopy （TEM）, three- dimensional excitation-emission fluorescent matrix （EEFM） spectroscopy, UV-Vis absorption, dynamic light- scattering （DLS）, zeta potential meter, and cyclic voltam- metry （CV）. The results demonstrated that at a temperature of 673K and an oxygen content of4%, approximately 99% of the NH3 was removed by catalytic oxidation over the nanosized Pt-Rh/γ-A12O3 catalyst. N2 was the main product in NH3-SCO process. Further, it reveals that the oxidation of NH3 was proceeds by the over-oxidation of NH3 into NO, which was conversely reacted with the NH3 to yield N2. Therefore, the application ofnanosized Pt-Rh/γ-A12O3 catalyst can significantly enhance the catalytic activity toward NH3 oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-A12O3 catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.
