Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray dif...Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.展开更多
Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization met...Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.展开更多
A first principal modeling of the gasification of a char particle is performed using single step mechanism. The char particle is considered to be spherical in shape and only the physical and chemical properties can ch...A first principal modeling of the gasification of a char particle is performed using single step mechanism. The char particle is considered to be spherical in shape and only the physical and chemical properties can change in the radial direction. The carbon dioxide is used as the gasification agent that reacts with the char and form carbon monoxide. The presence of both solid and gaseous phase species makes the reaction heterogeneous. The char particle is considered with varying porosity that also allows the change in the surface area of the particle. A time invariant temperature and pressure profile is used at which the Arrhenius rate constant and diffusion is calculated. The mass conservation of model results in the form of two coupled partial differential and one ordinary differential equation. The equations are solved with a set of initial and boundary conditions using the bulk species concentration at the particle surface. A second order accurate central differencing scheme is used to discretize space while backward differencing is used to discretize time. Finally, the results are presented for the concentration distribution of CO and CO2 in radial direction with respect to time. It shows that, maximum concentration of CO is present at the center of the particle while the concentration gradient becomes higher near the particle surface. The nonlinear concentration trend due to the diffusion is effectively captured. The results show that, completed conversion of char depend upon the time provided for the reaction which can be reduced by decreasing the size of particle or increasing the reaction temperature. The sensitivity study of temperature and initial porosity also performed and showed that temperature has high impact on char conversion as compare to initial porosity.展开更多
基金supported by the National Natural Science Foundation of China (21477146,21303263)the National High Technology Research and Development Program of China (863 Program,2015AA034603)+2 种基金Beijing Nova Program (Z141109001814072)the Specialized Research Fund for the Doctoral Program of Higher Education of China (20130007120011)the Science Foundation of China University of Petroleum-Beijing (YJRC-2013-13,2462013BJRC003)~~
文摘Au/3DOM(three-dimensionally ordered macroporous) Al2O3 and Au/CeO2/3DOM Al2O3 were prepared using a reduction-deposition method and characterized using scanning electron microscopy,N2 adsorption-desorption,X-ray diffraction,transmission electron microscopy,ultraviolet-visible spectroscopy,temperature-programmed hydrogen reduction,and X-ray photoelectron spectroscopy.Au nanoparticles of similar sizes were well dispersed and supported on the inner walls of uniform macropores.The norminal Au loading is 2%.Al-Ce-O solid solution in CeO2/3DOM Al2O3 catalysts can be formed due to the incorporation of Al^3+ ions into the ceria lattice,which causes the creation of extrinsic oxygen vacancies.The extrinsic oxygen vacancies improved the oxygen-transport properties.The strong metal-support interactions between Au and CeO2 increased the amount of active oxygen on the Au nanoparticle surfaces,and this promoted soot oxidation.The activities of the Au-based catalysts were higher than those of the supports(Al2O3 or CeO2/3DOM Al2O3) at low temperature.Au/CeO2/3DOM Al2O3 had the highest catalytic activity for soot combustion,with T(10),T(50),and T(90) values of 273,364,and 412℃,respectively.
文摘Pd/C catalysts were prepared by deposited Pd nanoparticles (NPs) on different carbon supports including activated carbon (AC), graphite oxide (GO), and reduced graphite oxide (rGO) using sol-immobilization method. Through transmission electron microscopy, powder X-ray di raction, and X-ray photoelectron spectroscopy, the role of the carbon supports for the catalytic performances of Pd/C catalysts was examined in selective hydrogenation of acetylene. The results indicate that Pd/AC exhibited higher activity and selectivity than Pd/GO and Pd/rGO in the gas phase selective hydrogenation of acetylene. Thermal and chemical treatment of AC supports also have some effect on the catalytic performance of Pd/AC catalysts. The differences in the activity and selectivity of various Pd/C catalysts were partly attributed to the metal-support interaction.
文摘A first principal modeling of the gasification of a char particle is performed using single step mechanism. The char particle is considered to be spherical in shape and only the physical and chemical properties can change in the radial direction. The carbon dioxide is used as the gasification agent that reacts with the char and form carbon monoxide. The presence of both solid and gaseous phase species makes the reaction heterogeneous. The char particle is considered with varying porosity that also allows the change in the surface area of the particle. A time invariant temperature and pressure profile is used at which the Arrhenius rate constant and diffusion is calculated. The mass conservation of model results in the form of two coupled partial differential and one ordinary differential equation. The equations are solved with a set of initial and boundary conditions using the bulk species concentration at the particle surface. A second order accurate central differencing scheme is used to discretize space while backward differencing is used to discretize time. Finally, the results are presented for the concentration distribution of CO and CO2 in radial direction with respect to time. It shows that, maximum concentration of CO is present at the center of the particle while the concentration gradient becomes higher near the particle surface. The nonlinear concentration trend due to the diffusion is effectively captured. The results show that, completed conversion of char depend upon the time provided for the reaction which can be reduced by decreasing the size of particle or increasing the reaction temperature. The sensitivity study of temperature and initial porosity also performed and showed that temperature has high impact on char conversion as compare to initial porosity.