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
XRD, Raman, TEM, and N2-adsorption were utilized to characterize CeO2/SiO2 prepared by coprecipi-tation and surfactant-assisted method. The results show that nanocrystalline CeO2 can be uniformly supported on the surf...XRD, Raman, TEM, and N2-adsorption were utilized to characterize CeO2/SiO2 prepared by coprecipi-tation and surfactant-assisted method. The results show that nanocrystalline CeO2 can be uniformly supported on the surface of SiO2 particles, when the molar ratio of Si4+/(Ce3++Si4+) is less than 35% in coprecipitation samples. At higher Si content, the surface of SiO2 can not be fully covered by CeO2. With surfactant (CTAB) added, the u-iformly supported structure can even exist when the molar ratio of Si4+/(Ce3++Si4+) is as high as 53%. It is because Ce and Si complexes can be well dispersed in precursor solution in present of CTAB. However, the uniformly supported structure can not be synthesised through surfactant-assisted approch for its hydrothermal threatment, which can easily lead to separate aggregation of nanocrystalline CeO2 and SiO2 particles.展开更多
CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction （...CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction （TPR）, and FT-IR, the influence of the cerium content on the catalytic performance of CeO2-Co3O4 was investigated. The results indicate that the prepared CeO2-Co3O4 catalysts exhibit a better activity than that of pure CeO2 or pure Co3O4. The catalyst with the Ce/Co atomic ratio 1 ： 16 exhibits the best activity, which converts 77% of CO at room temperature and completely oxidizes CO at 45 ℃.展开更多
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XRD, Raman, TEM, and N2-adsorption were utilized to characterize CeO2/SiO2 prepared by coprecipi-tation and surfactant-assisted method. The results show that nanocrystalline CeO2 can be uniformly supported on the surface of SiO2 particles, when the molar ratio of Si4+/(Ce3++Si4+) is less than 35% in coprecipitation samples. At higher Si content, the surface of SiO2 can not be fully covered by CeO2. With surfactant (CTAB) added, the u-iformly supported structure can even exist when the molar ratio of Si4+/(Ce3++Si4+) is as high as 53%. It is because Ce and Si complexes can be well dispersed in precursor solution in present of CTAB. However, the uniformly supported structure can not be synthesised through surfactant-assisted approch for its hydrothermal threatment, which can easily lead to separate aggregation of nanocrystalline CeO2 and SiO2 particles.
文摘CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction （TPR）, and FT-IR, the influence of the cerium content on the catalytic performance of CeO2-Co3O4 was investigated. The results indicate that the prepared CeO2-Co3O4 catalysts exhibit a better activity than that of pure CeO2 or pure Co3O4. The catalyst with the Ce/Co atomic ratio 1 ： 16 exhibits the best activity, which converts 77% of CO at room temperature and completely oxidizes CO at 45 ℃.
