The structure and catalytic properties of SrTi1- xMgxO3- δ perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD), X ray photoelectron spectroscopy (XPS) ...The structure and catalytic properties of SrTi1- xMgxO3- δ perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD), X ray photoelectron spectroscopy (XPS) and Temperature programmed desorption (O2 TPD) methods. It has been shown that doping Mg2+ cations to the B site of SrTi1- xMgxO3- δ perovskite type catalysts results in the formation of oxygen vacancies in the lattices of oxide catalysts. With increasing the amount of Mg2+ doped in the B site of SrTi1- xMgxO3- δ , methane conversion and C2 selectivity first increase and then decrease remarkably. The SrTi1- xMgxO3- δ catalyst with x=0.1 has the highest methane conversion and C2 yield. It is suggested that the oxygen vacancies produced by Mg2+ cations doping are the sites responsible for oxygen activation, and the adsorbed oxygen species on the surface of SrTi1- xMgxO3- δ catalysts are the main active species for OCM reaction. However, the over high content of the adsorbed oxygen species on the surface results in the complete oxidation of methane. Introducing water steam into feedstock can improve the catalytic properties of SrTi1- xMgxO3- δ perovskite type catalysts for OCM reaction at lower temperature. The SrTi0.9Mg0.1O3- δ catalyst has the methane conversion of 28.0 % with C2 hydrocarbons selectivity of 36.8 % under reaction temperature of 550 ℃ .展开更多
The structure and catalytic properties of SrTiO3 perovskite-type oxide catalysts for oxidative coupling of methane (OCM) have been studied by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and m...The structure and catalytic properties of SrTiO3 perovskite-type oxide catalysts for oxidative coupling of methane (OCM) have been studied by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and microreactor tests. It has been shown that OCM catalytic properties of SrTiO3 catalysts are correlated to the Sr/Ti atomic ratio. Increasing Sr/Ti ratio in the perovskite?-type SrTiO3 catalysts results in the surface enrichment of Sr element, leading to the the higher content of adsorbed oxygen species on the surface of catalysts and thus higher C2 selectivity for OCM reaction.展开更多
The structure and catalytic properties of SrTi0.9M0.1O3- δ (M=Mg,Al, Zr) perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD),X ray photoelectron spectr...The structure and catalytic properties of SrTi0.9M0.1O3- δ (M=Mg,Al, Zr) perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD),X ray photoelectron spectroscopy (XPS) and temperature programmed desorption of oxygen(O2 TPD) methods. It has been shown that doping the cations of lower valence (e.g. Mg2+ , Al3+ ) to the B site of SrTi0.9M0.1O3- δ perovskite type catalysts results in the higher content of adsorbed oxygen species on the surface of catalysts and thus higher C2 selectivity for OCM reaction. It is suggested that the oxygen vacancies of SrTi0.9M0.1O3- δ (M=Mg, Al, Zr) perovskite type catalysts are the sites responsible for oxygen activation, and the adsorbed oxygen species on the surface of SrTi0.9M0.1O3- δ catalysts are the main active species for OCM reaction.展开更多
XRD and XPS are used to study the dispersion state of CuO on ceria surface.The dispersion capacity values of CuO measured by the two methods are consistent,which are of 1.20 mmol CuO/100 m CeO2.In addition,the results...XRD and XPS are used to study the dispersion state of CuO on ceria surface.The dispersion capacity values of CuO measured by the two methods are consistent,which are of 1.20 mmol CuO/100 m CeO2.In addition,the results reveal that highly dispersed Cu2 + ions are formed at low CuO loadings and that increasing the CuO content to a value higher than its dispersion capacity produces crystalline CuO after the surface vacant sites on CeO2 are filled.The atomic composition of the outermost layer of the CuO/CeO2 samples has been probed by using static secondary ion mass spectroscopy (SSIMS),and the ratios of Cu/Ce are found to be 0.93 and 0.46 for the 1.22 and 0 61 mmol CuO/CeO2 samples respectively.Temperature-programmed reduction (TPR) profile with two reduction peaks at 156 and 16513 suggests that the reduction of highly dispersed Cu2+ ions consists of two steps and is easier than that of CuO crystallites,in which the TPR profile has only one reduction peak at about 249℃.The above experimental results are in good agreement with the prediction of the incorporation model.展开更多
Since it was first reported by Keller and Bhasin in 1982 that ethane and ethylene could be produced through direct oxidation of methane, methane oxidative coupling （MOC） has attracted increasing interest in the worl...Since it was first reported by Keller and Bhasin in 1982 that ethane and ethylene could be produced through direct oxidation of methane, methane oxidative coupling （MOC） has attracted increasing interest in the world. By now some highly efficient catalysts have been explored such as Li/MgO, La<sub>2</sub>O<sub>3</sub>, and [Th, La]O<sub>2-x</sub>, and C<sub>2</sub> yields can reach 15—20％. However, such high yields are obtained at the high temperature of 700—800℃. The kinetic and mechanism studies show that at such high temperature展开更多
文摘The structure and catalytic properties of SrTi1- xMgxO3- δ perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD), X ray photoelectron spectroscopy (XPS) and Temperature programmed desorption (O2 TPD) methods. It has been shown that doping Mg2+ cations to the B site of SrTi1- xMgxO3- δ perovskite type catalysts results in the formation of oxygen vacancies in the lattices of oxide catalysts. With increasing the amount of Mg2+ doped in the B site of SrTi1- xMgxO3- δ , methane conversion and C2 selectivity first increase and then decrease remarkably. The SrTi1- xMgxO3- δ catalyst with x=0.1 has the highest methane conversion and C2 yield. It is suggested that the oxygen vacancies produced by Mg2+ cations doping are the sites responsible for oxygen activation, and the adsorbed oxygen species on the surface of SrTi1- xMgxO3- δ catalysts are the main active species for OCM reaction. However, the over high content of the adsorbed oxygen species on the surface results in the complete oxidation of methane. Introducing water steam into feedstock can improve the catalytic properties of SrTi1- xMgxO3- δ perovskite type catalysts for OCM reaction at lower temperature. The SrTi0.9Mg0.1O3- δ catalyst has the methane conversion of 28.0 % with C2 hydrocarbons selectivity of 36.8 % under reaction temperature of 550 ℃ .
文摘The structure and catalytic properties of SrTiO3 perovskite-type oxide catalysts for oxidative coupling of methane (OCM) have been studied by using X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and microreactor tests. It has been shown that OCM catalytic properties of SrTiO3 catalysts are correlated to the Sr/Ti atomic ratio. Increasing Sr/Ti ratio in the perovskite?-type SrTiO3 catalysts results in the surface enrichment of Sr element, leading to the the higher content of adsorbed oxygen species on the surface of catalysts and thus higher C2 selectivity for OCM reaction.
文摘The structure and catalytic properties of SrTi0.9M0.1O3- δ (M=Mg,Al, Zr) perovskite type catalysts for oxidative coupling of methane (OCM) have been studied by using X ray diffraction (XRD),X ray photoelectron spectroscopy (XPS) and temperature programmed desorption of oxygen(O2 TPD) methods. It has been shown that doping the cations of lower valence (e.g. Mg2+ , Al3+ ) to the B site of SrTi0.9M0.1O3- δ perovskite type catalysts results in the higher content of adsorbed oxygen species on the surface of catalysts and thus higher C2 selectivity for OCM reaction. It is suggested that the oxygen vacancies of SrTi0.9M0.1O3- δ (M=Mg, Al, Zr) perovskite type catalysts are the sites responsible for oxygen activation, and the adsorbed oxygen species on the surface of SrTi0.9M0.1O3- δ catalysts are the main active species for OCM reaction.
基金supported by the National Natural Science Foundation of China
文摘XRD and XPS are used to study the dispersion state of CuO on ceria surface.The dispersion capacity values of CuO measured by the two methods are consistent,which are of 1.20 mmol CuO/100 m CeO2.In addition,the results reveal that highly dispersed Cu2 + ions are formed at low CuO loadings and that increasing the CuO content to a value higher than its dispersion capacity produces crystalline CuO after the surface vacant sites on CeO2 are filled.The atomic composition of the outermost layer of the CuO/CeO2 samples has been probed by using static secondary ion mass spectroscopy (SSIMS),and the ratios of Cu/Ce are found to be 0.93 and 0.46 for the 1.22 and 0 61 mmol CuO/CeO2 samples respectively.Temperature-programmed reduction (TPR) profile with two reduction peaks at 156 and 16513 suggests that the reduction of highly dispersed Cu2+ ions consists of two steps and is easier than that of CuO crystallites,in which the TPR profile has only one reduction peak at about 249℃.The above experimental results are in good agreement with the prediction of the incorporation model.
文摘Since it was first reported by Keller and Bhasin in 1982 that ethane and ethylene could be produced through direct oxidation of methane, methane oxidative coupling （MOC） has attracted increasing interest in the world. By now some highly efficient catalysts have been explored such as Li/MgO, La<sub>2</sub>O<sub>3</sub>, and [Th, La]O<sub>2-x</sub>, and C<sub>2</sub> yields can reach 15—20％. However, such high yields are obtained at the high temperature of 700—800℃. The kinetic and mechanism studies show that at such high temperature
