The hollow inverse CeO2/CuO@SiO2 catalysts with different Ce/Cu mass ratios were synthesized by the two-step hydrothermal and incipient wetness impregnation methods,and characterized by multitechnique characterization...The hollow inverse CeO2/CuO@SiO2 catalysts with different Ce/Cu mass ratios were synthesized by the two-step hydrothermal and incipient wetness impregnation methods,and characterized by multitechnique characterizations,such as SEM,TEM,XRD,H2-TPR,XPS and N2 adsorption-desorption techniques.It is found that the hollow shell is composed of CuO and SiO2,and CeO2 nanoparticles are coated on the surface of CuO@SiO2 support.And the CeO2/CuO@SiO2 catalyst with the Ce/Cu mass ratios of 1:1 denoted as 1 CeO2/CuO@SiO2,which possesses a maximum amount of highly dispersed copper species and medium-sized CuO as well as the highest concentration of oxygen vacancies,exhibits the highest catalytic activity and widest full CO conversion window.The barrier effect of the SiO2 shell effectively prevents the reduction of CuO species,which broadens temperature window of CO total conversion and enhances CO2 selectivity above 155℃over the 1 CeO2/CuO@SiO2 catalyst in comparison with the CuO-CeO2 and CeO2-CuO catalysts.展开更多
Three series of CeO2/CuO samples were prepared by impregnation method and characterized by XRD, N2 adsorption-desorption, temperatureprogrammed reduction (TPR), XPS and TEM techniques. In comparison with the samples...Three series of CeO2/CuO samples were prepared by impregnation method and characterized by XRD, N2 adsorption-desorption, temperatureprogrammed reduction (TPR), XPS and TEM techniques. In comparison with the samples prepared with CuO as initial support, the samples with Cu(OH)2 as initial support have higher reducibilities and smaller relative TPR peak areas, and also larger specific surface areas at calcina- tion temperatures of 400 ℃--600 ℃. As a result, Cu(OH)2 is better than CuO as initial support for preferential oxidation of CO in excess H2 (CO-PROX). The best catalytic performance was achieved on the sample calcined at 600 ℃ and with an atomic ratio of Ce/Cu at 40%. XPS analyses indicate that more interface linkages Ce-O-Cu could be formed when it was calcined at 600 ℃. And the atomic ratio of Ce/Cu at 40% led to a proper reducibility for the sample as illustrated by the TPR measurements.展开更多
The CuO/CeO2 catalysts were investigated by means of X-ray diffraction (XRD), laser Raman spectroscopy (LRS), X-ray photoelectronic spectroscopy (XPS), temperature-programmed reduction (TPR), in situ Fourier t...The CuO/CeO2 catalysts were investigated by means of X-ray diffraction (XRD), laser Raman spectroscopy (LRS), X-ray photoelectronic spectroscopy (XPS), temperature-programmed reduction (TPR), in situ Fourier transform infrared spectroscopy (FTIR) and NO+CO reaction. The results revealed that the low temperature (〈150℃) catalytic performances were enhanced for CO pretreated samples. During CO pretreatment, the surface Cu+/Cu0 and oxygen vacancies on ceria surface were present. The low va- lence copper species activated the adsorbed CO and surface oxygen vacancies facilitated the NO dissociation. These effects in turn led to higher activities of CuO/CeO2 for NO reduction. The current study provided helpful understandings of active sites and reaction mechanism in NO+CO reaction.展开更多
A modified CuO/CeO2 catalyst was prepared by surfactant-assisted impregnation method and showed better catalytic activity for low temperature CO oxidation than that from conventional impregnation method. The physicoch...A modified CuO/CeO2 catalyst was prepared by surfactant-assisted impregnation method and showed better catalytic activity for low temperature CO oxidation than that from conventional impregnation method. The physicochemical properties of different CuO/CeO2 catalysts were characterized by thermogravimetrie and differential scanning calorimetric measurements (TG-DSC), X-ray diffraction (XRD), N2 adsorpti0n-desorption, Raman spectroscopy, H2 temperature-programmed reduction (H2-TPR), tern- perature-programmed desorption of 02 (O2-TPD), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The re- sults suggested that the addition of hexadecyl trimethyl ammonium bromide (CTAB) into the impregnation solution could improve the dispersion of CuO species, which could facilitate Cu2+ incorporating into CeO2 lattice and strengthened the synergistic effects between CuO and CeO2, making the lattice oxygen more active, and eventually resulting in enhanced activity for CO oxidation.展开更多
This work described in situ combustion synthesis method for depositing CuO-CeO2 on the FeCrAI honeycomb supports. The influence of the solution concentration and the role of the additive were studied and analyzed by s...This work described in situ combustion synthesis method for depositing CuO-CeO2 on the FeCrAI honeycomb supports. The influence of the solution concentration and the role of the additive were studied and analyzed by scanning electron microscopy (SEM), X-ray diffractometer (XRD), and temperature programmed reduction (TPR) techniques. The results showed that 200 g/L of the active solution was the most appropriate concentration for preparing the monolithic catalysts, and the additives of praseodymium and lanthanum improved the adhesion stability of the monolithic catalysts. The addition of Pr did not greatly affect the catalytic performance, but CO could not be totally converted into CO2 after the addition of La into the CuO-CeO2/Al2O3/FeCrAl catalysts.展开更多
CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were ...CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were examined by means of a microreactor-GC system, HRTEM, XRD, TPR and XPS techniques. The results show that CuO has not catalytic activity and the activity of CeO2 is quite low for CO oxidation. However, the catalytic activity of CuO/CeO2 and Cu/ CeO2 catalysts increases significantly. Furthermore, the activity of CuO/CeO2 is higher than that of Cu/CeO2 catalysts.展开更多
This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 cata...This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 catalysts with yttrium content in the range of 0-5wt.%. Properties of the obtained samples were characterized and analyzed by X-ray diffraction (XRD), Raman spectroscopy, H2-TPR, cyclic voltammetry (CV) and the BET method. The results revealed that catalytic activity was increased with the yttrium content at first, but then decreased with the further increase of yttrium content. Herein, CuO/CeO2 catalyst doped with 2wt.% of yttrium showed the highest catalytic activity (CO conversion reaches 93.4% at 250 ℃) and thermal stability for WGS reaction. The catalytic activity was correlated with the surface area, the area of peak γ of H2-TPR profile (i.e., the reduction of surface copper oxide (crystalline forms) interacted with surface oxygen vacancies on ceria), and the area of peak C2 and A1 (Cu^0→←Cu^2+ in cyclic voltammetry process), respectively. Besides, Raman spectra provided evidences for a synergistic Cu-Ovacancy interaction, and it was indicated that doping yttrium may facilitate the formation of oxygen vacancies on ceria.展开更多
基金Project supported by the National Natural Science Foundation of China(21466024)the Natural Science Foundation of Inner Mongolia(2018MS02020,2018BS02008)
摘要The hollow inverse CeO2/CuO@SiO2 catalysts with different Ce/Cu mass ratios were synthesized by the two-step hydrothermal and incipient wetness impregnation methods,and characterized by multitechnique characterizations,such as SEM,TEM,XRD,H2-TPR,XPS and N2 adsorption-desorption techniques.It is found that the hollow shell is composed of CuO and SiO2,and CeO2 nanoparticles are coated on the surface of CuO@SiO2 support.And the CeO2/CuO@SiO2 catalyst with the Ce/Cu mass ratios of 1:1 denoted as 1 CeO2/CuO@SiO2,which possesses a maximum amount of highly dispersed copper species and medium-sized CuO as well as the highest concentration of oxygen vacancies,exhibits the highest catalytic activity and widest full CO conversion window.The barrier effect of the SiO2 shell effectively prevents the reduction of CuO species,which broadens temperature window of CO total conversion and enhances CO2 selectivity above 155℃over the 1 CeO2/CuO@SiO2 catalyst in comparison with the CuO-CeO2 and CeO2-CuO catalysts.
摘要Three series of CeO2/CuO samples were prepared by impregnation method and characterized by XRD, N2 adsorption-desorption, temperatureprogrammed reduction (TPR), XPS and TEM techniques. In comparison with the samples prepared with CuO as initial support, the samples with Cu(OH)2 as initial support have higher reducibilities and smaller relative TPR peak areas, and also larger specific surface areas at calcina- tion temperatures of 400 ℃--600 ℃. As a result, Cu(OH)2 is better than CuO as initial support for preferential oxidation of CO in excess H2 (CO-PROX). The best catalytic performance was achieved on the sample calcined at 600 ℃ and with an atomic ratio of Ce/Cu at 40%. XPS analyses indicate that more interface linkages Ce-O-Cu could be formed when it was calcined at 600 ℃. And the atomic ratio of Ce/Cu at 40% led to a proper reducibility for the sample as illustrated by the TPR measurements.
基金supported by National Basic Research Program of China(2010CB732300)National Natural Science Foundation of China(21273110,20973091)Natural Science Foundation for the Youth(21203091)
摘要The CuO/CeO2 catalysts were investigated by means of X-ray diffraction (XRD), laser Raman spectroscopy (LRS), X-ray photoelectronic spectroscopy (XPS), temperature-programmed reduction (TPR), in situ Fourier transform infrared spectroscopy (FTIR) and NO+CO reaction. The results revealed that the low temperature (〈150℃) catalytic performances were enhanced for CO pretreated samples. During CO pretreatment, the surface Cu+/Cu0 and oxygen vacancies on ceria surface were present. The low va- lence copper species activated the adsorbed CO and surface oxygen vacancies facilitated the NO dissociation. These effects in turn led to higher activities of CuO/CeO2 for NO reduction. The current study provided helpful understandings of active sites and reaction mechanism in NO+CO reaction.
基金supported by the National Natural Science Foundation of China(21273150)‘‘Shu Guang’’Project(10GG23)of Shanghai Municipal Education CommissionShanghai Education Development Foundation
摘要A modified CuO/CeO2 catalyst was prepared by surfactant-assisted impregnation method and showed better catalytic activity for low temperature CO oxidation than that from conventional impregnation method. The physicochemical properties of different CuO/CeO2 catalysts were characterized by thermogravimetrie and differential scanning calorimetric measurements (TG-DSC), X-ray diffraction (XRD), N2 adsorpti0n-desorption, Raman spectroscopy, H2 temperature-programmed reduction (H2-TPR), tern- perature-programmed desorption of 02 (O2-TPD), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The re- sults suggested that the addition of hexadecyl trimethyl ammonium bromide (CTAB) into the impregnation solution could improve the dispersion of CuO species, which could facilitate Cu2+ incorporating into CeO2 lattice and strengthened the synergistic effects between CuO and CeO2, making the lattice oxygen more active, and eventually resulting in enhanced activity for CO oxidation.
基金Project supported by the National Key Basic Research Program (973 Program,2009CB226112)National Natural Science Foundation of China (21066004)Scientific Research Start Foundation of High-level Introduction Talent of Inner Mongolia University(Grant No.207062) for funding this research
摘要This work described in situ combustion synthesis method for depositing CuO-CeO2 on the FeCrAI honeycomb supports. The influence of the solution concentration and the role of the additive were studied and analyzed by scanning electron microscopy (SEM), X-ray diffractometer (XRD), and temperature programmed reduction (TPR) techniques. The results showed that 200 g/L of the active solution was the most appropriate concentration for preparing the monolithic catalysts, and the additives of praseodymium and lanthanum improved the adhesion stability of the monolithic catalysts. The addition of Pr did not greatly affect the catalytic performance, but CO could not be totally converted into CO2 after the addition of La into the CuO-CeO2/Al2O3/FeCrAl catalysts.
基金Projected supported by the National Natural Science Foundation of China (20271028) and Tianjin Natural Science Foundation(033602511)
摘要CeO2 was synthesized via sol-gel process and used as supporter to prepare CuO/CeO2, Cu/CeO2 catalysts by impregnation method. The catalytic properties and characterization of CeO2, CuO/CeO2 and Cu/CeO2 catalysts were examined by means of a microreactor-GC system, HRTEM, XRD, TPR and XPS techniques. The results show that CuO has not catalytic activity and the activity of CeO2 is quite low for CO oxidation. However, the catalytic activity of CuO/CeO2 and Cu/ CeO2 catalysts increases significantly. Furthermore, the activity of CuO/CeO2 is higher than that of Cu/CeO2 catalysts.
基金supported by the National Natural Science Foundation of China (20771025)A-type Science and Technology Projects of Fujian Provincial Department of Education (JA08021)
摘要This paper presented a study on the role of yttrium addition to CuO/CeO2 catalyst for water-gas shift reaction. A single-step co-precipitation method was used for preparation of a series of yttrium doped CuO/CeO2 catalysts with yttrium content in the range of 0-5wt.%. Properties of the obtained samples were characterized and analyzed by X-ray diffraction (XRD), Raman spectroscopy, H2-TPR, cyclic voltammetry (CV) and the BET method. The results revealed that catalytic activity was increased with the yttrium content at first, but then decreased with the further increase of yttrium content. Herein, CuO/CeO2 catalyst doped with 2wt.% of yttrium showed the highest catalytic activity (CO conversion reaches 93.4% at 250 ℃) and thermal stability for WGS reaction. The catalytic activity was correlated with the surface area, the area of peak γ of H2-TPR profile (i.e., the reduction of surface copper oxide (crystalline forms) interacted with surface oxygen vacancies on ceria), and the area of peak C2 and A1 (Cu^0→←Cu^2+ in cyclic voltammetry process), respectively. Besides, Raman spectra provided evidences for a synergistic Cu-Ovacancy interaction, and it was indicated that doping yttrium may facilitate the formation of oxygen vacancies on ceria.