A new catalyst of Co/La_(4)Ga_(2)O_(9) for CO_(2) hydrogenation to produce ethanol was prepared by reducing LaCo^(0).5 Ga0.5 O3,which showed excellent selectivity to ethanol(%35 C-mol%)at mild reaction conditions(270&...A new catalyst of Co/La_(4)Ga_(2)O_(9) for CO_(2) hydrogenation to produce ethanol was prepared by reducing LaCo^(0).5 Ga0.5 O3,which showed excellent selectivity to ethanol(%35 C-mol%)at mild reaction conditions(270°C,3.5 MPa,3000 m L g-1 h-1).The catalysts were characterized by N_(2) adsorption/desorption,XRD,XAFS,CO and CO_(2)-TPD,H2 chemisorption,XPS and TEM techniques.The interaction between Co nanoparticles(NPs)and La2+4 Ga_(2)O_(9) oxide resulted in Co^(0)-Coon the surface of Co NPs.It was proposed that La_(4)Ga_(2)O_(9) could catalyze reverse water gas shift reaction(r-WGS),which converted CO_(2) to CO.Then,the CO migrated to Co^(0)-Co^(2+)on Co NPs,where it was hydrogenated to form ethanol like higher alcohols synthesis from syngas.The results suggest that by controlling the oxidation state of cobalt,and combined with a kind of active site for activating CO_(2) to form CO,a catalyst with excellent selectivity to ethanol could be obtained for CO_(2) hydrogenation,which means that the complex reaction may be proceed with high selectivity using only one active metal component.展开更多
The key point in CO2 methanation is to improve the activity at low temperature and the stability.For this purpose,a new cerium-modified Ni-La2O3/ZrO2 catalyst was prepared using La1-xCexNiO3/ZrO2 with perovskite phase...The key point in CO2 methanation is to improve the activity at low temperature and the stability.For this purpose,a new cerium-modified Ni-La2O3/ZrO2 catalyst was prepared using La1-xCexNiO3/ZrO2 with perovskite phase as the precursor,which was obtained by citrate complexation combined with an impregnation method.The resulting catalyst was characterized through Nitrogen adsorption and desorption,X-ray diffraction (XRD),Transmission electron microscopy (TEM),Hydrogen temperature programmed reduction (H2-TPR),Temperature-programmed desorption of CO2 (CO2-TPD) and that of H2 (H2-TPD),and X-ray photoelectron spectroscopy (XPS) techniques,and the catalytic performances for CO2 methanation was investigated.Cerium modification could improve the effective activation of CO2,thus enhancing the activity at low temperature for CO2 methanation.The metal Ni nanoparticles prepared using this method were highly dispersed and showed excellent resistance to sintering,leading to very good stability,which could be attributed to the following:Ni nanoparticles could be confined by cerium-modified La2O3;La2O3could be confined by the cerium ions at the La2O3/ZrO2 interface;and the cerium ions were confined by ZrO2.展开更多
A new scheme for the preparation of highly dispersed precious metal catalysts is proposed in this work. Samples of LaCol-xPtxO3/SiO2 （x = 0.03, 0.05, 0.07, 0.09, and 0.10） were prepared through a simple method of ci...A new scheme for the preparation of highly dispersed precious metal catalysts is proposed in this work. Samples of LaCol-xPtxO3/SiO2 （x = 0.03, 0.05, 0.07, 0.09, and 0.10） were prepared through a simple method of citrate acid complexa-tion combined with impregnation. In a nanocrystallite of LaCOl-xPtxO3, ions of lanthanum, cobalt, and platinum are evenly mixed at the atomic level and confined within the nanocrystallite. In the reduction process, platinum ions were reduced and migrated onto the surface of the nanocrystallite, and the platinum should be highly dispersed owing to the even mixing of the platinum ions in the precursor. When x = 0.05 or lower, the highest dispersion of Pt could be achieved. The highly dispersed Pt is stable, because of the strong interaction between Pt atoms and the support. The catalysts were characterized by BET surface area, temperature-programmed reduction, X-ray diffraction, transmission electron microscopy, CO temperature-programmed desorption, and turnover frequency. Compared with general precious metal Pt catalysts, the LaCo0.95Pt0.05O3/ SiO2 catalyst exhibited better activity for CO oxidation, and it maintained stability at a high temperature of 400 ℃ for 250 h with complete CO conversion.展开更多
基金the National Natural Science Foundation of China(Nos.21872101,21962014)Tianjin science and technology commission(No.18JCZDJC31300)Beijing Synchrotron Radiation Facility(BSRF)。
文摘A new catalyst of Co/La_(4)Ga_(2)O_(9) for CO_(2) hydrogenation to produce ethanol was prepared by reducing LaCo^(0).5 Ga0.5 O3,which showed excellent selectivity to ethanol(%35 C-mol%)at mild reaction conditions(270°C,3.5 MPa,3000 m L g-1 h-1).The catalysts were characterized by N_(2) adsorption/desorption,XRD,XAFS,CO and CO_(2)-TPD,H2 chemisorption,XPS and TEM techniques.The interaction between Co nanoparticles(NPs)and La2+4 Ga_(2)O_(9) oxide resulted in Co^(0)-Coon the surface of Co NPs.It was proposed that La_(4)Ga_(2)O_(9) could catalyze reverse water gas shift reaction(r-WGS),which converted CO_(2) to CO.Then,the CO migrated to Co^(0)-Co^(2+)on Co NPs,where it was hydrogenated to form ethanol like higher alcohols synthesis from syngas.The results suggest that by controlling the oxidation state of cobalt,and combined with a kind of active site for activating CO_(2) to form CO,a catalyst with excellent selectivity to ethanol could be obtained for CO_(2) hydrogenation,which means that the complex reaction may be proceed with high selectivity using only one active metal component.
基金supported by the National Natural Science Foundation of China(Nos.21872101,21576192)the Natural Science Foundation of Tianjin(18JCZDJC31300)。
文摘The key point in CO2 methanation is to improve the activity at low temperature and the stability.For this purpose,a new cerium-modified Ni-La2O3/ZrO2 catalyst was prepared using La1-xCexNiO3/ZrO2 with perovskite phase as the precursor,which was obtained by citrate complexation combined with an impregnation method.The resulting catalyst was characterized through Nitrogen adsorption and desorption,X-ray diffraction (XRD),Transmission electron microscopy (TEM),Hydrogen temperature programmed reduction (H2-TPR),Temperature-programmed desorption of CO2 (CO2-TPD) and that of H2 (H2-TPD),and X-ray photoelectron spectroscopy (XPS) techniques,and the catalytic performances for CO2 methanation was investigated.Cerium modification could improve the effective activation of CO2,thus enhancing the activity at low temperature for CO2 methanation.The metal Ni nanoparticles prepared using this method were highly dispersed and showed excellent resistance to sintering,leading to very good stability,which could be attributed to the following:Ni nanoparticles could be confined by cerium-modified La2O3;La2O3could be confined by the cerium ions at the La2O3/ZrO2 interface;and the cerium ions were confined by ZrO2.
基金supported by the National Natural Science Foundation of China(Nos.21576192,21776214)
文摘A new scheme for the preparation of highly dispersed precious metal catalysts is proposed in this work. Samples of LaCol-xPtxO3/SiO2 （x = 0.03, 0.05, 0.07, 0.09, and 0.10） were prepared through a simple method of citrate acid complexa-tion combined with impregnation. In a nanocrystallite of LaCOl-xPtxO3, ions of lanthanum, cobalt, and platinum are evenly mixed at the atomic level and confined within the nanocrystallite. In the reduction process, platinum ions were reduced and migrated onto the surface of the nanocrystallite, and the platinum should be highly dispersed owing to the even mixing of the platinum ions in the precursor. When x = 0.05 or lower, the highest dispersion of Pt could be achieved. The highly dispersed Pt is stable, because of the strong interaction between Pt atoms and the support. The catalysts were characterized by BET surface area, temperature-programmed reduction, X-ray diffraction, transmission electron microscopy, CO temperature-programmed desorption, and turnover frequency. Compared with general precious metal Pt catalysts, the LaCo0.95Pt0.05O3/ SiO2 catalyst exhibited better activity for CO oxidation, and it maintained stability at a high temperature of 400 ℃ for 250 h with complete CO conversion.
