Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion)...Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in cata- lytic decomposition of N2O. CZM-AC(II) (prepared by ammoniacal copper (II) complex ion) with 9.4 wt% Cu con- tent was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 400 ℃. CZM-CA (prepared using Cu( CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 425 ℃. CZM-CC, CZM- CN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500 ℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(II) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.展开更多
Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and fiel...Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and field emission scanning electron microscopy. XPS analysis revealed that surface nickel is present in three forms: metal particles, NiO and Ni(OH)2. It is suggested that nickel(0) valent atoms are essential for the interaction with N2O molecules at the catalyst surfaces. Bare NiO exhibited a very low N2O decomposition reactivity. However, the alkali-containing catalysts exhibited a marked activity enhancement.展开更多
CePO4 (in particular, monoclinic CePO4) has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds (prepared by precipitation) in ai...CePO4 (in particular, monoclinic CePO4) has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds (prepared by precipitation) in air at 900 ℃. Monoclinic CePO4 nanowires were prepared by calcining hexagonal CePO4 nanowires (prepared by hydrothermal synthesis at 150 ℃) in air at 900 ℃. Both monoclinic CePO4 materials were used to support Rh2O3 by impregnation using Rh(NO3)3 as a precursor (followed by calcination). The catalytic performance of Rh2O3/monoclinic CePO4 composite materials in N2O decomposition and CO oxidation was investigated. It was found that Rh2O3 supported on monoclinic CePO4 nanowims was much more active than Rh2O3 supported on monoclinic CePO4 nanoparticles. The stability of catalysts as a function of reaction time on stream was studied in both reactions. The influence of co-fed CO2, O2, and H2O on the catalytic activity in N20 decomposition was also studied. These catalysts were characterized by employing N2 adsorption-desorption, ICP-OES, XRD, TEM, XPS, H2-TPR, O2-TPD, and CO2-TPD. The correlation between physicochemical properties and catalytic properties was discussed.展开更多
Recently,a one-pot self-assembly method was proposed for the synthesis of mesoporous Al2O3 and MOx-Al2O3 composite materials.However,few attempts have been made to use mesoporous MOx-Al2O3 composites to support metal ...Recently,a one-pot self-assembly method was proposed for the synthesis of mesoporous Al2O3 and MOx-Al2O3 composite materials.However,few attempts have been made to use mesoporous MOx-Al2O3 composites to support metal oxides for catalysis.In the present work,mesoporous MOx-Al2O3(M = Mn,Fe,Co,Ni,Cu,Ba)materials were prepared by a one-pot self-assembly method using Pluronic P123 as a structure-directing agent.The obtained mesoporous materials were loaded with Rh2O3 nanoparticles via impregnation with Rh(NO3)3 followed by calcination in air at 500°C.The resulting catalysts were characterized by X-ray diffraction,N2 adsorption-desorption measurements,transmission electron microscopy,inductively coupled plasma optical emission spectrometry,X-ray photoelectron spectroscopy,and their catalytic activity and stability for CO oxidation and N2O decomposition were tested.The Rh2O3 nanoparticles were found to be on the order of1 nm in size and were highly dispersed on the high surface area mesoporous MOx-Al2O3 supports.A number of the Rh2O3/mesoporous MOx-Al2O3 catalysts exhibited higher catalytic activity than the Rh2O3/mesoporous Al2O3 prepared for comparison.展开更多
Hexagonal CePO4 nanorods were prepared by a precipitation method and hexagonal CePO4 nanowires were prepared by hydrothermal synthesis at 150 ℃. Rh (NO3)3 was then used as a precursor for the impregnation of Rh203 ...Hexagonal CePO4 nanorods were prepared by a precipitation method and hexagonal CePO4 nanowires were prepared by hydrothermal synthesis at 150 ℃. Rh (NO3)3 was then used as a precursor for the impregnation of Rh203 onto these CePO4 materials. The Rh203 supported on the CePO4 nanowires was much more active for the catalytic decomposition of N20 than the RhzO3 supported on CePO4 nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO2, O2, H20 or O2/H20) on the N20 decomposition was also investigated. The samples were characterized by N2 adsorption-desorption, induc- tively coupled plasma optical emission spectroscopy, X- ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-pro- grammed reduction, oxygen temperature-programmed desorption, and CO2 temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.展开更多
Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on...Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.展开更多
基金Supported by the National Natural Science Foundation of China(Grant No.21477022)
文摘Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in cata- lytic decomposition of N2O. CZM-AC(II) (prepared by ammoniacal copper (II) complex ion) with 9.4 wt% Cu con- tent was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 400 ℃. CZM-CA (prepared using Cu( CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 425 ℃. CZM-CC, CZM- CN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500 ℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(II) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.
文摘Direct N2O decomposition has been investigated over bare NiO and a series of its alkali-promoted catalysts. These catalysts were characterized by X-ray diffractometry, X-ray photoelectron spectroscopy (XPS) and field emission scanning electron microscopy. XPS analysis revealed that surface nickel is present in three forms: metal particles, NiO and Ni(OH)2. It is suggested that nickel(0) valent atoms are essential for the interaction with N2O molecules at the catalyst surfaces. Bare NiO exhibited a very low N2O decomposition reactivity. However, the alkali-containing catalysts exhibited a marked activity enhancement.
基金Supported by the National Natural Science Foundation of China(21177028,21477022)
文摘CePO4 (in particular, monoclinic CePO4) has been rarely used to make supported catalysts. Herein, monoclinic CeP04 nanoparticles were prepared by calcining hexagonal CePO4 nanomds (prepared by precipitation) in air at 900 ℃. Monoclinic CePO4 nanowires were prepared by calcining hexagonal CePO4 nanowires (prepared by hydrothermal synthesis at 150 ℃) in air at 900 ℃. Both monoclinic CePO4 materials were used to support Rh2O3 by impregnation using Rh(NO3)3 as a precursor (followed by calcination). The catalytic performance of Rh2O3/monoclinic CePO4 composite materials in N2O decomposition and CO oxidation was investigated. It was found that Rh2O3 supported on monoclinic CePO4 nanowims was much more active than Rh2O3 supported on monoclinic CePO4 nanoparticles. The stability of catalysts as a function of reaction time on stream was studied in both reactions. The influence of co-fed CO2, O2, and H2O on the catalytic activity in N20 decomposition was also studied. These catalysts were characterized by employing N2 adsorption-desorption, ICP-OES, XRD, TEM, XPS, H2-TPR, O2-TPD, and CO2-TPD. The correlation between physicochemical properties and catalytic properties was discussed.
基金supported by the National Natural Science Foundation of China (21177028)~~国家自然科学基金(21177028)
文摘Recently,a one-pot self-assembly method was proposed for the synthesis of mesoporous Al2O3 and MOx-Al2O3 composite materials.However,few attempts have been made to use mesoporous MOx-Al2O3 composites to support metal oxides for catalysis.In the present work,mesoporous MOx-Al2O3(M = Mn,Fe,Co,Ni,Cu,Ba)materials were prepared by a one-pot self-assembly method using Pluronic P123 as a structure-directing agent.The obtained mesoporous materials were loaded with Rh2O3 nanoparticles via impregnation with Rh(NO3)3 followed by calcination in air at 500°C.The resulting catalysts were characterized by X-ray diffraction,N2 adsorption-desorption measurements,transmission electron microscopy,inductively coupled plasma optical emission spectrometry,X-ray photoelectron spectroscopy,and their catalytic activity and stability for CO oxidation and N2O decomposition were tested.The Rh2O3 nanoparticles were found to be on the order of1 nm in size and were highly dispersed on the high surface area mesoporous MOx-Al2O3 supports.A number of the Rh2O3/mesoporous MOx-Al2O3 catalysts exhibited higher catalytic activity than the Rh2O3/mesoporous Al2O3 prepared for comparison.
文摘Hexagonal CePO4 nanorods were prepared by a precipitation method and hexagonal CePO4 nanowires were prepared by hydrothermal synthesis at 150 ℃. Rh (NO3)3 was then used as a precursor for the impregnation of Rh203 onto these CePO4 materials. The Rh203 supported on the CePO4 nanowires was much more active for the catalytic decomposition of N20 than the RhzO3 supported on CePO4 nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO2, O2, H20 or O2/H20) on the N20 decomposition was also investigated. The samples were characterized by N2 adsorption-desorption, induc- tively coupled plasma optical emission spectroscopy, X- ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-pro- grammed reduction, oxygen temperature-programmed desorption, and CO2 temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.
基金supported by the Hi-Tech Research and Development Program (863) of China (No. 2012AA062501)the Natural Science Foundation of Hubei Province (No. 2009CDB246)the Postgraduates Innovation Foundation of Huazhong University of Science and Technology of China (No. HF-08-11-2011-261)
文摘Three groups of cobalt mixed oxide catalysts(Mg/Zn-Co, Mg/Zn-Ce-C, K/Na-Mg/Zn-Ce-Co)were prepared by sol-gel or impregnation methods. The synergistic effects of transition metal, rare earth metal and alkali metal on cobalt mixed catalysts for nitrous oxide(N2O)decomposing to N2 and O2were investigated. The experimental results revealed that the catalytic activity for N2 O decomposition was promoted as Co2+was replaced partially by Zn2+/Mg2+, moreover, the characterization analysis by XRD and XPS showed that Zn2+/Mg2+replaced Co2+successfully into the spinel structure of Co3O4 and promoted significantly the catalytic activity. Especially, the addition of CeO2 and K2O/Na2O decreased the binding energy and resulted in an increase in the density of the electron cloud around Co and an improvement of the catalytic activity. Of the investigated cobalt mixed catalysts, the best catalytic activity was shown by 2% K-Zn0.5-Ce0.05-Co catalyst.