CeO2-based oxygen materials were prepared with co-precipitation method and characterized via Brunauer-Emmet Teller(BET)method,X-ray diffraction(XRD)and temperature-programmed reduction(H2-TPR).This paper revealed that...CeO2-based oxygen materials were prepared with co-precipitation method and characterized via Brunauer-Emmet Teller(BET)method,X-ray diffraction(XRD)and temperature-programmed reduction(H2-TPR).This paper revealed that three CeO2-based oxygen storage materials are all forming homogeneous solid solution.Among the samples,CeO2-ZrO2-Al2O3(CZA)has the best textural properties and excellent thermal stability.The specific surface area and pore volume of aged CZA are 90 m2/g and 0.29 mL/g.We proposed a viewpoint:Al3+ might insert among the interspace of fluorite structure or highly dispersal in solid solutions.展开更多
The electrocatalytic activity and stability of Pt/C catalyst modified by using CeO_2-ZrO_2 mixed oxides for the alcohols electrochemical oxidation as probes were investigated. The catalyst samples were characterized b...The electrocatalytic activity and stability of Pt/C catalyst modified by using CeO_2-ZrO_2 mixed oxides for the alcohols electrochemical oxidation as probes were investigated. The catalyst samples were characterized by X-ray diffraction(XRD) and scanning electron microscopy(SEM). The electrochemical properties were measured by a three electrode system on electrochemical workstation(IVIUM). The results showed that the presence of CeO_2-ZrO_2 might be associated with the presence of Pt, which indicated that possibly there was synergistic effect between CeO_2-ZrO_2 and Pt nanoparticles. The electrocatalytic activity and stability of Pt-MO_x/C(M=Ce, Zr) for methanol and ethanol oxidation was better than that of Pt-CeO_2/C, which was attributed to that CeO_2-ZrO_2 composited oxides enhanced oxygen mobility and promoted oxygen storage capacity(OSC). Furthermore, the best performance was found when the molar ratio of CeO_2 to ZrO_2 was 2:1 for the oxidation of methanol and ethanol. The forward peak current density of Pt-MO_x/C(M=Ce, Zr, Ce:Zr=2:1) towards the methanol electrooxidation was about 3.8 times that of Pt-CeO_2/C. Pt-MO_x/C(M=Ce, Zr) appeared to be a promising and less expensive methanol oxidation anode catalyst.展开更多
Hollow CuO-CeO2-ZrO2nano-particles were prepared with supercritical anti-solvent apparatus by using methanol as sol-vent and supercritical carbon dioxide as anti-solvent. Two key factors (i.e., pressure and temperat...Hollow CuO-CeO2-ZrO2nano-particles were prepared with supercritical anti-solvent apparatus by using methanol as sol-vent and supercritical carbon dioxide as anti-solvent. Two key factors (i.e., pressure and temperature) were investigated to explore the effects of catalyst structure and physic-chemical properties (i.e., morphology, reducing property, oxygen storage capacity and specific surface area). The resulting materials were characterized with X-ray diffraction (XRD), high resolution transmission electron micros-copy (HRTEM), Brunauer-Emmett-Teller (BET),hydrogen temperature programmed reduction (H2-TPR) and oxygen storage capac-ity (OSC) measurement, respectively. The experimental results showed that lower temperatures promoted production of hollow struc-ture nano-particulates. The particle morphology also changed significantly, i.e. the solid construction was first transferred to hollow structure then back to solid construction. The optimal conditions for obtaining hollow nano-particles were determined at 45 °C, 18.0–24.0 MPa.展开更多
CeO2-ZeO2 solid solutions are extensively used as oxygen storage promoters in the current automotive three-way catalysts. High thermal stability of the textural properties is one of the most important requirements for...CeO2-ZeO2 solid solutions are extensively used as oxygen storage promoters in the current automotive three-way catalysts. High thermal stability of the textural properties is one of the most important requirements for practical application since temperatures up to 1273 K are easily experienced by these materials under real working conditions. In the present paper, we investigated how hydrothermal treatments applied to cakes of doped and undoped ZrO2-rich CeO2-ZrO2 precursors might improve the thermal stability of the final CeO2-ZrO2 solid solution. A rationale was developed that allowed to correlate the morphology of the hydrothermaUy treated cake with the thermal stability at 1273 K of the final product, which did not depend on the composition of the mixed oxides.展开更多
A series of CeO2-ZrO2-WO3 catalysts for the selective catalytic reduction (SCR) of NO with NH3 were prepared by hydrothermal method. The influence of calcination temperature on the catalytic activity, microstructure...A series of CeO2-ZrO2-WO3 catalysts for the selective catalytic reduction (SCR) of NO with NH3 were prepared by hydrothermal method. The influence of calcination temperature on the catalytic activity, microstructure, surface acidity and redox behavior of CeO2-ZrO2-WO3 catalyst was investigated using various characterization methods. It was found that the CeO2-ZrO2-WO3 catalyst calcined at 600 ℃ showed the best catalytic performance and excellent N2 selectivity, and yielded more than 90% NO conversion in a wide temperature range of 250-500 ℃ with a space velocity (GHSV) of 60000 131. As the calcination temperature was increased from 400 to 600 ℃, the NO conversion obviously increased, but decreased at higher calcination temperature. The results implied that the higher surface area, the strongest synergistic interaction, the superior redox property and the highly dispersed or amorphous WO3 species contributed to the excellent SCR activity of the CeO2-ZrO2-WO3 catalyst calcined at 600℃.展开更多
Praseodymium (Pr) was impregnated to CeO2-ZrO2 solid solution by an impregnation method. The as-obtained Pr modi- fied CeO2-ZrO2 was impregnated with 1 wt.% Pd to prepare the catalysts. The structure and reducibilit...Praseodymium (Pr) was impregnated to CeO2-ZrO2 solid solution by an impregnation method. The as-obtained Pr modi- fied CeO2-ZrO2 was impregnated with 1 wt.% Pd to prepare the catalysts. The structure and reducibility of the fresh and hydrother- really aged catalysts were characterized by X-ray diffraction (XRD), Raman, X-ray photoelectron spectroscopy (XPS), CO chemi- sorption and H2 temperature-programmed reduction (H2-TPR). The oxygen storage capacity (OSC) was evaluated with CO serving as probe gas. Effects of impregnated Pr on the structure and oxygen storage capacity of catalysts were investigated. The results showed that the aged Pr-impregnated samples had much higher OSC and better reducibility than the unmodified ones. The scheme of structural evolutions of the catalysts with and without Pr was also established. Partial of the impregnated Pr diffused into the bulk of CeO2-ZrO2 during ageing, which inhibited the sintering, and increased the amount of oxygen vacancies in CeO2-ZrO2 support. Furthermore, those impregnated Pr species which covered on the surface of the support obstructed the strong metal-support interaction between Pd and Ce so as to reduce the encapsulation of Pd as well as the back spill-over of the oxygen during the catalytic process.展开更多
Nickel and sulfate co-modified CeO2-ZrO2 catalysts were prepared by sol-gel method. The catalysts were characterized by XRD, FTIR, XPS, NH3 chemisorption and NH3-SCR activity tests. The results showed that the enhance...Nickel and sulfate co-modified CeO2-ZrO2 catalysts were prepared by sol-gel method. The catalysts were characterized by XRD, FTIR, XPS, NH3 chemisorption and NH3-SCR activity tests. The results showed that the enhanced acidity of CeO2-ZrO2 catalysts by nickel and sulfate co-modification was responsible for the broadened temperature window and improved the selectivity to N2 in NH3-SCR deNOx. The introduction of nickel to CeO2-ZrO2 solid solutions resulted in more Ce3+ on surface of catalyst, leading to an in...展开更多
摘要CeO2-based oxygen materials were prepared with co-precipitation method and characterized via Brunauer-Emmet Teller(BET)method,X-ray diffraction(XRD)and temperature-programmed reduction(H2-TPR).This paper revealed that three CeO2-based oxygen storage materials are all forming homogeneous solid solution.Among the samples,CeO2-ZrO2-Al2O3(CZA)has the best textural properties and excellent thermal stability.The specific surface area and pore volume of aged CZA are 90 m2/g and 0.29 mL/g.We proposed a viewpoint:Al3+ might insert among the interspace of fluorite structure or highly dispersal in solid solutions.
基金supported by National Natural Science Foundation of China(51474133,21407084)Talent Incubation Funding of School of Materials and Metallurgy(2014CY012)
摘要The electrocatalytic activity and stability of Pt/C catalyst modified by using CeO_2-ZrO_2 mixed oxides for the alcohols electrochemical oxidation as probes were investigated. The catalyst samples were characterized by X-ray diffraction(XRD) and scanning electron microscopy(SEM). The electrochemical properties were measured by a three electrode system on electrochemical workstation(IVIUM). The results showed that the presence of CeO_2-ZrO_2 might be associated with the presence of Pt, which indicated that possibly there was synergistic effect between CeO_2-ZrO_2 and Pt nanoparticles. The electrocatalytic activity and stability of Pt-MO_x/C(M=Ce, Zr) for methanol and ethanol oxidation was better than that of Pt-CeO_2/C, which was attributed to that CeO_2-ZrO_2 composited oxides enhanced oxygen mobility and promoted oxygen storage capacity(OSC). Furthermore, the best performance was found when the molar ratio of CeO_2 to ZrO_2 was 2:1 for the oxidation of methanol and ethanol. The forward peak current density of Pt-MO_x/C(M=Ce, Zr, Ce:Zr=2:1) towards the methanol electrooxidation was about 3.8 times that of Pt-CeO_2/C. Pt-MO_x/C(M=Ce, Zr) appeared to be a promising and less expensive methanol oxidation anode catalyst.
基金supported by the National Natural Science Foundation of China(20976120)Natural Science Foundation of Tianjin(09JCYBJC06200)
摘要Hollow CuO-CeO2-ZrO2nano-particles were prepared with supercritical anti-solvent apparatus by using methanol as sol-vent and supercritical carbon dioxide as anti-solvent. Two key factors (i.e., pressure and temperature) were investigated to explore the effects of catalyst structure and physic-chemical properties (i.e., morphology, reducing property, oxygen storage capacity and specific surface area). The resulting materials were characterized with X-ray diffraction (XRD), high resolution transmission electron micros-copy (HRTEM), Brunauer-Emmett-Teller (BET),hydrogen temperature programmed reduction (H2-TPR) and oxygen storage capac-ity (OSC) measurement, respectively. The experimental results showed that lower temperatures promoted production of hollow struc-ture nano-particulates. The particle morphology also changed significantly, i.e. the solid construction was first transferred to hollow structure then back to solid construction. The optimal conditions for obtaining hollow nano-particles were determined at 45 °C, 18.0–24.0 MPa.
基金supported by the National Natural Science Foundation of China(21173153)National High-Tech Research and Development Program of China(863)(2013AA065304)~~
基金PRIN 2006, "Caratterizzazione spettroscopica e morfologica di Me-POSS eterogeneizzati", MEL Chemicals
摘要CeO2-ZeO2 solid solutions are extensively used as oxygen storage promoters in the current automotive three-way catalysts. High thermal stability of the textural properties is one of the most important requirements for practical application since temperatures up to 1273 K are easily experienced by these materials under real working conditions. In the present paper, we investigated how hydrothermal treatments applied to cakes of doped and undoped ZrO2-rich CeO2-ZrO2 precursors might improve the thermal stability of the final CeO2-ZrO2 solid solution. A rationale was developed that allowed to correlate the morphology of the hydrothermaUy treated cake with the thermal stability at 1273 K of the final product, which did not depend on the composition of the mixed oxides.
基金Project supported by the National Natural Science Foundation of China(21377048,21307047)the Opening Project of Key Laboratory of Green Catalysis of Sichuan Institutes of High Education(LYJ1309)
摘要A series of CeO2-ZrO2-WO3 catalysts for the selective catalytic reduction (SCR) of NO with NH3 were prepared by hydrothermal method. The influence of calcination temperature on the catalytic activity, microstructure, surface acidity and redox behavior of CeO2-ZrO2-WO3 catalyst was investigated using various characterization methods. It was found that the CeO2-ZrO2-WO3 catalyst calcined at 600 ℃ showed the best catalytic performance and excellent N2 selectivity, and yielded more than 90% NO conversion in a wide temperature range of 250-500 ℃ with a space velocity (GHSV) of 60000 131. As the calcination temperature was increased from 400 to 600 ℃, the NO conversion obviously increased, but decreased at higher calcination temperature. The results implied that the higher surface area, the strongest synergistic interaction, the superior redox property and the highly dispersed or amorphous WO3 species contributed to the excellent SCR activity of the CeO2-ZrO2-WO3 catalyst calcined at 600℃.
基金supported by National Natural Science Foundation of China(51202116)Ministry of Science and Technology,China(2010CB732304,2013AA065302)
摘要Praseodymium (Pr) was impregnated to CeO2-ZrO2 solid solution by an impregnation method. The as-obtained Pr modi- fied CeO2-ZrO2 was impregnated with 1 wt.% Pd to prepare the catalysts. The structure and reducibility of the fresh and hydrother- really aged catalysts were characterized by X-ray diffraction (XRD), Raman, X-ray photoelectron spectroscopy (XPS), CO chemi- sorption and H2 temperature-programmed reduction (H2-TPR). The oxygen storage capacity (OSC) was evaluated with CO serving as probe gas. Effects of impregnated Pr on the structure and oxygen storage capacity of catalysts were investigated. The results showed that the aged Pr-impregnated samples had much higher OSC and better reducibility than the unmodified ones. The scheme of structural evolutions of the catalysts with and without Pr was also established. Partial of the impregnated Pr diffused into the bulk of CeO2-ZrO2 during ageing, which inhibited the sintering, and increased the amount of oxygen vacancies in CeO2-ZrO2 support. Furthermore, those impregnated Pr species which covered on the surface of the support obstructed the strong metal-support interaction between Pd and Ce so as to reduce the encapsulation of Pd as well as the back spill-over of the oxygen during the catalytic process.
基金Project supported by the "863 Project" (2009AA06Z304 and 2009AA064801)
摘要Nickel and sulfate co-modified CeO2-ZrO2 catalysts were prepared by sol-gel method. The catalysts were characterized by XRD, FTIR, XPS, NH3 chemisorption and NH3-SCR activity tests. The results showed that the enhanced acidity of CeO2-ZrO2 catalysts by nickel and sulfate co-modification was responsible for the broadened temperature window and improved the selectivity to N2 in NH3-SCR deNOx. The introduction of nickel to CeO2-ZrO2 solid solutions resulted in more Ce3+ on surface of catalyst, leading to an in...