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
Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, ...Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, BET, SEM, TEM, DTA-TG and CO2-TPD were used to characterize the catalysts. CH4-CO2 reforming to synthesis gas （syngas） was performed to test the catalytic behavior of the catalysts. The catalyst Pt-CZ/MgO-IE（D） prepared using ion exchange resin exhibits more regular structure, smaller and more unique particle sizes, and stronger basicity than the catalyst Pt-CZ/MgO prepared from commercial MgO. At 1073 K and atmospheric pressure, Pt-CZ/MgO-IE（D） catalyst has a higher activity and greater stability than Pt-CZ/MgO catalyst for CH4-CO2 reforming reaction at high gas hourly space velocity of 36000 mL/（g.h） with a stoichiometric feed of CH4 and C02. Activity measurement and characterization results demonstrate that modification of the support using ion exchange resin method can promote the surface structural property and stability, therefore enhancing the activity and stability for CH4-CO2 reforming reaction.展开更多
Larger amounts of alkalis, alkali earth metals and sulfides in flue gas from glass furnace were easier to deactivate selective catalytic reduction （SCR） catalyst compared to the flue gases from other stationary sour...Larger amounts of alkalis, alkali earth metals and sulfides in flue gas from glass furnace were easier to deactivate selective catalytic reduction （SCR） catalyst compared to the flue gases from other stationary sources. Catalyst regeneration has been an emerging research topic for flue gas denitrification in glass furnace. Regeneration of the deactivated TiO2-ZrO2-CeO2 /Al2TiO 5 -TiO2-SiO2 （ATS） complex phase ceramics catalysts used for NH3 -SCR of NO x in glass furnace was studied in this work. Effects of regeneration methods, including washing with different aqueous solutions and sulfuric acid, thermal regeneration, thermal reduction regeneration, and thermal regeneration with SO2 , on catalytic performance were comparatively investigated. In comparison of catalytic activities between the catalysts before and after regeneration, results showed that washing was the most effective regeneration method, and the sulfuric acid concentration of the washing solution was an important factor. Washing time directly affected catalyst regeneration efficiency and catalyst life. The regenerated TiO2-ZrO2 -CeO2 /ATS catalyst regained more than 90% NO conversion after being washed with 10 wt.% H2SO4 for 30 min.展开更多
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
Sub-micrometer ultra fine CeO2-ZrO2 mixed oxides have been prepared by milling solid cerium carbonate and zirconium oxy-chloride with ammonia and followed by filtering, drying and calcining procedures. The effects of ...Sub-micrometer ultra fine CeO2-ZrO2 mixed oxides have been prepared by milling solid cerium carbonate and zirconium oxy-chloride with ammonia and followed by filtering, drying and calcining procedures. The effects of Ce/Zr molar ratio, milling time and calcining temperature on the phase composition, particle size and morphology, surface charge, as well as the polishing property were investigated. The results show that the mixed oxide calcined at 1 000 ℃ is composed of cubic ceria doped with zirconium and tetragonal zirconia doped with cerium, and the phase composition varies with calcination temperature and the Ce/Zr molar ratio. The monoclinic zirconia is observed when decreasing calcination temperature and shortening milling time, demonstrating that milling and calcining can force the phase transformation from monoclinic zirconia to cerium stabilized tetragonal zirconia and zirconium doped cubic ceria solid solutions. The removal rate for the optical glass polishing varies with Ce/Zr molar ratio. A synergetic polishing effect is found when Ce/Zr molar ratio below 4, and the optimal Ce/Zr molar ratio is 1∶1. At the same time, the cubic ceria content, density, particle size and surface charge all increase when calcination temperature increasing from 800 ℃ to 1 100 ℃. However, the particle morphology changes from disperse quasi-sphere to irregular aggregation and the maximal removal rate for optical glass polishing lies at 1 000 ℃.These facts show that the polishing property of the synthesized ceria-zirconia mixed oxide is affected by the particle physical characteristics comprehensively.展开更多
基金supported by the National Natural Science Foundation of China(20976120)Natural Science Foundation of Tianjin(09JCYBJC06200)
文摘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 (No. 20873013)
文摘Pt-CeO2-ZrO2/MgO （Pt-CZ/MgO） catalysts with 0.8 wt% Pt, 3.0 wt% CeO2 and 3.0 wt% ZrO2 were prepared by wet impregnation method. Support MgO was obtained using ion exchange resin method or using commercial MgO. XRD, BET, SEM, TEM, DTA-TG and CO2-TPD were used to characterize the catalysts. CH4-CO2 reforming to synthesis gas （syngas） was performed to test the catalytic behavior of the catalysts. The catalyst Pt-CZ/MgO-IE（D） prepared using ion exchange resin exhibits more regular structure, smaller and more unique particle sizes, and stronger basicity than the catalyst Pt-CZ/MgO prepared from commercial MgO. At 1073 K and atmospheric pressure, Pt-CZ/MgO-IE（D） catalyst has a higher activity and greater stability than Pt-CZ/MgO catalyst for CH4-CO2 reforming reaction at high gas hourly space velocity of 36000 mL/（g.h） with a stoichiometric feed of CH4 and C02. Activity measurement and characterization results demonstrate that modification of the support using ion exchange resin method can promote the surface structural property and stability, therefore enhancing the activity and stability for CH4-CO2 reforming reaction.
基金supported by the National Natural Science Foundation of China(21273043,21077026)Science and Technology Commission of Shanghai Municipality,China(13DZ2275200)~~
基金Project supported by National Natural Science Foundation of China(51272105,51172107,21106071)the New Teachers'Fund for Doctor Stations Sponsored by the Ministry of Education of China(20113221120004)+1 种基金the National Key Technology R&D Program of China(2012BAE01B03)the Supporting Program for Sci&Tech Research of Jiangsu Province of China(2011023)
文摘Larger amounts of alkalis, alkali earth metals and sulfides in flue gas from glass furnace were easier to deactivate selective catalytic reduction （SCR） catalyst compared to the flue gases from other stationary sources. Catalyst regeneration has been an emerging research topic for flue gas denitrification in glass furnace. Regeneration of the deactivated TiO2-ZrO2-CeO2 /Al2TiO 5 -TiO2-SiO2 （ATS） complex phase ceramics catalysts used for NH3 -SCR of NO x in glass furnace was studied in this work. Effects of regeneration methods, including washing with different aqueous solutions and sulfuric acid, thermal regeneration, thermal reduction regeneration, and thermal regeneration with SO2 , on catalytic performance were comparatively investigated. In comparison of catalytic activities between the catalysts before and after regeneration, results showed that washing was the most effective regeneration method, and the sulfuric acid concentration of the washing solution was an important factor. Washing time directly affected catalyst regeneration efficiency and catalyst life. The regenerated TiO2-ZrO2 -CeO2 /ATS catalyst regained more than 90% NO conversion after being washed with 10 wt.% H2SO4 for 30 min.
文摘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.
文摘Sub-micrometer ultra fine CeO2-ZrO2 mixed oxides have been prepared by milling solid cerium carbonate and zirconium oxy-chloride with ammonia and followed by filtering, drying and calcining procedures. The effects of Ce/Zr molar ratio, milling time and calcining temperature on the phase composition, particle size and morphology, surface charge, as well as the polishing property were investigated. The results show that the mixed oxide calcined at 1 000 ℃ is composed of cubic ceria doped with zirconium and tetragonal zirconia doped with cerium, and the phase composition varies with calcination temperature and the Ce/Zr molar ratio. The monoclinic zirconia is observed when decreasing calcination temperature and shortening milling time, demonstrating that milling and calcining can force the phase transformation from monoclinic zirconia to cerium stabilized tetragonal zirconia and zirconium doped cubic ceria solid solutions. The removal rate for the optical glass polishing varies with Ce/Zr molar ratio. A synergetic polishing effect is found when Ce/Zr molar ratio below 4, and the optimal Ce/Zr molar ratio is 1∶1. At the same time, the cubic ceria content, density, particle size and surface charge all increase when calcination temperature increasing from 800 ℃ to 1 100 ℃. However, the particle morphology changes from disperse quasi-sphere to irregular aggregation and the maximal removal rate for optical glass polishing lies at 1 000 ℃.These facts show that the polishing property of the synthesized ceria-zirconia mixed oxide is affected by the particle physical characteristics comprehensively.
