In order to develop a catalyst with high activity for catalytic wet oxidation (CWO) process at room temperature and atmospheric pressure, Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst was prepared by consecutive impregnation me...In order to develop a catalyst with high activity for catalytic wet oxidation (CWO) process at room temperature and atmospheric pressure, Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst was prepared by consecutive impregnation method and the prepared parameters were optimized. The structure of the catalyst was characterized by BET, XRF, SEM and XPS technologies, and the actual wastewater was used to investigate the catalytic activity of Fe2O3-CeO2-TiO2/γ-Al2O3 in CWO process. The experimental results showed that the prepared catalyst exhibited good catalytic activity when the doping amount of Ti was 1.0 wt% (the weight ratio of Ti to carriers), and the middle product, Fe2O3-CeO2-TiO2/γ-Al2O3, was calcined in 450℃ for 2 h. The CWO experiment for treating actual dye wastewater indicated that the COD, color and TOC of actual wastewater were decreased by 62.23%, 50.12% and 41.26% in 3 h, respectively, and the ratio of BOD5/COD was increased from 0.19 to 0.30.展开更多
Ce0.67Zr0.33O2-Al2O3 solid solution was prepared by the co-precipitation method. Fe2O3-based catalysts supported on the solid solution were obtained by the impregnation method. The article revealed that the optimal lo...Ce0.67Zr0.33O2-Al2O3 solid solution was prepared by the co-precipitation method. Fe2O3-based catalysts supported on the solid solution were obtained by the impregnation method. The article revealed that the optimal loading amount of Fe2O3 on Ce0.67Zr0.33 O2-Al2O3 in our experimental condition for catalytic combustion of methane was 8% ( mass fraction). The prepared catalysts were characterized by BET, TPR, XRD analyses, and their catalytic activity was investigated after being calcined at 873 K and after being aged in water gas at 1273 K. When the loading amount of Fe203 was 8% ( mass fraction), the catalyst held the highest activity, and the best temperature speciality and thermal stability. The complete-conversion temperature of methane for fresh and aged sample was 788 and 838 K, respectively. The range between the light-off temperature and the complete-conversion temperature was only 15 K. The characterization results of XRD indicated that Fe2O3 was well dispersed on the Ce0.67Zr0.33O2-Al2O3 matrix. The results of BET and TPR were in good harmony with the catalytic activity results.展开更多
Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated....Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. The relationship between the structures and catalytic activities of the catalysts was discussed. The results showed that the catalytic activity and stability of the Ni/ZrO2-CeO2-Al2O3 catalyst was better than those of other catalysts with the highest CH4 conversion, H2/CO and H2/COx ratio at 750 ℃. The catalyst showed a little deactivation along the reaction time during its 72 h on stream with the mean deactivation rate of 0.08%/h. The catalytic performance of the Ni/ZrO2-CeO2-Al2O3 catalyst was also affected by reaction temperature, no2 : nCH4 molar ratio and nH2O : nCH4 molar ratio. TPR, XRD and XPS measurements indicated that the formation of ZrO2-CeO2 solid solution could improve the dispersion of NiO, and inhibit the formation of NiAl2O3, and thus significantly promoted the catalytic activity of the Ni/ZrO2-CeO2-Al2O3 catalyst.展开更多
γ-A12O3-supported CeO2 catalysts were pre- pared by microemulsion and impregnation methods and characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM) techniques. At the same time, the des...γ-A12O3-supported CeO2 catalysts were pre- pared by microemulsion and impregnation methods and characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM) techniques. At the same time, the desulfurization activity of catalysts was investigated. The results show that nanoscale active substances and a high desulfurization effect are achieved by microemulsion, exhibiting a significant dominance compared with traditional impregnation method. The optimal preparation condition is temperature of 30 ℃ and ratio of [H20]/[surface active agent] of 7 with slow demulsification. The activated catalysts still keep high and stable desulfurization activity during a wide temperature range of 450-600 ℃. Among a series of prepared catalysts, the desulfurization rate of 6CeOz/γ-A1203 is the highest, reaching up to 80 % when temperature is higher than 550℃. The catalytic reduction mechanism of SO2 over nano-CeOz/γ-A1203 follows redox mechanism.展开更多
Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffTaction (XRD), low temperature nitrogen adsorption-desorption,...Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffTaction (XRD), low temperature nitrogen adsorption-desorption, oxygen pulsing technique, H2-temperamre programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The Pd-only three-way catalysts (Pd-TWC) supported on these materials were prepared by incipient wetness method and studied by activity tests. The results demonstrated that the CZAN supports obtained by the two methods showed better structural, textural and redox properties than the CZA without Nd2O3, and the addition of Nd203 improved the catalytic activity of TWC. Especially, the CZAN-i support prepared by impregnation method had better thermal stability and redox property. Meanwhile, the Pd/CZAN-i catalyst exhibited the best catalytic performance. XPS measurements indicated that the Nd-modified samples possessed more Ce3+ and oxygen vacancies on the surface of samples, which led to a better redox property. The excellent redox property of support materials helped to improve the catalytic activity of TWC.展开更多
Fe(II)/γ-Al2O3 powders synthesized using the dipping method were produced from a mixed aqueous solution containing aluminium oxide (γ-Al2O3) and iron(II)-precursor (FeSO4), and used for photoFenton degradati...Fe(II)/γ-Al2O3 powders synthesized using the dipping method were produced from a mixed aqueous solution containing aluminium oxide (γ-Al2O3) and iron(II)-precursor (FeSO4), and used for photoFenton degradation of phthalocyanine dyes (PCs) under ultraviolet (UV) irradiation in an up-flow fluidized bed. The catalysts were characterized by XRD, ESCA, BET, EDS and SEM. The results showed that Fe2+ ion was compounded on the γ-Al2O3 carder. The effects of different reaction parameters such as catalyst activity, dosage and solution pH on the decolorization of PCs were assessed. Results indicated that maximum decolorization (more than 95%) of PCs occurred with 20 wt% Fe(II)/γ-Al2O3 catalyst (dosage of 60 g/L) using a combination of UV irradiation and heterogeneous Fenton system. The degradation efficiency of PCs increases as pH decreases, exhibiting a maximum efficiency at pH 3.5. The recycled catalyst was capable of repeating three runs without a significant decrease in treatment efficiency, and this demonstrated the stability and reusability of catalyst.展开更多
A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts c...A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts calcined at different temperatures were characterized using NH3-TPD, pyridine-FTIR, X-ray diffraction, and Raman techniques. It was found that the calcination process could not only change the structure of these catalysts but also modify the amount of surface acidity on the catalysts. The catalyst calcined at 400 ℃ exhibited the highest conversion of acetylene (94.6%) and highest selectivity to vinyl fluoride (83.4%) and lower coke deposition selectivity (0.72%). The highest activity was related to the largest amount of surface acidity on the catalyst, and the coke deposition was also related to the total amount of surface acidic sites.展开更多
基金The National Basic Research Program (973) of China (No. 2004CB418505) the Foundation for Excellent Youth of HeilongjiangProvince
摘要In order to develop a catalyst with high activity for catalytic wet oxidation (CWO) process at room temperature and atmospheric pressure, Fe2O3-CeO2-TiO2/γ-Al2O3 catalyst was prepared by consecutive impregnation method and the prepared parameters were optimized. The structure of the catalyst was characterized by BET, XRF, SEM and XPS technologies, and the actual wastewater was used to investigate the catalytic activity of Fe2O3-CeO2-TiO2/γ-Al2O3 in CWO process. The experimental results showed that the prepared catalyst exhibited good catalytic activity when the doping amount of Ti was 1.0 wt% (the weight ratio of Ti to carriers), and the middle product, Fe2O3-CeO2-TiO2/γ-Al2O3, was calcined in 450℃ for 2 h. The CWO experiment for treating actual dye wastewater indicated that the COD, color and TOC of actual wastewater were decreased by 62.23%, 50.12% and 41.26% in 3 h, respectively, and the ratio of BOD5/COD was increased from 0.19 to 0.30.
基金Project supported by the National Natural Science Key Foundation of China (20333030)
摘要Ce0.67Zr0.33O2-Al2O3 solid solution was prepared by the co-precipitation method. Fe2O3-based catalysts supported on the solid solution were obtained by the impregnation method. The article revealed that the optimal loading amount of Fe2O3 on Ce0.67Zr0.33 O2-Al2O3 in our experimental condition for catalytic combustion of methane was 8% ( mass fraction). The prepared catalysts were characterized by BET, TPR, XRD analyses, and their catalytic activity was investigated after being calcined at 873 K and after being aged in water gas at 1273 K. When the loading amount of Fe203 was 8% ( mass fraction), the catalyst held the highest activity, and the best temperature speciality and thermal stability. The complete-conversion temperature of methane for fresh and aged sample was 788 and 838 K, respectively. The range between the light-off temperature and the complete-conversion temperature was only 15 K. The characterization results of XRD indicated that Fe2O3 was well dispersed on the Ce0.67Zr0.33O2-Al2O3 matrix. The results of BET and TPR were in good harmony with the catalytic activity results.
基金supported by Guangdong Provincial Natural Science Foundation of China(030514)Science and Technology Plan of Guangdong Province of China(2004B33401006)Doctoral Startup Foundation of Guang Dong Pharmaceutical University.
摘要Ni catalysts supported on Al2O3, ZrO2-Al2O3, CeO2-Al2O3 and ZrO2-CeO2-Al2O3 were prepared by coprecipitation method, and their catalytic performances for autothermal reforming of methane to hydrogen were investigated. The Ni-supported catalysts were characterized by XRD, TPR and XPS. The relationship between the structures and catalytic activities of the catalysts was discussed. The results showed that the catalytic activity and stability of the Ni/ZrO2-CeO2-Al2O3 catalyst was better than those of other catalysts with the highest CH4 conversion, H2/CO and H2/COx ratio at 750 ℃. The catalyst showed a little deactivation along the reaction time during its 72 h on stream with the mean deactivation rate of 0.08%/h. The catalytic performance of the Ni/ZrO2-CeO2-Al2O3 catalyst was also affected by reaction temperature, no2 : nCH4 molar ratio and nH2O : nCH4 molar ratio. TPR, XRD and XPS measurements indicated that the formation of ZrO2-CeO2 solid solution could improve the dispersion of NiO, and inhibit the formation of NiAl2O3, and thus significantly promoted the catalytic activity of the Ni/ZrO2-CeO2-Al2O3 catalyst.
基金financially supported by the Natural Science Foundation of Hubei Province, China(No. 2009CDB246)the Applied Basic Research Project of Wuhan City (No. 2015060101010068)
摘要γ-A12O3-supported CeO2 catalysts were pre- pared by microemulsion and impregnation methods and characterized by X-ray diffraction (XRD) and scanning electron microscope (SEM) techniques. At the same time, the desulfurization activity of catalysts was investigated. The results show that nanoscale active substances and a high desulfurization effect are achieved by microemulsion, exhibiting a significant dominance compared with traditional impregnation method. The optimal preparation condition is temperature of 30 ℃ and ratio of [H20]/[surface active agent] of 7 with slow demulsification. The activated catalysts still keep high and stable desulfurization activity during a wide temperature range of 450-600 ℃. Among a series of prepared catalysts, the desulfurization rate of 6CeOz/γ-A1203 is the highest, reaching up to 80 % when temperature is higher than 550℃. The catalytic reduction mechanism of SO2 over nano-CeOz/γ-A1203 follows redox mechanism.
基金Project supported by National Natural Science Foundation of China (20773090, 20803049)the Specialized Research Fund for the Doctoral Program of Higher Education (20070610026, 200806100009)
摘要Ce-Zr-Al-Nd2O3 (CZAN) support materials were prepared by co-precipitation and impregnation methods, respectively. They were characterized by X-ray diffTaction (XRD), low temperature nitrogen adsorption-desorption, oxygen pulsing technique, H2-temperamre programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The Pd-only three-way catalysts (Pd-TWC) supported on these materials were prepared by incipient wetness method and studied by activity tests. The results demonstrated that the CZAN supports obtained by the two methods showed better structural, textural and redox properties than the CZA without Nd2O3, and the addition of Nd203 improved the catalytic activity of TWC. Especially, the CZAN-i support prepared by impregnation method had better thermal stability and redox property. Meanwhile, the Pd/CZAN-i catalyst exhibited the best catalytic performance. XPS measurements indicated that the Nd-modified samples possessed more Ce3+ and oxygen vacancies on the surface of samples, which led to a better redox property. The excellent redox property of support materials helped to improve the catalytic activity of TWC.
摘要Fe(II)/γ-Al2O3 powders synthesized using the dipping method were produced from a mixed aqueous solution containing aluminium oxide (γ-Al2O3) and iron(II)-precursor (FeSO4), and used for photoFenton degradation of phthalocyanine dyes (PCs) under ultraviolet (UV) irradiation in an up-flow fluidized bed. The catalysts were characterized by XRD, ESCA, BET, EDS and SEM. The results showed that Fe2+ ion was compounded on the γ-Al2O3 carder. The effects of different reaction parameters such as catalyst activity, dosage and solution pH on the decolorization of PCs were assessed. Results indicated that maximum decolorization (more than 95%) of PCs occurred with 20 wt% Fe(II)/γ-Al2O3 catalyst (dosage of 60 g/L) using a combination of UV irradiation and heterogeneous Fenton system. The degradation efficiency of PCs increases as pH decreases, exhibiting a maximum efficiency at pH 3.5. The recycled catalyst was capable of repeating three runs without a significant decrease in treatment efficiency, and this demonstrated the stability and reusability of catalyst.
基金ACKNOWLEDGMENT This work was supported by the National Natural Science Foundation of China (No.20873125),
摘要A La-modified Al2O3 catalyst was prepared with deposition-precipitation method. The effect of calcination temperature on the reactivity for vapor phase hydrofluorination of acetylene to vinyl fluoride. The catalysts calcined at different temperatures were characterized using NH3-TPD, pyridine-FTIR, X-ray diffraction, and Raman techniques. It was found that the calcination process could not only change the structure of these catalysts but also modify the amount of surface acidity on the catalysts. The catalyst calcined at 400 ℃ exhibited the highest conversion of acetylene (94.6%) and highest selectivity to vinyl fluoride (83.4%) and lower coke deposition selectivity (0.72%). The highest activity was related to the largest amount of surface acidity on the catalyst, and the coke deposition was also related to the total amount of surface acidic sites.