In this work we prepared several CeO2-TiO2 catalysts for the NH3-SCR reactionusing co-precipitation with assistance of microwave irradiation.The catalytic NH3-SCR activities over CeO2-TiO2 catalysts at low temperature...In this work we prepared several CeO2-TiO2 catalysts for the NH3-SCR reactionusing co-precipitation with assistance of microwave irradiation.The catalytic NH3-SCR activities over CeO2-TiO2 catalysts at low temperatures are largely enhanced by the treatment of microwave irradiation,the operation temperature window is also broadened.For better understanding the promotion mechanism,the catalyst prepared by conventional co-precipitation with and without microwave irradiation treatment was characterized with H2-TPR,NH3-TPD,XPS,XRD and BET.Microwave irradiation treatment accelerates the crystallite rate of CeO2-TiO2 catalysts,and greatly enlarges their surface area by adjusting their microstructures.The resistance to SO2 and H2O is also improved via regulating the hierarchical pore structure by the microwave irradiation.Microwave irradiation treatment can also improve the redox property and increase the acid sites over the catalyst surfaces.The result of in situ DRIFTS suggests that the microwave irradiation treatment generates more Br?nsted acid sites on CeO2-TiO2-2 h catalyst,helpful in SCR reactions.XPS results show that after microwave irradiation on the CeO2-TiO2 catalysts,the surface demonstrates an elevated concentration of chemisorbed oxygen,consequently leading to better oxidation of NO to NO2.Additionally,the molar ratio of Ce3+/Ce4+has been elevated after being treated by microwave irradiation,a vital factor in enhancing the NH3-SCR activities.展开更多
The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoe...The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoelectron spectroscopy(XPS),H2 temperature-programmed reduction(H2-TPR),X-ray diffraction(XRD)and Pd dispersion analysis were used for their characterization.Pd/Cc0.76Zro.18 La0.06O1.97 catalyst showed the highest BET surface area,best Pd dispersion capability and strongest metal-support interaction.Moreover,XPS showed that there was lattice defect oxygen or mobile oxygen.According to the result of O 1s measurements the lattice defect oxygen or mobile oxygen helped to maintain Pd in a partly oxidized state and increased the activity for methanol decomposition.The Pd/Ce0.76Zr0.18La0.0601.97 catalyst exhibited the best activity.A 100%conversion of methanol was achieved at around 260°C,which was about 20-40°C lower than other catalysts.展开更多
Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N...Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.展开更多
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
V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for N...V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.展开更多
基金Project supported by the National Natural Science Foundation of China(21577005)the National Key Research and Development Program of China(2016YFB0600400)
摘要In this work we prepared several CeO2-TiO2 catalysts for the NH3-SCR reactionusing co-precipitation with assistance of microwave irradiation.The catalytic NH3-SCR activities over CeO2-TiO2 catalysts at low temperatures are largely enhanced by the treatment of microwave irradiation,the operation temperature window is also broadened.For better understanding the promotion mechanism,the catalyst prepared by conventional co-precipitation with and without microwave irradiation treatment was characterized with H2-TPR,NH3-TPD,XPS,XRD and BET.Microwave irradiation treatment accelerates the crystallite rate of CeO2-TiO2 catalysts,and greatly enlarges their surface area by adjusting their microstructures.The resistance to SO2 and H2O is also improved via regulating the hierarchical pore structure by the microwave irradiation.Microwave irradiation treatment can also improve the redox property and increase the acid sites over the catalyst surfaces.The result of in situ DRIFTS suggests that the microwave irradiation treatment generates more Br?nsted acid sites on CeO2-TiO2-2 h catalyst,helpful in SCR reactions.XPS results show that after microwave irradiation on the CeO2-TiO2 catalysts,the surface demonstrates an elevated concentration of chemisorbed oxygen,consequently leading to better oxidation of NO to NO2.Additionally,the molar ratio of Ce3+/Ce4+has been elevated after being treated by microwave irradiation,a vital factor in enhancing the NH3-SCR activities.
基金the National Natural Science Foundation of China(20773090)the Specialized Research Fund for the Doctoral Program of Higher Education of China(20070610026,200806100009)
摘要The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoelectron spectroscopy(XPS),H2 temperature-programmed reduction(H2-TPR),X-ray diffraction(XRD)and Pd dispersion analysis were used for their characterization.Pd/Cc0.76Zro.18 La0.06O1.97 catalyst showed the highest BET surface area,best Pd dispersion capability and strongest metal-support interaction.Moreover,XPS showed that there was lattice defect oxygen or mobile oxygen.According to the result of O 1s measurements the lattice defect oxygen or mobile oxygen helped to maintain Pd in a partly oxidized state and increased the activity for methanol decomposition.The Pd/Ce0.76Zr0.18La0.0601.97 catalyst exhibited the best activity.A 100%conversion of methanol was achieved at around 260°C,which was about 20-40°C lower than other catalysts.
基金supported by the National Natural Science Foundation of China (No. 20773090, 20803049)the National High Technology Researchand Development Program of China (863 Program, No. 2006AA06Z347)the Specialized Research Fund for the Doctoral Program of Higher Education(20070610026)
摘要Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.
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supported by the National Natural Science Foundation of China (51372137)the National High Technology Research and Development Program of China (863 Program,2015AA034603)~~
摘要V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.