A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]....A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]. Their activity for selective catalytic reduction of nitrogen oxides(NO_x) with NH3 was determined. The results show that the Cu-SSZ-13(HTS) catalyst exhibits a better ammonia selective catalytic reduction(NH3-SCR)activity compared with the other two catalysts, over which more than 90% NO conversion is obtained at 215-600℃under the space velocity of 180,000 h^(-1). The characterization results reveal that the Cu-SSZ-13(HTS) catalyst possesses more amount of stable Cu^(2+) in the six-membered ring and high ability for NH3 and NO adsorption, leading to its high NH3-SCR activity, although this catalyst has low surface area. On the other hand, the activity of Cu-SSZ-13(IE) catalyst is almost the same as that of Cu-SSZ-13(IWI) catalyst at the temperature lower than 400 ℃, but the activity of the former is much higher than that of the latter at > 400 ℃ due to the high activity of Cu-SSZ-13(IWI) catalyst for NH3 oxidation.展开更多
The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel...The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel engines. In this work, V2O5/WO3-TiO2 (VWT) and SiO2- doped V2O5/WO3-TiO2 (VWTSi10)) catalysts were prepared by impregnation method and characterized by Brunauer- Emmett-Teller (BET), X-ray diffraction (XRD), Raman, temperature programmed reduction by hydrogen (H2-TPR), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption by ammonia (NH3- TPD). The doping of SiO2 promotes the thermal stability of V2O5/WO3-TiO? for NH3-SCR significantly. After calcination at 650 °C for 50 h, the operation window of 10% SiO2-doped V2O5/WO3-TiO2 is 220-480 °C, while the maximum NOV conversion on V2O5/WO3-TiO2 is about 77%. The presenee of SiO2 obviously blocks the transformation of TiO2 from anatase to rutile and stabilizes the dispersion of VOv and WO3 on the surface. It is available for the existence of V44 and the amount of surface acid sites increases, which inhabits the NH3 oxidation at the high temperature range and promotes NH3-SCR activity.展开更多
A series of 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2 catalysts were prepared by impregnation method based on the presynthesis of Sn_(0.9)Ce_(0.1)O_2 support prepared by co-precipitation method, and then characterized by Brunaue...A series of 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2 catalysts were prepared by impregnation method based on the presynthesis of Sn_(0.9)Ce_(0.1)O_2 support prepared by co-precipitation method, and then characterized by Brunauer–Emmett–Teller(BET), X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), Raman, CO chemical adsorption and hydrogen temperature-programmed reduction(H_2-TPR) techniques. The effect of calcination temperature of the composite oxide support on the catalytic performances of the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst for the CH_4 total oxidation was studied. It is found that the catalytic activity of the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst increases with the increase in calcination temperature of the Pd/Sn_(0.9)Ce_(0.1)O_2 support. The 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2/1100 catalyst(the Pd/Sn_(0.9)Ce_(0.1)O_2 support was calcined at 1100 ℃) exhibits the best reactive activity(T_(10)= 255 ℃). The excellent activity of the 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2/1100 catalyst should be attributed to the high reducibility of PdO, the excellent oxygen mobility of the support and the high content of active Pd^(2+) species on the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst.展开更多
The unsupported Cu and Ag catalysts with different oxidation states were prepared, and their catalytic performances for propylene epoxidation were investigated.The metallic Cu catalyst exhibits much higher catalytic a...The unsupported Cu and Ag catalysts with different oxidation states were prepared, and their catalytic performances for propylene epoxidation were investigated.The metallic Cu catalyst exhibits much higher catalytic activity and propylene oxide(PO) selectivity than Cu2 O and Cu O catalysts.The Cu0 species are the main active sites for propylene epoxidation, but Cu2 O and Cu O species are in favor of CO2 and acrolein production.The PO selectivity of 54.2 % and propylene conversion of 2.6 % can be achieved over the metallic Cu catalyst at 160 °C in initial stage, but metallic Cu catalyst would be oxidized to Cu2 O during propylene epoxidation, resulting in a sharp decrease in the PO selectivity and propylene conversion.Nanosize Ag Cuxbimetallic catalysts were prepared.It is found that adding Ag to the metallic Cu catalysts can prevent the oxidation of Cu and make Ag Cuxbimetallic catalysts more stable under the condition of propylene epoxidation.The Ag/Cu molar ratio can remarkably affect the catalytic performance of Ag Cuxcatalyst and the selectivity to PO and acrolein.After Ag Cuxwas supported on MOx-modified a-Al2O3, its catalytic performance can be improved and has a close relationship with the acid–base property of support.展开更多
基金financially supported by the National Key Research and Development Program of China (No. 2016YFC0204300)the National Natural Science Foundation of China (Nos. 21577034 and 21333003)the Science and Technology Commission of Shanghai Municipality (No. 16ZR1407900)
文摘A series of Cu-SSZ-13 catalysts with the same Cu loading were prepared by different methods of incipient wetness impregnation [Cu-SSZ-13(IWI)], ion exchange[Cu-SSZ-13(IE)] and hydro-thermal synthesis [Cu-SSZ-13(HTS)]. Their activity for selective catalytic reduction of nitrogen oxides(NO_x) with NH3 was determined. The results show that the Cu-SSZ-13(HTS) catalyst exhibits a better ammonia selective catalytic reduction(NH3-SCR)activity compared with the other two catalysts, over which more than 90% NO conversion is obtained at 215-600℃under the space velocity of 180,000 h^(-1). The characterization results reveal that the Cu-SSZ-13(HTS) catalyst possesses more amount of stable Cu^(2+) in the six-membered ring and high ability for NH3 and NO adsorption, leading to its high NH3-SCR activity, although this catalyst has low surface area. On the other hand, the activity of Cu-SSZ-13(IE) catalyst is almost the same as that of Cu-SSZ-13(IWI) catalyst at the temperature lower than 400 ℃, but the activity of the former is much higher than that of the latter at > 400 ℃ due to the high activity of Cu-SSZ-13(IWI) catalyst for NH3 oxidation.
基金financially supported by the National Key Research and Development Program of China (No. 2016YFC0204300)the National High Technology Research and Development Program of China (No. 2015AA034603)+2 种基金the National Natural Science Foundation of China (Nos. 21333003 and 21571061)the "Shu Guang" Project of the Shanghai Municipal Education Commission (No. 12SG29)the Commission of Science and Technology of Shanghai Municipality (No. 15DZ1205305)
文摘The selective catalytic reduction of NOV with NH3 (NH3-SCR) is a very effective technology to control the emission of NOA, and the thermal stability of NH3-SCR catalyst is very important for removal of NOV from diesel engines. In this work, V2O5/WO3-TiO2 (VWT) and SiO2- doped V2O5/WO3-TiO2 (VWTSi10)) catalysts were prepared by impregnation method and characterized by Brunauer- Emmett-Teller (BET), X-ray diffraction (XRD), Raman, temperature programmed reduction by hydrogen (H2-TPR), X-ray photoelectron spectroscopy (XPS) and temperature programmed desorption by ammonia (NH3- TPD). The doping of SiO2 promotes the thermal stability of V2O5/WO3-TiO? for NH3-SCR significantly. After calcination at 650 °C for 50 h, the operation window of 10% SiO2-doped V2O5/WO3-TiO2 is 220-480 °C, while the maximum NOV conversion on V2O5/WO3-TiO2 is about 77%. The presenee of SiO2 obviously blocks the transformation of TiO2 from anatase to rutile and stabilizes the dispersion of VOv and WO3 on the surface. It is available for the existence of V44 and the amount of surface acid sites increases, which inhabits the NH3 oxidation at the high temperature range and promotes NH3-SCR activity.
基金financially supported by the National Key Research and Development Program of China (No. 2016YFC0204300)the National Key Basic Research Program of China (No. 2013CB933200)Science and Technology Commission of Shanghai Municipality (No. 16ZR1407900)
文摘A series of 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2 catalysts were prepared by impregnation method based on the presynthesis of Sn_(0.9)Ce_(0.1)O_2 support prepared by co-precipitation method, and then characterized by Brunauer–Emmett–Teller(BET), X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), Raman, CO chemical adsorption and hydrogen temperature-programmed reduction(H_2-TPR) techniques. The effect of calcination temperature of the composite oxide support on the catalytic performances of the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst for the CH_4 total oxidation was studied. It is found that the catalytic activity of the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst increases with the increase in calcination temperature of the Pd/Sn_(0.9)Ce_(0.1)O_2 support. The 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2/1100 catalyst(the Pd/Sn_(0.9)Ce_(0.1)O_2 support was calcined at 1100 ℃) exhibits the best reactive activity(T_(10)= 255 ℃). The excellent activity of the 0.2 wt% Pd/Sn_(0.9)Ce_(0.1)O_2/1100 catalyst should be attributed to the high reducibility of PdO, the excellent oxygen mobility of the support and the high content of active Pd^(2+) species on the Pd/Sn_(0.9)Ce_(0.1)O_2 catalyst.
基金financially supported by the National Basic Research Program of China (No. 2010CB732300)
文摘The unsupported Cu and Ag catalysts with different oxidation states were prepared, and their catalytic performances for propylene epoxidation were investigated.The metallic Cu catalyst exhibits much higher catalytic activity and propylene oxide(PO) selectivity than Cu2 O and Cu O catalysts.The Cu0 species are the main active sites for propylene epoxidation, but Cu2 O and Cu O species are in favor of CO2 and acrolein production.The PO selectivity of 54.2 % and propylene conversion of 2.6 % can be achieved over the metallic Cu catalyst at 160 °C in initial stage, but metallic Cu catalyst would be oxidized to Cu2 O during propylene epoxidation, resulting in a sharp decrease in the PO selectivity and propylene conversion.Nanosize Ag Cuxbimetallic catalysts were prepared.It is found that adding Ag to the metallic Cu catalysts can prevent the oxidation of Cu and make Ag Cuxbimetallic catalysts more stable under the condition of propylene epoxidation.The Ag/Cu molar ratio can remarkably affect the catalytic performance of Ag Cuxcatalyst and the selectivity to PO and acrolein.After Ag Cuxwas supported on MOx-modified a-Al2O3, its catalytic performance can be improved and has a close relationship with the acid–base property of support.