Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb mo...Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer(XRD), Brunauer-Emmett-Teller(BET), Transmission electron microscopy(TEM), Fourier transform infrared spectroscopy(FT-IR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS), Raman and Hydrogen temperature-programmed reduction(H2-TPR). The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.展开更多
CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were p...CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.展开更多
The CeO2@TiO2 core-shell nanostructure catalyst prepared by a two-step hydrothermal method was used for selective catalytic reduction (SCR) of NOx with NH3 in this study. The catalyst presented the obvious core-shel...The CeO2@TiO2 core-shell nanostructure catalyst prepared by a two-step hydrothermal method was used for selective catalytic reduction (SCR) of NOx with NH3 in this study. The catalyst presented the obvious core-shell structure, and the shell was amorphous TiO2 which could protect the active center from the SO2 erosion. The catalyst showed high activity and stability, excellent N2 selectivity and superior SO2 resistance and H2O tolerance. Characterizations such as TEM, HR-TEM, XRD, BET, XPS, NH3-TPD, and H2-TPR were carried out. The results indicated that the catalyst had large surface area and the active sites were well dispersed on the surface. The NH3-TPD, H2-TPR and XPS results implied that its increased SCR activity might be due to the enhancement of NH3 chemisorption and the increase of active oxygen species, both of which were conductive to NH3 activation. The excellent catalytic performance suggests that it is a promising candidate for SCR catalyst.展开更多
The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition beha...The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.展开更多
A MnOx-NbOx-CeO2 catalyst for low temperature selective catalytic reduction(SCR) of NOx with NH3 was prepared by a sol-gel method, and characterized by NH3-NO/NO2 SCR catalytic activity, NO/NH3 oxidation activity, N...A MnOx-NbOx-CeO2 catalyst for low temperature selective catalytic reduction(SCR) of NOx with NH3 was prepared by a sol-gel method, and characterized by NH3-NO/NO2 SCR catalytic activity, NO/NH3 oxidation activity, NOx/NH3 TPD, XRD, BET, H2-TPR and in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy(DRIFTS). The results indicate that the Mn Ox-Nb Ox-CeO2 catalyst shows excellent low temperature NH3-SCR activity in the temperature range of 150-300℃. Water vapor inhibits the low temperature activity of the catalyst in standard SCR due to the inhibition of NOx adsorption. As the NO2 content increases in the feed, water vapor does not affect the activity in NO2 SCR. Meanwhile, water vapor significantly enhances the N2 selectivity of the fresh and the aged catalysts due to its inhibition of the decomposition of NH4NO3 into N2O.展开更多
The selective catalytic reduction (SCR) activities of the MoO3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated. The results showed that the addition o...The selective catalytic reduction (SCR) activities of the MoO3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated. The results showed that the addition of MoO3 could enhance the NOx conversion at low temperature and the best SCR activity was obtained when the dosage of MoO3 reached 5 wt.%. The NH3-TPD and DRIFTS experiments indicated that the addition of MoO3 changed the type and number of acid sites on the surface of catalysts and reaction activities of acid sites were altered at the same time. The redox capacity and amount of active oxygen species got improved for V3Mo5/WTi catalyst, which could be confirmed by the H2-TPR and transient response experiments. Water vapor inhibited the NOx conversion at low temperature. Deposition of ammonium sulfate or bisulfate might be main reason for the loss of catalytic activity in the presence of SO2 at low temperature. Choosing the suitable NH3/NO ratio and elevation of reaction temperature both could weaken the influence of SO2 on the SCR activity of the V3MoSAFTi catalyst. Thermal treatment of the deactivated catalyst at 350℃ could get the low temperature activity recovered. The decrease of GHSV improved the deNOx efficiency at low temperature and we speculated that the rational technological process and operation parameters could contribute to the application of this kind of catalysts in real industrial environment.展开更多
基金supported by the Natural Science Foundation of China (Nos. 21376261, 21173270)the Beijing Natural Science Foundation (2142027)+1 种基金Doctor select Foundation (No. 20130007110007)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)
文摘Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer(XRD), Brunauer-Emmett-Teller(BET), Transmission electron microscopy(TEM), Fourier transform infrared spectroscopy(FT-IR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS), Raman and Hydrogen temperature-programmed reduction(H2-TPR). The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.
基金financially supported by the National Natural Science Foundation of China (Nos. 21376261, 21173270, 21177160)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)+2 种基金the Beijing Natural Science Foundation (2142027)the Doctoral Selection Fund (No. 20130007110007)the China University of Petroleum Fund (No. KYJJ2012-06-31)
文摘CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.
基金financially supported by the National Natural Science Foundation of China(No.51508281)the Natural Science Foundation of Jiangsu Province(No.BK20130907)Research Startup Funds Program for High Level Talent of Nanjing Normal University(No.2013105XGQ0056)
文摘The CeO2@TiO2 core-shell nanostructure catalyst prepared by a two-step hydrothermal method was used for selective catalytic reduction (SCR) of NOx with NH3 in this study. The catalyst presented the obvious core-shell structure, and the shell was amorphous TiO2 which could protect the active center from the SO2 erosion. The catalyst showed high activity and stability, excellent N2 selectivity and superior SO2 resistance and H2O tolerance. Characterizations such as TEM, HR-TEM, XRD, BET, XPS, NH3-TPD, and H2-TPR were carried out. The results indicated that the catalyst had large surface area and the active sites were well dispersed on the surface. The NH3-TPD, H2-TPR and XPS results implied that its increased SCR activity might be due to the enhancement of NH3 chemisorption and the increase of active oxygen species, both of which were conductive to NH3 activation. The excellent catalytic performance suggests that it is a promising candidate for SCR catalyst.
基金supported by the National Natural Science Foundation of China(No.51576039)
文摘The deposition of NH4 HSO4 and the poisoning effect of SO2 on SCR catalyst are the main obstacles that restrict the industrial application of CeO2-doped SCR catalysts.In this work,deposited NH4 HSO4 decomposition behavior and SO2 poisoning over V2 O5-MoO3/TiO2 catalysts modified with CeO2 and SiO2 were investigated.By the means of characterization analysis,it was found that the addition of SiO2 into VMo/Ti-Ce had an impact on the interaction existed between catalyst surface atoms and NH4 HSO4.Temperatureprogrammed methods and in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)experiments indicated that the doping of SiO2 promoted the decomposition of deposited NH4 HSO4 on VMo/Ti-Ce catalyst surface by reducing the thermal stability of NH4 HSO4 and enhancing the NH4 HSO4 reactivity with NO in low temperature.And this improvement may be the reason for the better catalytic activity than VMo/Ti-Ce in the case of NH4 HSO4 deposition.Accompanied with cerium sulfate species generated over catalyst surface,the conversion of SO2 to SO3 was inhibited in SiCe mixed catalyst.The addition of SiO2 could promote the decomposition of cerium sulfate,which may be a potential strategy to enhance the resistance of SO2 poisoning over CeO2-modifed catalysts.
基金supported by the Ministry of Science and Technology of China (No. 2010CB732304)the Science and Technology Department of Zhejiang Province Project (No. 2011C31010)the National Natural Science Foundation of China (No. 51202126)
文摘A MnOx-NbOx-CeO2 catalyst for low temperature selective catalytic reduction(SCR) of NOx with NH3 was prepared by a sol-gel method, and characterized by NH3-NO/NO2 SCR catalytic activity, NO/NH3 oxidation activity, NOx/NH3 TPD, XRD, BET, H2-TPR and in-situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy(DRIFTS). The results indicate that the Mn Ox-Nb Ox-CeO2 catalyst shows excellent low temperature NH3-SCR activity in the temperature range of 150-300℃. Water vapor inhibits the low temperature activity of the catalyst in standard SCR due to the inhibition of NOx adsorption. As the NO2 content increases in the feed, water vapor does not affect the activity in NO2 SCR. Meanwhile, water vapor significantly enhances the N2 selectivity of the fresh and the aged catalysts due to its inhibition of the decomposition of NH4NO3 into N2O.
基金financially supported by the Policy-induced Project of Jiangsu Province for the Industry-UniversityResearch Cooperation (BY2015070-21)the Natural Science Fund Program of Jiangsu Province (BK20150749)
文摘The selective catalytic reduction (SCR) activities of the MoO3 doped V/WTi catalysts prepared by the incipient wetness impregnation method at low temperature were investigated. The results showed that the addition of MoO3 could enhance the NOx conversion at low temperature and the best SCR activity was obtained when the dosage of MoO3 reached 5 wt.%. The NH3-TPD and DRIFTS experiments indicated that the addition of MoO3 changed the type and number of acid sites on the surface of catalysts and reaction activities of acid sites were altered at the same time. The redox capacity and amount of active oxygen species got improved for V3Mo5/WTi catalyst, which could be confirmed by the H2-TPR and transient response experiments. Water vapor inhibited the NOx conversion at low temperature. Deposition of ammonium sulfate or bisulfate might be main reason for the loss of catalytic activity in the presence of SO2 at low temperature. Choosing the suitable NH3/NO ratio and elevation of reaction temperature both could weaken the influence of SO2 on the SCR activity of the V3MoSAFTi catalyst. Thermal treatment of the deactivated catalyst at 350℃ could get the low temperature activity recovered. The decrease of GHSV improved the deNOx efficiency at low temperature and we speculated that the rational technological process and operation parameters could contribute to the application of this kind of catalysts in real industrial environment.