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
Ce-ZrO2 is a widely used three-way catalyst support. Because of the large surface area and excellent redox quality, Ce-ZrO2 may have potential application in selective catalytic reduction （SCR） systems. In the prese...Ce-ZrO2 is a widely used three-way catalyst support. Because of the large surface area and excellent redox quality, Ce-ZrO2 may have potential application in selective catalytic reduction （SCR） systems. In the present work, Ce-ZrO2 was introduced into a low-temperature SCR system and CeO2 and ZrO2 supports were also introduced to make a contrastive study. Mn/CeO2, Mn/ZrO2 and Mn/Ce-ZrO2 were prepared by impregnating these supports with Mn（NO3）2 solution, and have been characterized by N2-BET, XRD, TPR, TPD, XPS, FT-IR and TG. The activity and resistance to SO2 and H2O of the catalysts were investigated. Mn/Ce-ZrO2 and Mn/CeO2 were proved to have better low-temperature activities than Mn/ZrO2, and yielded 98.6% and 96.8% NO conversion at 180℃, respectively. This is mainly because Mn/Ce-ZrO2 and Mn/CeO2 had higher dispersion of manganese oxides, better redox properties and more weakly adsorbed oxygen species than Mn/ZrO2. In addition, Mn/Ce-ZrO2 showed a good resistance to SO2 and H2O and presented 87.1% NO conversion, even under SO2 and H2O treatment for 6 hours, and the activity of Mn/Ce-ZrO2 was almost restored to its original level after cutting off the injection of SO2 and H2O. This was due to the weak water absorption and weak sulfation process on the surface of the catalyst.展开更多
Samples of cerium-manganese oxides supported on modified glass-fiber with different Ce/Mn molar ratios （Ce-Mn/GF） were prepared by an impregnation method and tested for low-temperature （80 180 ℃） selective cataly...Samples of cerium-manganese oxides supported on modified glass-fiber with different Ce/Mn molar ratios （Ce-Mn/GF） were prepared by an impregnation method and tested for low-temperature （80 180 ℃） selective catalytic reduction （SCR） of NO with ammonia. This brand-new technology could remove NO and particles matter from coal-fired flue gas. The surface properties of the catalysts were examined by means of Bmnauer-Emmett-Teller （BET）, X-ray photoelectron spectroscopy （XPS）, X-ray diffraction （XRD）, and scanning electron microscopy （SEM）. The experimental results showed that the catalyst with a Ce/Mn molar ratio of 0.2 obtained high activity of 87.4% NO conversion at 150 ℃ under a high space velocity of 50000 h1. Deactivation poisoned by SO2 still occurred, but the Ce-Mn/GF（0.2） catalyst performed desirable tolerance to SO2 with decreasing 50% in 40 min and then maintaining at about 30% NO conversion. Characterization results indicated that the excellent low-temperature catalytic activity was related to the high specific surface area, pore structure, and amorphous phase.展开更多
The effect of molybdenum oxide on the activity and durability of Ce O2-Ti O2 catalyst for NO reduction by NH3 was examined. It was found that the introduction of Mo could improve the low-temperature NH3-SCR activity a...The effect of molybdenum oxide on the activity and durability of Ce O2-Ti O2 catalyst for NO reduction by NH3 was examined. It was found that the introduction of Mo could improve the low-temperature NH3-SCR activity and SO2/H2 O durability of the Ce O2-Ti O2 catalyst and an optimal loading of Mo was 4?wt.%. The best Mo O3/Ce O2-Ti O2 catalyst displayed over 90% NO conversion from 200 °C to 400 °C and obtained 4-fold increase in NO conversion compared to Ce O2-Ti O2 at 150 °C. The characterization results revealed that the number of Br?nsted acid sites over Mo O3/Ce O2-Ti O2 was significantly increased, and the adsorption of nitrate species was dramatically weakened because of the coverage of Mo O3, which were favorable for the high NH3-SCR performance. It is believed that the Mo O3/Ce O2-Ti O2 catalyst is a suitable substitute for the NH3-SCR reaction.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
Quantum chemical calculation was carried out to choose a promoter which can reduce the poisoning of V2O5/TiO2 catalysts by SO2. Several atoms were chosen as candidates and new catalysts were synthesized by impregnatio...Quantum chemical calculation was carried out to choose a promoter which can reduce the poisoning of V2O5/TiO2 catalysts by SO2. Several atoms were chosen as candidates and new catalysts were synthesized by impregnation method. The NOx conversion rate was measured at temperatures between 100 and 400 ℃ and poisoning effect was investigated. The most promising candidate promoter, Se, was excluded because of its high vapor pressure. On the other hand, Sb shows best promoting properties. Sb promoted catalyst reaches the maximum NOx conversion rate at 250 ℃. It also shows considerably enhanced resistance to poisoning of V2O5/TiO2 catalysts by SO2.展开更多
The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction（...The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction（XRD）, CO chemisorption, X-ray photoelectron spectroscopy（XPS）, Fourier transform infrared spectroscopy（FT-IR） and X-ray fluorescence（XRF）. After 10 h SO2 sulfation, it was found that the decrement on CO oxidation catalytic activity was limited on Pd/Ce0.75Zr0.25O2 compared to Pd/Ce O2-Ti O2 and Pd/Ce O2. It demonstrated that Pd/Ce0.75Zr0.25O2 was more sulfur resistant compared to the other two catalysts. After sulfur exposure, catalyst texture was not much influenced as shown by N2 adsorption and XRD, and surface Pd atoms were poisoned indicated by CO chemisorption results. Pd/Ce0.75Zr0.25O2 and Pd/Ce O2-Ti O2 exhibited less sulfur accumulation compared to Pd/Ce O2 in the sulfation process. Furthermore, XPS results clarified that surface sulfur amount, especially surface sulfates amount on the sulfated catalysts was more crucial for the deactivation in sulfur containing environment.展开更多
CuCeZrO_x and KCuCeZrO_x catalysts were synthesized and coated on the blank diesel particulate filter(DPF)substrate and a particulate matter(PM)loading apparatus was used for soot loading.The catalytic performances of...CuCeZrO_x and KCuCeZrO_x catalysts were synthesized and coated on the blank diesel particulate filter(DPF)substrate and a particulate matter(PM)loading apparatus was used for soot loading.The catalytic performances of soot oxidation were evaluated by temperature programmed combustion(TPC)test and characterization tests were conducted to investigate the physicochemical properties of the catalysts.The reaction mechanism in the oxidation process was analyzed with diffuse reflectance infrared Fourier transform spectroscopy.The results demonstrated that CuCeZrO_x catalyst exhibited high activities of soot oxidation at low temperature and the best results have been attained with Cu_(0.9)Ce_(0.05)Zr_(0.05)O_x over which the maximum soot oxidation rate decreased to 410~?C.Characterization tests have shown that catalysts containing 90%Cu have uniformly distributed grains and small particle sizes,which provide excellent oxidation activity by providing more active sites and forming a good bond between the catalyst and the soot.The low-temperature oxidation activity of soot could be further optimized due to the excellent elevated NO’s conversion rate by partially substituting Cu with K.The maximum particle oxidation rate can be easily realized at such a low temperature as 347~?C.展开更多
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supported by the National Natural Science Foundation of China (No. 51176077,50976050)the Tianjin Municipal Natural Science Foundation Project(No. 12JCZDJC29300)
文摘Ce-ZrO2 is a widely used three-way catalyst support. Because of the large surface area and excellent redox quality, Ce-ZrO2 may have potential application in selective catalytic reduction （SCR） systems. In the present work, Ce-ZrO2 was introduced into a low-temperature SCR system and CeO2 and ZrO2 supports were also introduced to make a contrastive study. Mn/CeO2, Mn/ZrO2 and Mn/Ce-ZrO2 were prepared by impregnating these supports with Mn（NO3）2 solution, and have been characterized by N2-BET, XRD, TPR, TPD, XPS, FT-IR and TG. The activity and resistance to SO2 and H2O of the catalysts were investigated. Mn/Ce-ZrO2 and Mn/CeO2 were proved to have better low-temperature activities than Mn/ZrO2, and yielded 98.6% and 96.8% NO conversion at 180℃, respectively. This is mainly because Mn/Ce-ZrO2 and Mn/CeO2 had higher dispersion of manganese oxides, better redox properties and more weakly adsorbed oxygen species than Mn/ZrO2. In addition, Mn/Ce-ZrO2 showed a good resistance to SO2 and H2O and presented 87.1% NO conversion, even under SO2 and H2O treatment for 6 hours, and the activity of Mn/Ce-ZrO2 was almost restored to its original level after cutting off the injection of SO2 and H2O. This was due to the weak water absorption and weak sulfation process on the surface of the catalyst.
基金Project supported by the National High Technology Research and Development Program of China(863 Program)(2008AA05Z305)the Scientific Research Foundation for the Returned Overseas Chinese Scholars,State Education Ministry(201109)+2 种基金the Master Dissertation Innovation Funded Projects(EG2013015)the Fundamental Research Funds for the Central Universities Special Fund Project(11D11315)Program of Shanghai Subject Chief Scientist(14XD1424700)
文摘Samples of cerium-manganese oxides supported on modified glass-fiber with different Ce/Mn molar ratios （Ce-Mn/GF） were prepared by an impregnation method and tested for low-temperature （80 180 ℃） selective catalytic reduction （SCR） of NO with ammonia. This brand-new technology could remove NO and particles matter from coal-fired flue gas. The surface properties of the catalysts were examined by means of Bmnauer-Emmett-Teller （BET）, X-ray photoelectron spectroscopy （XPS）, X-ray diffraction （XRD）, and scanning electron microscopy （SEM）. The experimental results showed that the catalyst with a Ce/Mn molar ratio of 0.2 obtained high activity of 87.4% NO conversion at 150 ℃ under a high space velocity of 50000 h1. Deactivation poisoned by SO2 still occurred, but the Ce-Mn/GF（0.2） catalyst performed desirable tolerance to SO2 with decreasing 50% in 40 min and then maintaining at about 30% NO conversion. Characterization results indicated that the excellent low-temperature catalytic activity was related to the high specific surface area, pore structure, and amorphous phase.
基金supported by the National Natural Science Foundation of China(21773106,21707066,21677069,and 21806077)the China Postdoctoral Science Foundation(2018M642206)~~
文摘The effect of molybdenum oxide on the activity and durability of Ce O2-Ti O2 catalyst for NO reduction by NH3 was examined. It was found that the introduction of Mo could improve the low-temperature NH3-SCR activity and SO2/H2 O durability of the Ce O2-Ti O2 catalyst and an optimal loading of Mo was 4?wt.%. The best Mo O3/Ce O2-Ti O2 catalyst displayed over 90% NO conversion from 200 °C to 400 °C and obtained 4-fold increase in NO conversion compared to Ce O2-Ti O2 at 150 °C. The characterization results revealed that the number of Br?nsted acid sites over Mo O3/Ce O2-Ti O2 was significantly increased, and the adsorption of nitrate species was dramatically weakened because of the coverage of Mo O3, which were favorable for the high NH3-SCR performance. It is believed that the Mo O3/Ce O2-Ti O2 catalyst is a suitable substitute for the NH3-SCR reaction.
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This research was supportedby a grant fromKorea Institute of Science and Technology(2E19500).
文摘Quantum chemical calculation was carried out to choose a promoter which can reduce the poisoning of V2O5/TiO2 catalysts by SO2. Several atoms were chosen as candidates and new catalysts were synthesized by impregnation method. The NOx conversion rate was measured at temperatures between 100 and 400 ℃ and poisoning effect was investigated. The most promising candidate promoter, Se, was excluded because of its high vapor pressure. On the other hand, Sb shows best promoting properties. Sb promoted catalyst reaches the maximum NOx conversion rate at 250 ℃. It also shows considerably enhanced resistance to poisoning of V2O5/TiO2 catalysts by SO2.
基金supported by the Introduction of Talent and Technology Cooperation Plan of Tianjin(14RCGFGX00849)
文摘The influence of sulfation on Pd/Ce0.75Zr0.25O2, Pd/Ce O2-Ti O2 and Pd/Ce O2 was investigated. Physical structure and chemical properties of different catalysts were characterized by N2 adsorption, X-ray diffraction（XRD）, CO chemisorption, X-ray photoelectron spectroscopy（XPS）, Fourier transform infrared spectroscopy（FT-IR） and X-ray fluorescence（XRF）. After 10 h SO2 sulfation, it was found that the decrement on CO oxidation catalytic activity was limited on Pd/Ce0.75Zr0.25O2 compared to Pd/Ce O2-Ti O2 and Pd/Ce O2. It demonstrated that Pd/Ce0.75Zr0.25O2 was more sulfur resistant compared to the other two catalysts. After sulfur exposure, catalyst texture was not much influenced as shown by N2 adsorption and XRD, and surface Pd atoms were poisoned indicated by CO chemisorption results. Pd/Ce0.75Zr0.25O2 and Pd/Ce O2-Ti O2 exhibited less sulfur accumulation compared to Pd/Ce O2 in the sulfation process. Furthermore, XPS results clarified that surface sulfur amount, especially surface sulfates amount on the sulfated catalysts was more crucial for the deactivation in sulfur containing environment.
基金the National Key R&D Program of China(Nos.2016YFC0205200 and 2016YFC0208000)the National Natural Science Foundation of China(No.51676127)
文摘CuCeZrO_x and KCuCeZrO_x catalysts were synthesized and coated on the blank diesel particulate filter(DPF)substrate and a particulate matter(PM)loading apparatus was used for soot loading.The catalytic performances of soot oxidation were evaluated by temperature programmed combustion(TPC)test and characterization tests were conducted to investigate the physicochemical properties of the catalysts.The reaction mechanism in the oxidation process was analyzed with diffuse reflectance infrared Fourier transform spectroscopy.The results demonstrated that CuCeZrO_x catalyst exhibited high activities of soot oxidation at low temperature and the best results have been attained with Cu_(0.9)Ce_(0.05)Zr_(0.05)O_x over which the maximum soot oxidation rate decreased to 410~?C.Characterization tests have shown that catalysts containing 90%Cu have uniformly distributed grains and small particle sizes,which provide excellent oxidation activity by providing more active sites and forming a good bond between the catalyst and the soot.The low-temperature oxidation activity of soot could be further optimized due to the excellent elevated NO’s conversion rate by partially substituting Cu with K.The maximum particle oxidation rate can be easily realized at such a low temperature as 347~?C.
