A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐W...A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐WO3/TiO2 catalyst.The physicochemical properties were investigated by using XRD,BET,NH3‐TPD,H2‐TPR,and XPS,and the catalytic performance and K‐poisoning resistance were evaluated via a NH3‐SCR model reaction.Ce^4+and Zr^4+co‐doping were found to enhance the conversion of NOx,and exhibit the best K‐poisoning resistance owing to the largest BET‐specific surface area,pore volume,and total acid site concentration,as well as the minimal effects on the surface acidity and redox ability from K poisoning.The V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst also presents outstanding H2O+SO2 tolerance.Finally,the in situ DRIFTS reveals that the NH3‐SCR reaction over the V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst follows an L‐H mechanism,and that K poisoning does not change the reaction mechanism.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
基金supported by the National Natural Science Foundation of China(21876168,21507130)the Key Projects for Common Key Technology Innovation in Key Industries in Chongqing(cstc2016zdcy-ztzx0020-01)+2 种基金the Chongqing Science&Technology Commission(cstc2016jcyjA0070,cstckjcxljrc13)the Open Project Program of Chongqing Key Laboratory of Catalysis and Functional Organic Molecules from Chongqing Technology and Business University(1456029)the Graduate Innovation Project of Chongqing Technology and Business University(yjscxx201803-028-22)~~
摘要A series of V2O5‐WO3/TiO2‐ZrO2,V2O5‐WO3/TiO2‐CeO2,and V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalysts were synthesized to improve the selective catalytic reduction(SCR)performance and the K‐poisoning resistance of a V2O5‐WO3/TiO2 catalyst.The physicochemical properties were investigated by using XRD,BET,NH3‐TPD,H2‐TPR,and XPS,and the catalytic performance and K‐poisoning resistance were evaluated via a NH3‐SCR model reaction.Ce^4+and Zr^4+co‐doping were found to enhance the conversion of NOx,and exhibit the best K‐poisoning resistance owing to the largest BET‐specific surface area,pore volume,and total acid site concentration,as well as the minimal effects on the surface acidity and redox ability from K poisoning.The V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst also presents outstanding H2O+SO2 tolerance.Finally,the in situ DRIFTS reveals that the NH3‐SCR reaction over the V2O5‐WO3/TiO2‐CeO2‐ZrO2 catalyst follows an L‐H mechanism,and that K poisoning does not change the reaction mechanism.
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)
摘要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)
摘要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.