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
8wt%WO3/SiO2 metathesis (disproportionation) catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-deso...8wt%WO3/SiO2 metathesis (disproportionation) catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy (SEM), X-ray diffraction (XRD), UV-visible diffuse reflectance spectroscopy (DRS) and scanning transmission electron microscopy-high-angle annular dark field (STEM HAADF). The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure: The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.展开更多
The influence of tungsten trioxide(WO3)loading on the selective catalytic reduction(SCR)of nitric oxide(NO)by ammonia(NH3)over WO3/cerium dioxide(CeO2)was investigated.The NO conversion first rose and then declined wi...The influence of tungsten trioxide(WO3)loading on the selective catalytic reduction(SCR)of nitric oxide(NO)by ammonia(NH3)over WO3/cerium dioxide(CeO2)was investigated.The NO conversion first rose and then declined with increasing WO3loading.It was found that the crystalline WO3in the1.6WO3/CeO2sample could be removed in25wt%ammonium hydroxide at70°C,which improved the catalytic activity of the sample.The obtained samples were characterized by X‐ray diffraction,Raman spectroscopy,X‐ray photoelectron spectroscopy,hydrogen(H2)temperature programmed reduction,NH3temperature programmed desorption,and in situ diffuse reflectance infrared Fourier transform spectroscopy.The results revealed that the dispersed WO3promoted the catalytic activity of WO3/CeO2while the crystalline WO3inhibited catalytic activity.The oxygen activation of CeO2was inhibited by the coverage of WO3,which weakened NO oxidation and adsorption of nitrate species over WO3/CeO2.In addition,the NH3adsorption performance on CeO2was improved by modification with WO3.NH3was the most stable adsorbed species under NH3SCR reaction conditions.In situ DRIFT spectra suggested that the NH3SCR reaction proceeded via the Eley‐Rideal mechanism over WO3/CeO2.Thus,when the loading of WO3was close to the dispersion capacity,the effects of NH3adsorption and activation were maximized to promote the reaction via the Eley‐Rideal route.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)~~
文摘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.
文摘8wt%WO3/SiO2 metathesis (disproportionation) catalysts with different pore structures were prepared by the incipient-wetness-impregnation method. The as-synthesized catalysts were characterized by N2 adsorpfion-desorption, scanning electron microscopy (SEM), X-ray diffraction (XRD), UV-visible diffuse reflectance spectroscopy (DRS) and scanning transmission electron microscopy-high-angle annular dark field (STEM HAADF). The results of STEM HAADF showed that WO3 species were not uniformly distributed on the SiO2 support. The experimental results of 8wt%WO3/SiO2 performance in ethene/decene metathesis revealed that the catalytic effect of 8wt%WO3/SiO2 catalyst and coke formation over it were closely related to the support pore structure: The 8wt%WO3/SiO2 catalyst with a more complicated pore structure showed better catalytic performance but the coke deposition rate was also faster.
基金supported by the National Natural Foundation of China(21607019,21503115)the Open Project Program of Jiangsu Key Laboratory of Vehicle Emissions Control(OVEC013)the Talent Introduction Project of Chongqing Three Gorges University~~
文摘The influence of tungsten trioxide(WO3)loading on the selective catalytic reduction(SCR)of nitric oxide(NO)by ammonia(NH3)over WO3/cerium dioxide(CeO2)was investigated.The NO conversion first rose and then declined with increasing WO3loading.It was found that the crystalline WO3in the1.6WO3/CeO2sample could be removed in25wt%ammonium hydroxide at70°C,which improved the catalytic activity of the sample.The obtained samples were characterized by X‐ray diffraction,Raman spectroscopy,X‐ray photoelectron spectroscopy,hydrogen(H2)temperature programmed reduction,NH3temperature programmed desorption,and in situ diffuse reflectance infrared Fourier transform spectroscopy.The results revealed that the dispersed WO3promoted the catalytic activity of WO3/CeO2while the crystalline WO3inhibited catalytic activity.The oxygen activation of CeO2was inhibited by the coverage of WO3,which weakened NO oxidation and adsorption of nitrate species over WO3/CeO2.In addition,the NH3adsorption performance on CeO2was improved by modification with WO3.NH3was the most stable adsorbed species under NH3SCR reaction conditions.In situ DRIFT spectra suggested that the NH3SCR reaction proceeded via the Eley‐Rideal mechanism over WO3/CeO2.Thus,when the loading of WO3was close to the dispersion capacity,the effects of NH3adsorption and activation were maximized to promote the reaction via the Eley‐Rideal route.