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
The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reducti...The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reduction of NOx by NH3.Four different methods,namely pre-impregnation,post-impregnation,coimpregnation,and co-precipitation,were used to synthesize a series of V2 O5-WO3-TiO2-CeO2-ZrO2 catalysts.The catalysts were characterized by XRD,BET,NH3-TPD,XPS,and H2-TPR techniques.Moreover,the activity and anti-K poisoning performance were tested by an NH3-SCR model reaction.The results show that the introduction of Ce^4+and Zr^4+can improve the catalytic performance of V2O5-WO3/TiO2 catalyst,but the impregnation method cannot enhance the anti-K poisoning performance.Ce^4+and Zr^4+introduced by co-precipitation method can effectively improve the tolerance of K,which is mainly due to the incorporation of Ce^4+and Zr^4+into TiO2 lattice to form a uniform TiO2-CeO2-ZrO2 solid solution,resulting in the optimal surface acidity and redox performance,and reducing the decreases caused by Kpoisoning.Furthermore,based on the best introduction method,we further optimized the molar ratio of Ce^4+/Zr^4+,It is found that the catalyst exhibits the best anti-K poisoning performance when the molar ratio of Ce^4+/Zr^4+is 2:1.展开更多
Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts...Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.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.
基金Project supported by the National Natural Science Foundation of China(21876168)the Key Projects for Common Key Technology Innovation in Key Industries in Chongqing(cstc2016zdcy-ztzx0020-01)+1 种基金Youth Innovation Promotion Association CAS(2019376)the Graduate Innovation Project of Chongqing Technology and Business University(yjscxx201803-028-22)。
文摘The purpose of this work is to explore the effects of the introduction methods of Ce^4+and Zr^4+on the physicochemical properties,activity,and K tolerance of V2 O5-WO3/TiO2 catalyst for the selective catalytic reduction of NOx by NH3.Four different methods,namely pre-impregnation,post-impregnation,coimpregnation,and co-precipitation,were used to synthesize a series of V2 O5-WO3-TiO2-CeO2-ZrO2 catalysts.The catalysts were characterized by XRD,BET,NH3-TPD,XPS,and H2-TPR techniques.Moreover,the activity and anti-K poisoning performance were tested by an NH3-SCR model reaction.The results show that the introduction of Ce^4+and Zr^4+can improve the catalytic performance of V2O5-WO3/TiO2 catalyst,but the impregnation method cannot enhance the anti-K poisoning performance.Ce^4+and Zr^4+introduced by co-precipitation method can effectively improve the tolerance of K,which is mainly due to the incorporation of Ce^4+and Zr^4+into TiO2 lattice to form a uniform TiO2-CeO2-ZrO2 solid solution,resulting in the optimal surface acidity and redox performance,and reducing the decreases caused by Kpoisoning.Furthermore,based on the best introduction method,we further optimized the molar ratio of Ce^4+/Zr^4+,It is found that the catalyst exhibits the best anti-K poisoning performance when the molar ratio of Ce^4+/Zr^4+is 2:1.
基金Project supported by Fujian Provincial Department of Science and Technology,China (2020Y0085)Youth Innovation Promotion Association,Chinese Academy of Sciences (2020309)the Cultivating Project of Strategic Priority Research Program of Chinese Academy of Sciences (XDPB1902)。
文摘Improving the alkali resistance of catalysts for selective catalytic reduction of NO_(x) with NH_(3) is still a challenge.In this work,the co-modification with Fe,Ce and sulfates on V_(2)O_(5)-WO_(3)/TiO_(2) catalysts(denoted as xSFeCeVWTi) significantly enhances its alkali resistance with K element as a representative.A series of xSFeCeVWTi catalysts was synthesized by wet impregnation with designed 0.05Fe/V, 1.5Ce/V and different S/V molar ratios x.The NO_(x) conversion and K resistance of xSFeCeVWTi catalysts increase with the increase of loading amounts of sulfates but no longer further increase as the sulfates load is excessive to block the pores of catalysts and hinder the adsorption of reactants.The optimal modified catalyst in about 2.2S/V actual loading ratio,corresponding to 10.5SFeCeVWTi sample,shows over 99.0%NO_(x) conversion and N_(2) selectivity at 300-400℃ after K-poisoning.The interaction between Fe,Ce and V improves its redox ability but slightly weakens surface acidity,while the proper amount of sulfate species enriches surface Br?nsted acid sites but attenuates its redox capability.However,a balance of redox capacity and surface acidity,caused by Fe,Ce and sulfate co-modification,contributes to the excellent K resistance of 10.5SFeCeVWTi catalyst.Finally,the change of physicochemical properties influences the reaction mechanism which follows the Eley-Rideal mechanism on 10.SSFeCeVWTi catalyst.These results show that the co-modification with Fe,Ce and sulfates is a good way to improve the alkali tolerance of V_(2)O_(5)-WO_(3)/TiO_(2) catalyst in industrial applications.
