Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introdu...Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introduction of contaminants into Cu-SAPO-18,the quantity of acidic sites and Cu^2+ species in catalyst decreases owing to the replacement of H^+ and Cu^2+ by K^+,Na^+,Ca^2+,and Mg^2+.Furthermore,the loss of isolated Cu^2+ induces the generation of CuO and CuAl2O4-like phases,which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst.Consequently,the deNOx performance of the contaminated Cu-SAPO-18 catalysts drops.Such decline in NH3-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/gcatal.In addition,the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K>Na>Ca>Mg,which is consistent with the order of reduction of acidic sites.To a certain degree,the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu2+ and the catalyst framework.Moreover,kinetic analysis of NH3-SCR was conducted,and the results indicate that there is no influence of contaminants on the NH3-SCR mechanism.展开更多
Cu-based catalysts, such as Cu/SiO2, Cu/γ-Al2O3 and Cu/SiO2-Al2O3, for the vapor phase synthesis of N-butylaniline from aniline and 1-butanol were investigated and the catalysts were characterized by BET, H2-TPR, XRD...Cu-based catalysts, such as Cu/SiO2, Cu/γ-Al2O3 and Cu/SiO2-Al2O3, for the vapor phase synthesis of N-butylaniline from aniline and 1-butanol were investigated and the catalysts were characterized by BET, H2-TPR, XRD and NH3-TPD techniques. The results indicated that the dispersion of copper on support was greatly influenced by the interaction between Cu and the support. Copper-based catalyst with larger amounts of acidic sites did not favor the synthesis of N-butylaniline because more by-products were produced. Among the tested catalysts, Cu/SiO2 showed excellent catalytic activity and stability with a yield of N-butylaniline above 90% during the reaction time of 200 h.展开更多
The effects of sorbed phosphate on the kinetics of Cu￣2+ secondary adsorption on three major types ofsoils in southern and Central China were studied using the batch method and flow (or miscible displacement)techniqu...The effects of sorbed phosphate on the kinetics of Cu￣2+ secondary adsorption on three major types ofsoils in southern and Central China were studied using the batch method and flow (or miscible displacement)techniques. Both of the methods showed that diffusions were the ratedetermining steps in the Cu￣2+ adsorp-tion by the soils. By the flow method, the course of Cu￣2+ adsorption kinetics consisted of two steps-sn initialrapid process and a later slow process of Cu￣2+ adsorption; while by the batch method, the 90% of Cu￣2+adsorption reaction was found to finish within first 1 minute. The results obtained using the flow method alsoindicated that for red soil and yellow-brown soil, Cu￣2+ adsorptions during the initial reaction periods wererestrained when the soils sorbed phosphate, whereas the adsorption reactions were stimulated at the finaltime. For grey Chao soil, sorbed phosphate retarded the Cu￣2+ adsorption in the whole reaction period. Theresults obtained using the batch method and flow techniques all implied that the different effects of sorbedphosphate would be attributed to its effects on Cu￣2+ ion diffusion in soil solution.展开更多
The study results of the effects of temperature and ionic strength on the adsorption kineties of Pb￣2+ and Cu￣2+ bylatosol, red soil and kaolinte coated with Mn oxide showed that Pb￣2+ and Cu￣2+ adsorption by all ...The study results of the effects of temperature and ionic strength on the adsorption kineties of Pb￣2+ and Cu￣2+ bylatosol, red soil and kaolinte coated with Mn oxide showed that Pb￣2+ and Cu￣2+ adsorption by all samples, as awhole, increased with missing temperature. Temperature also increased both values of X_m (the amount of ionadsorbed at equilibrium) and k (kinetica constant) of Pb￣2+ and Cu￣2+. The activation energies of Pb￣2+ adsorption werekaolin-Mn >red soil>goethite and those of Cu￣2+ were latosol> red soil > kaolin-Mn >goethite. For a given singlesample the activation energy of Cu￣2+ was greater than that of Pb￣2+. Raising ionic strength decreased the adsorptionof Pb￣2+ and Cu￣2+ by latosol, red soil and kaolinite coated with Mn oxide but increased Pb￣2+ and Cu￣2+ adsorption bygoethite. The contrary results could be explained by the different changes in ion forms of Pb￣2+ or Cu￣2+ and in surfacecbarge characteristics of latosol, red soil, kaolin-Mn and goethite. Increasing supporting electrolyte concentration in-creased X_m and k in goethite systems but decreased X_m and k in kaolin-Mn systems. All the time-dependent data fit-ted the surface second-order equation very well.展开更多
基金supported by the National Natural Science Foundation of China(21473064)~~
文摘Contaminants(K,Na,Ca,and Mg)were introduced into Cu-SAPO-18 via incipient wetness impregnation to investigate their effect on the selective catalytic reduction of NOx with NH3(NH3-SCR)over Cu-SAPO-18.After the introduction of contaminants into Cu-SAPO-18,the quantity of acidic sites and Cu^2+ species in catalyst decreases owing to the replacement of H^+ and Cu^2+ by K^+,Na^+,Ca^2+,and Mg^2+.Furthermore,the loss of isolated Cu^2+ induces the generation of CuO and CuAl2O4-like phases,which causes further loss in the Brunauer-Emmett-Teller surface area of the catalyst.Consequently,the deNOx performance of the contaminated Cu-SAPO-18 catalysts drops.Such decline in NH3-SCR performance becomes more pronounced by increasing the contaminant contents from 0.5 to 1.0 mmol/gcatal.In addition,the deactivation influence of the contaminants on Cu-SAPO-18 is presented in the order of K>Na>Ca>Mg,which is consistent with the order of reduction of acidic sites.To a certain degree,the effect of the acidic sites on the deactivation of Cu-SAPO-18 might be more significant than that of isolated Cu2+ and the catalyst framework.Moreover,kinetic analysis of NH3-SCR was conducted,and the results indicate that there is no influence of contaminants on the NH3-SCR mechanism.
基金financially supported by the Innovative Research Team in University of Liaoning (No. 2008T106)
文摘Cu-based catalysts, such as Cu/SiO2, Cu/γ-Al2O3 and Cu/SiO2-Al2O3, for the vapor phase synthesis of N-butylaniline from aniline and 1-butanol were investigated and the catalysts were characterized by BET, H2-TPR, XRD and NH3-TPD techniques. The results indicated that the dispersion of copper on support was greatly influenced by the interaction between Cu and the support. Copper-based catalyst with larger amounts of acidic sites did not favor the synthesis of N-butylaniline because more by-products were produced. Among the tested catalysts, Cu/SiO2 showed excellent catalytic activity and stability with a yield of N-butylaniline above 90% during the reaction time of 200 h.
文摘The effects of sorbed phosphate on the kinetics of Cu￣2+ secondary adsorption on three major types ofsoils in southern and Central China were studied using the batch method and flow (or miscible displacement)techniques. Both of the methods showed that diffusions were the ratedetermining steps in the Cu￣2+ adsorp-tion by the soils. By the flow method, the course of Cu￣2+ adsorption kinetics consisted of two steps-sn initialrapid process and a later slow process of Cu￣2+ adsorption; while by the batch method, the 90% of Cu￣2+adsorption reaction was found to finish within first 1 minute. The results obtained using the flow method alsoindicated that for red soil and yellow-brown soil, Cu￣2+ adsorptions during the initial reaction periods wererestrained when the soils sorbed phosphate, whereas the adsorption reactions were stimulated at the finaltime. For grey Chao soil, sorbed phosphate retarded the Cu￣2+ adsorption in the whole reaction period. Theresults obtained using the batch method and flow techniques all implied that the different effects of sorbedphosphate would be attributed to its effects on Cu￣2+ ion diffusion in soil solution.
文摘The study results of the effects of temperature and ionic strength on the adsorption kineties of Pb￣2+ and Cu￣2+ bylatosol, red soil and kaolinte coated with Mn oxide showed that Pb￣2+ and Cu￣2+ adsorption by all samples, as awhole, increased with missing temperature. Temperature also increased both values of X_m (the amount of ionadsorbed at equilibrium) and k (kinetica constant) of Pb￣2+ and Cu￣2+. The activation energies of Pb￣2+ adsorption werekaolin-Mn >red soil>goethite and those of Cu￣2+ were latosol> red soil > kaolin-Mn >goethite. For a given singlesample the activation energy of Cu￣2+ was greater than that of Pb￣2+. Raising ionic strength decreased the adsorptionof Pb￣2+ and Cu￣2+ by latosol, red soil and kaolinite coated with Mn oxide but increased Pb￣2+ and Cu￣2+ adsorption bygoethite. The contrary results could be explained by the different changes in ion forms of Pb￣2+ or Cu￣2+ and in surfacecbarge characteristics of latosol, red soil, kaolin-Mn and goethite. Increasing supporting electrolyte concentration in-creased X_m and k in goethite systems but decreased X_m and k in kaolin-Mn systems. All the time-dependent data fit-ted the surface second-order equation very well.
