The effects of the calorimetric buffer solutions were investigated while the two colorimetric reactions of AI-ferron complex and Fe-ferron complex occurred individually, and the effects of the testing wavelength and t...The effects of the calorimetric buffer solutions were investigated while the two colorimetric reactions of AI-ferron complex and Fe-ferron complex occurred individually, and the effects of the testing wavelength and the pH of the solutions were also investigated. A timed complexatian colorimetric analysis method of Al-Fe-ferron in view of the total concentration of {AI + Fe} was then established to determine the species distribution of polymeric Al-Fe. The testing wavelength was recommended at 362 net and the testing pH value was 5. With a comparison of the ratios of n(Al)/n(Fe), the standard adsorption curves of the polymeric Al-Fe solutions were derived from the experimental results. Furthermore, the solutions' composition were carious in both the molar n(Al)/n(Fe) ratios, i.e. 0/0, 5/5, 9/1 and 0/10, and the concentrations associated with the total ( Al + Fe which ranged from 10(-5) to 10(-4) mol/L..展开更多
A novel membrane distillation concentration method was used m prepare high concentration polyaluminum chloride （PAC1） with high content of AID or Ale. 2.52 mol/L PACl1 with 88% Alb and 2.38 mol/L PACl2 with 61% Ale ...A novel membrane distillation concentration method was used m prepare high concentration polyaluminum chloride （PAC1） with high content of AID or Ale. 2.52 mol/L PACl1 with 88% Alb and 2.38 mol/L PACl2 with 61% Ale were successfully prepared. Three coagulants, AlCl3, PACl1 and PACl2 were investigated on their hydrolysis behavior and speciation under different conditions. The effects of pH and dilution ratio on Al species distribution were investigated by ferron assay. Experimental result showed that pH had a significant effect on Al species distribution for the three coagulants. Dilution ratio had little effects on Alb and Alc distribution in whole dilution process except the beginning for PACl1 and PACl2. The results indicated that transformation of Al depends largely on their original composition. AlCl3 was the most unstable coagulant among these three coagulants during hydrolysis process. PACl1 and PACl2 with significant amounts of highly charged and stable polynuclear aluminum hydrolysis products were less affected by the hydrolysis conditions and could maintain high speciation stability under various conditions.展开更多
Nitrogen oxide(NO_(x))is one of the most critical contaminants in the air,and the control of NO_(x)emission from diesel vehicles is very important.Cu-based small-pore zeolites have already been applied for NO_(x)abate...Nitrogen oxide(NO_(x))is one of the most critical contaminants in the air,and the control of NO_(x)emission from diesel vehicles is very important.Cu-based small-pore zeolites have already been applied for NO_(x)abatement on diesel vehicles.Among the small-pore zeolites,Cu-SSZ-50 catalysts with good NH_(3)-SCR catalytic activity were believed to have potential for application.In this study,a one-pot synthesis method for Cu-SSZ-50 catalysts was developed for the first time,using the co-templates of Cu-TEPA and 2,6-dimethyl-N-methylpyridinium hydroxide.In this synthesis method,Cu-SSZ-50 with various Cu contents can be obtained by adjusting the amount of Cu-TEPA without the need for a further after-treatment process.The addition of Cu-TEPA affected the framework atoms and Cu species,and a lower Si/Al ratio and more SCR active Cu species were obtained.The synthesized catalyst with a Cu/Al ratio of 0.40 exhibited over 90%NO_(x)conversion between 200℃and 450℃for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).Meanwhile,over 80%NO_(x)conversion could be obtained from 250℃to 450℃after hydrothermal aging at 750℃for 16 h.In addition,both L-H and E-R mechanisms were proven to exist for the one-pot-synthesized Cu-SSZ-50 by in situ DRIFTS experiments.The simple synthesis procedure,excellent catalytic activity and hydrothermal stability brighten the prospects for the application of Cu-SSZ-50.展开更多
The flocculation efficiency of polyaluminum chloride (PAC) is closely related to the distribution and structure of its Al species, and Al13 is the optimal species in PAC for flocculation. A series of PAC containing Ca...The flocculation efficiency of polyaluminum chloride (PAC) is closely related to the distribution and structure of its Al species, and Al13 is the optimal species in PAC for flocculation. A series of PAC containing Ca was prepared by adding Ca before and after the basifying reac- tion. The effects of Ca on the Al species were studied by Al 27 nuclear magnetic resonance (NMR) and atomic force micro- scope (AFM) techniques. The experimental results show that the introduction of Ca increases the content of Alm and Al13 in PAC and decreases their chemical shifts in NMR spectra due to the electric repulsion between the positive Ca species and Al species and the formation of Al-O-Ca complexes. With the rise of Ca/Al molar ratio, the Al species in PAC tend to scatter. It is observed that the formerly branch-aggregated clusters are tending to form granule-aggregated ones whose diameter gets smaller and smaller, and the floccule aggre- gates are formed at a higher Ca/Al molar ratio. The intro- duction of Ca to PAC, which increases the Al13 content, is certainly to enhance the flocculation efficiency of PAC in water treatment.展开更多
Influence of total aluminum concentration (CAlT) on the generation and transformation of nanosized Al13 and Al30 in hydrolytic polyaluminum aqueous solutions was in-vestigated using high field 27Al NMR and time-develo...Influence of total aluminum concentration (CAlT) on the generation and transformation of nanosized Al13 and Al30 in hydrolytic polyaluminum aqueous solutions was in-vestigated using high field 27Al NMR and time-developed Al-Ferron complex colorimetry. When prepared at the opti-mal basicity (B) of Al13 generation and 80℃, the Al13 species in polyaluminum solution tends to further polymerize and convert to Al30 and higher polymers when CAlT >0.2 mol·L?1, but Al13 does not convert to Al30 quantificationally, as the formation of Alu from Al13 and Al30 is accelerated in the same way. The conversion rate of Al13 is accelerated by the in-crease in CAlT. When CAlT >0.75 mol·L?1, Al13 content de-creases rapidly, and Al30 content increases continuously and becomes the dominant nanometer polynuclear aluminum species. Alm is one of prerequisites of Al13 conversion to Al30. When CAlT increases and B reduces, the polymerization rate between Al13 and Alm increases, and at the same time, the dissociation reaction rate of Al13 and Al30 by H+ also increases. The latter becomes the dominant reaction in polyaluminum solution with low B value, so Al30 decreases with the increas-ing CAlT. The hydrolytic polyaluminum solution with Al13 content beyond 80% can only be prepared under the condi-tion of CAlT<0.5 mol·L?1 and optimal B value.展开更多
基金TheNationalNaturalScienceFoundationofChina (No .2 96 770 0 4)
文摘The effects of the calorimetric buffer solutions were investigated while the two colorimetric reactions of AI-ferron complex and Fe-ferron complex occurred individually, and the effects of the testing wavelength and the pH of the solutions were also investigated. A timed complexatian colorimetric analysis method of Al-Fe-ferron in view of the total concentration of {AI + Fe} was then established to determine the species distribution of polymeric Al-Fe. The testing wavelength was recommended at 362 net and the testing pH value was 5. With a comparison of the ratios of n(Al)/n(Fe), the standard adsorption curves of the polymeric Al-Fe solutions were derived from the experimental results. Furthermore, the solutions' composition were carious in both the molar n(Al)/n(Fe) ratios, i.e. 0/0, 5/5, 9/1 and 0/10, and the concentrations associated with the total ( Al + Fe which ranged from 10(-5) to 10(-4) mol/L..
基金supported by the National Natural Science Foundation of China (No 50708109, 20577061,40673003)the National Hi-Tech Research and Develop-ment Key Program (863) of China (No 2007AA06Z339)the Special Fund from the State Key Laboratory of Environmental Aquatic Chemistry (No 09Y02ESPCR,09Z01ESPCR)
文摘A novel membrane distillation concentration method was used m prepare high concentration polyaluminum chloride （PAC1） with high content of AID or Ale. 2.52 mol/L PACl1 with 88% Alb and 2.38 mol/L PACl2 with 61% Ale were successfully prepared. Three coagulants, AlCl3, PACl1 and PACl2 were investigated on their hydrolysis behavior and speciation under different conditions. The effects of pH and dilution ratio on Al species distribution were investigated by ferron assay. Experimental result showed that pH had a significant effect on Al species distribution for the three coagulants. Dilution ratio had little effects on Alb and Alc distribution in whole dilution process except the beginning for PACl1 and PACl2. The results indicated that transformation of Al depends largely on their original composition. AlCl3 was the most unstable coagulant among these three coagulants during hydrolysis process. PACl1 and PACl2 with significant amounts of highly charged and stable polynuclear aluminum hydrolysis products were less affected by the hydrolysis conditions and could maintain high speciation stability under various conditions.
基金financially supported by the National Natural Science Foundation of China(Nos.52200136,52225004 and 51978640)the Science and Technology Innovation“2025”major program in Ningbo(No.2020Z103)。
文摘Nitrogen oxide(NO_(x))is one of the most critical contaminants in the air,and the control of NO_(x)emission from diesel vehicles is very important.Cu-based small-pore zeolites have already been applied for NO_(x)abatement on diesel vehicles.Among the small-pore zeolites,Cu-SSZ-50 catalysts with good NH_(3)-SCR catalytic activity were believed to have potential for application.In this study,a one-pot synthesis method for Cu-SSZ-50 catalysts was developed for the first time,using the co-templates of Cu-TEPA and 2,6-dimethyl-N-methylpyridinium hydroxide.In this synthesis method,Cu-SSZ-50 with various Cu contents can be obtained by adjusting the amount of Cu-TEPA without the need for a further after-treatment process.The addition of Cu-TEPA affected the framework atoms and Cu species,and a lower Si/Al ratio and more SCR active Cu species were obtained.The synthesized catalyst with a Cu/Al ratio of 0.40 exhibited over 90%NO_(x)conversion between 200℃and 450℃for the selective catalytic reduction of NO_(x)with NH_(3)(NH_(3)-SCR).Meanwhile,over 80%NO_(x)conversion could be obtained from 250℃to 450℃after hydrothermal aging at 750℃for 16 h.In addition,both L-H and E-R mechanisms were proven to exist for the one-pot-synthesized Cu-SSZ-50 by in situ DRIFTS experiments.The simple synthesis procedure,excellent catalytic activity and hydrothermal stability brighten the prospects for the application of Cu-SSZ-50.
文摘The flocculation efficiency of polyaluminum chloride (PAC) is closely related to the distribution and structure of its Al species, and Al13 is the optimal species in PAC for flocculation. A series of PAC containing Ca was prepared by adding Ca before and after the basifying reac- tion. The effects of Ca on the Al species were studied by Al 27 nuclear magnetic resonance (NMR) and atomic force micro- scope (AFM) techniques. The experimental results show that the introduction of Ca increases the content of Alm and Al13 in PAC and decreases their chemical shifts in NMR spectra due to the electric repulsion between the positive Ca species and Al species and the formation of Al-O-Ca complexes. With the rise of Ca/Al molar ratio, the Al species in PAC tend to scatter. It is observed that the formerly branch-aggregated clusters are tending to form granule-aggregated ones whose diameter gets smaller and smaller, and the floccule aggre- gates are formed at a higher Ca/Al molar ratio. The intro- duction of Ca to PAC, which increases the Al13 content, is certainly to enhance the flocculation efficiency of PAC in water treatment.
基金supported by the National High Technology Research and Development Key Program of China(863 Program)(Grant No.2002AA601290)the National Natural Science Foundation of China(Grant No.50178067).
文摘Influence of total aluminum concentration (CAlT) on the generation and transformation of nanosized Al13 and Al30 in hydrolytic polyaluminum aqueous solutions was in-vestigated using high field 27Al NMR and time-developed Al-Ferron complex colorimetry. When prepared at the opti-mal basicity (B) of Al13 generation and 80℃, the Al13 species in polyaluminum solution tends to further polymerize and convert to Al30 and higher polymers when CAlT >0.2 mol·L?1, but Al13 does not convert to Al30 quantificationally, as the formation of Alu from Al13 and Al30 is accelerated in the same way. The conversion rate of Al13 is accelerated by the in-crease in CAlT. When CAlT >0.75 mol·L?1, Al13 content de-creases rapidly, and Al30 content increases continuously and becomes the dominant nanometer polynuclear aluminum species. Alm is one of prerequisites of Al13 conversion to Al30. When CAlT increases and B reduces, the polymerization rate between Al13 and Alm increases, and at the same time, the dissociation reaction rate of Al13 and Al30 by H+ also increases. The latter becomes the dominant reaction in polyaluminum solution with low B value, so Al30 decreases with the increas-ing CAlT. The hydrolytic polyaluminum solution with Al13 content beyond 80% can only be prepared under the condi-tion of CAlT<0.5 mol·L?1 and optimal B value.
