Artificial zeolite was modified by nano-Fe3O4 for development of functional adsorbents.Subsequently,adsorbents such as calcium cross-linked nano-Fe3O4 microspheres (Ca-MS),calcium cross-linked nano-Fe3O4 modified zeol...Artificial zeolite was modified by nano-Fe3O4 for development of functional adsorbents.Subsequently,adsorbents such as calcium cross-linked nano-Fe3O4 microspheres (Ca-MS),calcium cross-linked nano-Fe3O4 modified zeolite microspheres (Ca-MZS) and iron cross-linked nano-Fe3O4 modified zeolite microspheres (Fe-MZS) were prepared and compared for their adsorption performance.The effects of adsorbent dosage,solution pH,initial concentration and ion content on the removal of Cu^2+ from wastewater are investigated,and the adsorption kinetics and isotherms for the adsorbent materials were analyzed.The experimental results indicate that for the initial concentration of Cu^2+ of 30 mg/L,the adsorption is noted to be most stable.The optimal initial pH for adsorbing Cu^2+ is observed to be 5.5.At an optimal dosage of Ca-MZS of 900 mg/L,the adsorption capacity is measured to be 28.25 mg/g,along with the removal rate of 72.49%.The addition of Na+ and K+ affects the adsorption of Cu^2+.For the Na^+ and K^+ concentration of 0.2 mmol/L,the Cu^2+ removal rate by Ca-MZS drops to 11.94% and 22.12%,respectively.As compared with the adsorbents such as Natural Zeolite (NZ),Ca-MS and Fe-MZS,Ca-MZS demonstrates the best removal effect in solution,where the removal rate reaches 84.27%,with the maximum adsorption capacity of 28.09 mg/g.The Cu^2+ adsorption kinetics of Ca-MZS is observed to follow the Elovich kinetic model,with the adsorption isotherm data fitting the Freundlich isotherm model by using the non-linear method.展开更多
The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are ...The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are subjected to hydrothermal treatment at four different temperatures. For zeolite with a lower initial SiO2/Al2O3 ratio of 4.2, mesopores are easily formed because more framework aluminum is detached. Moreover, two kinds of mesopores are produced at a higher temperature due to the interconnection of vacancies and smaller mesopores. For zeolite with a higher initial SiO2/Al2O3 ratio of 6.0, there are less mesopores formed as compared with the lower initial SiO2/Al2O3 ratio sample, but there are some macropores formed. This may be attributed to the isolation of vacancies and the different distributions of aluminum in the crystal lattice of the zeolite. The experiment data show that NaY with the SiO2/Al2O3 ratio of 6.0 retains a high relative crystallinity during the hydrothermal treatment. This proves that a high framework SiO2/Al2O3 ratio benefits the stability of zeolite.展开更多
ITQ-2 zeolites were prepared by sequential alkali-swelling and ultrasonic-delamination of precursor MCM-22 and characterized by X-ray powder diffraction, scanning electron microscopy, nitrogen adsorption-desorption, a...ITQ-2 zeolites were prepared by sequential alkali-swelling and ultrasonic-delamination of precursor MCM-22 and characterized by X-ray powder diffraction, scanning electron microscopy, nitrogen adsorption-desorption, ammonia temperature-programmed desorption and in-situ Fourier-transform infrared spectroscopy. The delamination induced a change in the morphology of ITQ-2 zeolites from aggregated thin platelets to scattered platelets, together with a significant increase in external specific surface area, which reached a plateau at the ultrasonic treatment time of 3 h. The catalytic cracking of n-dodecane over ITQ-2 zeolites was evaluated with ITQ-2 coated on the inside wall of a tubular reactor at 550 ℃ and 4 MPa. The sample obtained by ultrasonic treatment of 3 h （ITQ-2-3） gave the highest initial conversion of n-dodecane, whereas those of 5 h and I h gave the conversion even lower than MCM-22, which was in agreement with the trend of the ratio of strong Lewis acid to the total acid amount. Although the amount of cokes deposited on ITQ-2-3 was larger than that on MCM-22, the former deactivated slowly, suggesting that a large external specific surface area benefits the stability of zeolite coatings,展开更多
In this paper,we have investigated the spectral characteristics of Eu^(3+)ion sorbed on NaY,NaX and NaA zeolites.During calcination,the influence of Eu^(3+)ion's positions in zeolites on its spectral structures ar...In this paper,we have investigated the spectral characteristics of Eu^(3+)ion sorbed on NaY,NaX and NaA zeolites.During calcination,the influence of Eu^(3+)ion's positions in zeolites on its spectral structures are dis- cussed emphatically.The experimental results show that the electric dipole-to-magnetic dipole transition inten- sity ratios of Eu^(3+)emission in NaY,NaX and NaA zeolites calcinated at the same temperature increase in proper order.The bonding actions between Eu^(3+)ion and framework oxygens are studied by the measurements of excitation spectra and X-ray photoelectron spectroscopy.In the Eu^(3+)content ranging from 0.95% to 10.5%,the concentration quenching of the fluorescence in Eu(Ⅲ)-NaY is not observed.展开更多
The dispersion behavior of MoO_3 on ZSM-11 and effect of dispersed MoO_3 on the fram ework structure of ZSM-11 have been studjed using X-ray diffraction and infrared spectroscopy
An Hβ-supported heteropoly acid （H3PW12O40 （HPW）/Hβ） catalyst was successfully prepared by wetness impregnation, and investigated in the alkylation of toluene with tert-butyl alcohol for the synthesis of 4-tert-...An Hβ-supported heteropoly acid （H3PW12O40 （HPW）/Hβ） catalyst was successfully prepared by wetness impregnation, and investigated in the alkylation of toluene with tert-butyl alcohol for the synthesis of 4-tert-butyltoluene （PTBT）. X-ray diffraction, scanning electron microscopy, transmis- sion electron microscopy, fourier-transform infrared spectroscopy, inductively coupled plas- ma-optical emission spectrometry, the brunauer emmett teller （BET） method, tempera- ture-programmed NH3 desorption, and pyridine adsorption infrared spectroscopy were used to characterize the catalyst. The results showed that loading HPW on Hβ effectively increased the B acidity and decreased the pore size of Hβ. The B acidity of HPW/Hβ was 142.97 μmol/g, which is 69.74% higher than that of Hβ （84.23 μmol/g）. The catalytic activity of the HPW/Hβ catalyst was much better than that of the parent Hβ zeolite because of its high B acidity. The toluene conversion over HPW/Hβ reached 73.1%, which is much higher than that achieved with Hβ （54.0%）. When HPW was loaded on Hβ, the BET surface area of Hβ decreased from 492.5 to 379.6 m2/g, accompa- nied by a significant decrease in the pore size from 3.90 to 3.17 nm. Shape selectivity can therefore play an important role and increase the product selectivity of the HPW/Hβ catalyst compared with that of the parent Hβ. PTBT （kinetic diameter 0.58 nm） can easily diffuse through the narrowed pores of HPW/Hβ, but 3-tert-butyltoluene （kinetic diameter 0.65 nm） diffusion is restricted because of steric hindrance in these narrow pores. This results in high PTBT selectivity over HPW/Hβ （around 81%）. The HPW/Hβ catalyst gave a stable catalytic performance in reusability tests.展开更多
A series of phosphorus-modified PITQ-13 catalysts was prepared by wet impregnation of NH4H2PO4 solution into an HITQ-13 parent. The catalysts were characterized using XRD, N2 adsorption, MAS NMR and NH3-TPD. Their cat...A series of phosphorus-modified PITQ-13 catalysts was prepared by wet impregnation of NH4H2PO4 solution into an HITQ-13 parent. The catalysts were characterized using XRD, N2 adsorption, MAS NMR and NH3-TPD. Their catalytic performance in 1-butene catalytic cracking was evaluated in a fixed fluidized bed reactor. The results showed that the crystallinity, surface area and pore volume of P-modified PITQ-13 catalysts decreased with the increasing amounts of P. The number of weak acid sites increased, whereas that of strong acidity decreased. The selectivity to propylene in 1-butene cracking reactions increased because of the decrease in strong acidity. The yield of propylene achieved 41.6% over PITQ-13-2 catalyst with a P content of 1.0 wt%, which was 5.1% greater than that achieved over HITQ-13 catalyst.展开更多
In this paper,a novel compound was developed by mixing H_(3)PO_(4)-modified cauliflower leaves hydrochar(CLH)and coal gangue-based Na-X zeolite(ZL).An alkaline soil contaminated with cadmium(Cd)and lead(Pb)was amended...In this paper,a novel compound was developed by mixing H_(3)PO_(4)-modified cauliflower leaves hydrochar(CLH)and coal gangue-based Na-X zeolite(ZL).An alkaline soil contaminated with cadmium(Cd)and lead(Pb)was amended through the individual and synergistic application of CLH and ZL(1%CLH,2%CLH,1%ZL,2%ZL and 1%CLH+1%ZL),and Chinese cabbage was grown on it.Individual application of CLH was superior to ZL on decreasing the pH of alkaline soil and increasing soil available phosphorus(Olsen-P)and soil organic matter(SOM).In contrast,their combined application significantly improved the soil cation exchange capacity(CEC).Besides,the 1%CLH+1%ZL was the most efficient treatment in decreasing diethylenetriamine pentaacetate(DTPA)-extractable Cd/Pb and concentrations of these two metals in cabbage root and shoot.Their synergistic application could better increase Cd and Pb immobilization and cabbage yield than their alone application.Furthermore,the immobilization of Pb for all treatments was higher than that of Cd.The synergistic immobilization mechanism of CLH and ZL reflected that the CLH precipitated and complexed with these two metals,which may block the pores of hydrochar or wrap on the surface of hydrochar.So the continuous adsorption and complexation were prevented.Nevertheless,ZL could probably alleviate this obstacle.This finding provides helpful information about using CLH combined with ZL as a soil stabilizer to immobilize heavy metals in contaminated alkaline soil.展开更多
When spacecraft operate in space,most organic materials will release small molecular hydrocarbons and large molecular organic gases due to gas evolution effect under high vacuum conditions.These gases can deposit on t...When spacecraft operate in space,most organic materials will release small molecular hydrocarbons and large molecular organic gases due to gas evolution effect under high vacuum conditions.These gases can deposit on the surface of spacecraft,adversely affecting its performance.Adsorption becomes the first choice for removing such organic pollutants in the space environment.Zeolite material has a stable and dense porous structure,and has been widely used in the field of pollution adsorption.In this work,Al2O3 was deposited on the surfaces of 5A zeolite for the first time by atomic layer deposition(ALD)technology.As a result,the adsorption performance of Al2O3 coated 5A zeolite(zeolite@Al2O3)was significantly modified.The corresponding adsorption process was clarified via adsorption kinetics study.展开更多
In order to separate ZSM-5 zeolite powders from solution easily, a series of magnetic ZSM-5 zeolites were prepared by hydrothermal synthesis with the addition of magnetic Fe3O4 panicles during the crystalline process....In order to separate ZSM-5 zeolite powders from solution easily, a series of magnetic ZSM-5 zeolites were prepared by hydrothermal synthesis with the addition of magnetic Fe3O4 panicles during the crystalline process. The products were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, infrared （IR） spectrum, energy dispersive X-ray （EDX）, specific surface area, magnetic susceptibility and adsorption capability. It was found that the magnetic ZSM-5 zeolites had good magnetism and the magnetic susceptibility increased with the increasing amount of Fe3O4 panicles. Compared with the pure ZSM-5 zeolite, the adsorption capability of magnetic ZSM-5 zeolites was acceptable. When the magnetic zeolites were used to adsorb Pb^2＋ from solution, the magnetic zeolite powder could be conveniently separated with magnetic separation technology.展开更多
基金Funded by the Science Foundation of Hubei Province of China(2015CFB706)。
文摘Artificial zeolite was modified by nano-Fe3O4 for development of functional adsorbents.Subsequently,adsorbents such as calcium cross-linked nano-Fe3O4 microspheres (Ca-MS),calcium cross-linked nano-Fe3O4 modified zeolite microspheres (Ca-MZS) and iron cross-linked nano-Fe3O4 modified zeolite microspheres (Fe-MZS) were prepared and compared for their adsorption performance.The effects of adsorbent dosage,solution pH,initial concentration and ion content on the removal of Cu^2+ from wastewater are investigated,and the adsorption kinetics and isotherms for the adsorbent materials were analyzed.The experimental results indicate that for the initial concentration of Cu^2+ of 30 mg/L,the adsorption is noted to be most stable.The optimal initial pH for adsorbing Cu^2+ is observed to be 5.5.At an optimal dosage of Ca-MZS of 900 mg/L,the adsorption capacity is measured to be 28.25 mg/g,along with the removal rate of 72.49%.The addition of Na+ and K+ affects the adsorption of Cu^2+.For the Na^+ and K^+ concentration of 0.2 mmol/L,the Cu^2+ removal rate by Ca-MZS drops to 11.94% and 22.12%,respectively.As compared with the adsorbents such as Natural Zeolite (NZ),Ca-MS and Fe-MZS,Ca-MZS demonstrates the best removal effect in solution,where the removal rate reaches 84.27%,with the maximum adsorption capacity of 28.09 mg/g.The Cu^2+ adsorption kinetics of Ca-MZS is observed to follow the Elovich kinetic model,with the adsorption isotherm data fitting the Freundlich isotherm model by using the non-linear method.
文摘The effects of the initial framework SiO2/Al2O3 ratio and temperature on the structural changes of NaY zeolites during hydrothermal treatments are studied. Two samples with different framework SiO2/Al2O3 ratios are subjected to hydrothermal treatment at four different temperatures. For zeolite with a lower initial SiO2/Al2O3 ratio of 4.2, mesopores are easily formed because more framework aluminum is detached. Moreover, two kinds of mesopores are produced at a higher temperature due to the interconnection of vacancies and smaller mesopores. For zeolite with a higher initial SiO2/Al2O3 ratio of 6.0, there are less mesopores formed as compared with the lower initial SiO2/Al2O3 ratio sample, but there are some macropores formed. This may be attributed to the isolation of vacancies and the different distributions of aluminum in the crystal lattice of the zeolite. The experiment data show that NaY with the SiO2/Al2O3 ratio of 6.0 retains a high relative crystallinity during the hydrothermal treatment. This proves that a high framework SiO2/Al2O3 ratio benefits the stability of zeolite.
文摘ITQ-2 zeolites were prepared by sequential alkali-swelling and ultrasonic-delamination of precursor MCM-22 and characterized by X-ray powder diffraction, scanning electron microscopy, nitrogen adsorption-desorption, ammonia temperature-programmed desorption and in-situ Fourier-transform infrared spectroscopy. The delamination induced a change in the morphology of ITQ-2 zeolites from aggregated thin platelets to scattered platelets, together with a significant increase in external specific surface area, which reached a plateau at the ultrasonic treatment time of 3 h. The catalytic cracking of n-dodecane over ITQ-2 zeolites was evaluated with ITQ-2 coated on the inside wall of a tubular reactor at 550 ℃ and 4 MPa. The sample obtained by ultrasonic treatment of 3 h （ITQ-2-3） gave the highest initial conversion of n-dodecane, whereas those of 5 h and I h gave the conversion even lower than MCM-22, which was in agreement with the trend of the ratio of strong Lewis acid to the total acid amount. Although the amount of cokes deposited on ITQ-2-3 was larger than that on MCM-22, the former deactivated slowly, suggesting that a large external specific surface area benefits the stability of zeolite coatings,
基金The project supported by the Science Foundation of Laboratory of Rare Earth Chemistry and Physics
文摘In this paper,we have investigated the spectral characteristics of Eu^(3+)ion sorbed on NaY,NaX and NaA zeolites.During calcination,the influence of Eu^(3+)ion's positions in zeolites on its spectral structures are dis- cussed emphatically.The experimental results show that the electric dipole-to-magnetic dipole transition inten- sity ratios of Eu^(3+)emission in NaY,NaX and NaA zeolites calcinated at the same temperature increase in proper order.The bonding actions between Eu^(3+)ion and framework oxygens are studied by the measurements of excitation spectra and X-ray photoelectron spectroscopy.In the Eu^(3+)content ranging from 0.95% to 10.5%,the concentration quenching of the fluorescence in Eu(Ⅲ)-NaY is not observed.
文摘Ru3(CO)12 entrapped within NaY zeolite cages was prepared by monolayer dispersion technique.which can be reversibly decarbonylated and recarbonylated.
文摘The dispersion behavior of MoO_3 on ZSM-11 and effect of dispersed MoO_3 on the fram ework structure of ZSM-11 have been studjed using X-ray diffraction and infrared spectroscopy
文摘An Hβ-supported heteropoly acid （H3PW12O40 （HPW）/Hβ） catalyst was successfully prepared by wetness impregnation, and investigated in the alkylation of toluene with tert-butyl alcohol for the synthesis of 4-tert-butyltoluene （PTBT）. X-ray diffraction, scanning electron microscopy, transmis- sion electron microscopy, fourier-transform infrared spectroscopy, inductively coupled plas- ma-optical emission spectrometry, the brunauer emmett teller （BET） method, tempera- ture-programmed NH3 desorption, and pyridine adsorption infrared spectroscopy were used to characterize the catalyst. The results showed that loading HPW on Hβ effectively increased the B acidity and decreased the pore size of Hβ. The B acidity of HPW/Hβ was 142.97 μmol/g, which is 69.74% higher than that of Hβ （84.23 μmol/g）. The catalytic activity of the HPW/Hβ catalyst was much better than that of the parent Hβ zeolite because of its high B acidity. The toluene conversion over HPW/Hβ reached 73.1%, which is much higher than that achieved with Hβ （54.0%）. When HPW was loaded on Hβ, the BET surface area of Hβ decreased from 492.5 to 379.6 m2/g, accompa- nied by a significant decrease in the pore size from 3.90 to 3.17 nm. Shape selectivity can therefore play an important role and increase the product selectivity of the HPW/Hβ catalyst compared with that of the parent Hβ. PTBT （kinetic diameter 0.58 nm） can easily diffuse through the narrowed pores of HPW/Hβ, but 3-tert-butyltoluene （kinetic diameter 0.65 nm） diffusion is restricted because of steric hindrance in these narrow pores. This results in high PTBT selectivity over HPW/Hβ （around 81%）. The HPW/Hβ catalyst gave a stable catalytic performance in reusability tests.
基金supported by PetroChina Company Limited(12-09-01-01)the National Basic Research Program of China(973 Program,2012CB215001)
文摘A series of phosphorus-modified PITQ-13 catalysts was prepared by wet impregnation of NH4H2PO4 solution into an HITQ-13 parent. The catalysts were characterized using XRD, N2 adsorption, MAS NMR and NH3-TPD. Their catalytic performance in 1-butene catalytic cracking was evaluated in a fixed fluidized bed reactor. The results showed that the crystallinity, surface area and pore volume of P-modified PITQ-13 catalysts decreased with the increasing amounts of P. The number of weak acid sites increased, whereas that of strong acidity decreased. The selectivity to propylene in 1-butene cracking reactions increased because of the decrease in strong acidity. The yield of propylene achieved 41.6% over PITQ-13-2 catalyst with a P content of 1.0 wt%, which was 5.1% greater than that achieved over HITQ-13 catalyst.
基金This work was financially supported by the National Natural Science Foundation of China(No.21701099)the Science and Technology Innovation Project of Colleges and Universities of Shanxi Province in 2020(No.2020L0721)the Basic Research Project of Shanxi Province,China(No.201801D121267).
文摘In this paper,a novel compound was developed by mixing H_(3)PO_(4)-modified cauliflower leaves hydrochar(CLH)and coal gangue-based Na-X zeolite(ZL).An alkaline soil contaminated with cadmium(Cd)and lead(Pb)was amended through the individual and synergistic application of CLH and ZL(1%CLH,2%CLH,1%ZL,2%ZL and 1%CLH+1%ZL),and Chinese cabbage was grown on it.Individual application of CLH was superior to ZL on decreasing the pH of alkaline soil and increasing soil available phosphorus(Olsen-P)and soil organic matter(SOM).In contrast,their combined application significantly improved the soil cation exchange capacity(CEC).Besides,the 1%CLH+1%ZL was the most efficient treatment in decreasing diethylenetriamine pentaacetate(DTPA)-extractable Cd/Pb and concentrations of these two metals in cabbage root and shoot.Their synergistic application could better increase Cd and Pb immobilization and cabbage yield than their alone application.Furthermore,the immobilization of Pb for all treatments was higher than that of Cd.The synergistic immobilization mechanism of CLH and ZL reflected that the CLH precipitated and complexed with these two metals,which may block the pores of hydrochar or wrap on the surface of hydrochar.So the continuous adsorption and complexation were prevented.Nevertheless,ZL could probably alleviate this obstacle.This finding provides helpful information about using CLH combined with ZL as a soil stabilizer to immobilize heavy metals in contaminated alkaline soil.
基金National Natural Science Foundation of China(Grant No.51702067).
文摘When spacecraft operate in space,most organic materials will release small molecular hydrocarbons and large molecular organic gases due to gas evolution effect under high vacuum conditions.These gases can deposit on the surface of spacecraft,adversely affecting its performance.Adsorption becomes the first choice for removing such organic pollutants in the space environment.Zeolite material has a stable and dense porous structure,and has been widely used in the field of pollution adsorption.In this work,Al2O3 was deposited on the surfaces of 5A zeolite for the first time by atomic layer deposition(ALD)technology.As a result,the adsorption performance of Al2O3 coated 5A zeolite(zeolite@Al2O3)was significantly modified.The corresponding adsorption process was clarified via adsorption kinetics study.
基金Supported by National Natural Science Foundation of China(No.20476021)Natural Science Foundation of Hebei Province(No.B2010000042)+1 种基金Tianjin Natural Science Foundation(No.10JCYBJC04300)Program for Changjiang Scholars and Innovative Research Teamin University(IRT1059)
文摘In order to separate ZSM-5 zeolite powders from solution easily, a series of magnetic ZSM-5 zeolites were prepared by hydrothermal synthesis with the addition of magnetic Fe3O4 panicles during the crystalline process. The products were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, infrared （IR） spectrum, energy dispersive X-ray （EDX）, specific surface area, magnetic susceptibility and adsorption capability. It was found that the magnetic ZSM-5 zeolites had good magnetism and the magnetic susceptibility increased with the increasing amount of Fe3O4 panicles. Compared with the pure ZSM-5 zeolite, the adsorption capability of magnetic ZSM-5 zeolites was acceptable. When the magnetic zeolites were used to adsorb Pb^2＋ from solution, the magnetic zeolite powder could be conveniently separated with magnetic separation technology.
