The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorabl...The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorable site for the distribution of Fe is T1O6,followed by T2O5,T4O2 and T3O1,and energy differences for Fe in different T sites are less than 0.09 eV,indicating that Fe atoms may distribute in all kinds of T sites in MOR.In addition,the adsorption energies for NH3 at each crystallographic position of H-[Fe]MOR were also determined.Finally,it can be concluded that the Br（o）nsted acid site at T2O5 is stronger than the other acid sites,and the adsorption of NH3 on Br（o）nsted acid sites is more stable than on Lewis acid sites.展开更多
Fe3O4-octadecyltrichlorosilane（Fe3O4-OTS）was synthesized and used to remove dyes in a competitive system.Fe3O4-OTS was prepared by slow hydrolysis of OTS in cyclohexane on the surface of Fe3O4obtained through coprec...Fe3O4-octadecyltrichlorosilane（Fe3O4-OTS）was synthesized and used to remove dyes in a competitive system.Fe3O4-OTS was prepared by slow hydrolysis of OTS in cyclohexane on the surface of Fe3O4obtained through coprecipitation method.Scanning electron microscope（SEM）,energy dispersive spectrometer（EDS）,and contact angle analyzer（CA）were used to analyze the properties of Fe3O4-OTS.Methyl orange（MO）and methylene blue（MB）were selected as model molecules to study the influence mechanism of p H and ionic strength on competitive adsorption.The results of EDS and CA indicated that Fe3O4 was modified successfully with OTS on the surface.Silicon appeared and carbon content increased obviously on the surface of adsorbent.Contact angle of adsorbent increased from 0~o to 107~o after being modified by OTS.Fe3O4-OTS showed good separation for MO and MB in competitive system,which has potential to separate dyes in sewage.Separation factor（β~OB）changed from 18.724 to 0.017,when p H changed from 7 to 12,revealing that MO and MB could be separated almost thoroughly by Fe3O4-OTS.p H could change the surface charge of Fe3O4-OTS and structure of dyes,and thus change the interactions of competitive system indirectly.Even though hydrophobic interaction was enhanced,ionic strength reduced the difference of electrostatic interaction between dyes and Fe3O4-OTS.So it is unfavorable to separate dyes with opposite charges when ionic strength increases.These findings may provide theoretical guidances to separate two-component dye pollutants.展开更多
Carbon-coated Fe3O4（ Fe3O4/C） microspheres activated with 1-ethyl-3-（3-dimethylaminopropyl）-carbodiimide hydrochloride（EDC） were prepared, characterized and applied to adsorb bovine serum albumin（BSA）. The pre...Carbon-coated Fe3O4（ Fe3O4/C） microspheres activated with 1-ethyl-3-（3-dimethylaminopropyl）-carbodiimide hydrochloride（EDC） were prepared, characterized and applied to adsorb bovine serum albumin（BSA）. The prepared magnetic microspheres had spherical core-shell structure with a uniform and continuous carbon coating coupled with activation by EDC, and possessed superparamagnetic characteristics. The experimental results showed that the adsorption amount of BSA on the EDC-activated Fe3O4/C（Fe3O4/C-EDC） microspheres was higher than that on the Fe3O4/C microspheres. The maximum adsorption of BSA on Fe3O4/C-EDC microspheres occurred at pH 4.7, which was the isoelectric point of BSA. At low concentrations（below 1.0 M）, salt had no noticeable effect on BSA adsorption. The BSA adsorption of Fe3O4/C-EDC microspheres had a better fit to the Langmuir model than the Freundlich isotherm and Temkin isotherm model, and the kinetic data were well described by the pseudo-second-order model. The adsorption equilibrium could be reached within 20 min. High desorption efficiency（97.6%） of BSA from Fe3O4/C-EDC microspheres was obtained with 0.5 M Na2HPO4（pH 9.4） as the desorbent.展开更多
A facile method for synthesis of the magnetic Fe_3O_4 nanoparticles was introduced.Magnetic nanoparticles were prepared via co-precipitation method with(PMF) and without(AMF) 0.15 T static magnetic field.The effects o...A facile method for synthesis of the magnetic Fe_3O_4 nanoparticles was introduced.Magnetic nanoparticles were prepared via co-precipitation method with(PMF) and without(AMF) 0.15 T static magnetic field.The effects of magnetic field on the properties of magnetic nanoparticles were studied by XRD,TEM,SEM,VSM and BET.The results showed that the magnetic field in the co-precipitation reaction process did not result in the phase change of the Fe_3O_4 nanoparticles but improved the crystallinity.The morphology of Fe_3O_4 nanoparticles was varied from random spherical particles to rod-like cluster structure.The VSM results indicated that the saturation magnetization value of the Fe_3O_4 nanoparticles was significantly improved by the magnetic field.The BET of Fe_3O_4nanoparticles prepared with the magnetic field was larger than the control by 23.5%.The batch adsorption experiments of Mn(Ⅱ) on the PMF and AMF Fe_3O_4 nanoparticles showed that the Mn(II) equilibrium capacity was increased with the pH value increased.At pH 8,the Mn(Ⅱ) adsorption capacity for the PMF and AMF Fe_3O_4 was reached at 36.81 and 28.36 mg·g^(-1),respectively.The pseudo-second-order model fitted better the kinetic models and the Freundlich model fitted isotherm model well for both PMF and AMF Fe_3O_4.The results suggested that magnetic nanoparticles prepared by the magnetic field presented a fairly good potential as an adsorbent for an efficient removal of Mn(Ⅱ) from aqueous solution.展开更多
Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6A...Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.展开更多
In this study, the adsorption kinetics, equilibrium and thermodynamics of Fe3+ ions on natural (NAP) and synthetic (HAP) apaties were examined. The adsorption efficiency of Fe3+ onto the NAP and HAP was increased with...In this study, the adsorption kinetics, equilibrium and thermodynamics of Fe3+ ions on natural (NAP) and synthetic (HAP) apaties were examined. The adsorption efficiency of Fe3+ onto the NAP and HAP was increased with increasing temperature. The kinetics of adsorption of Fe3+ ions was discussed using three kinetic models, the pseudo-first-order, the pseudo-second-order and the intra-particle diffusion model. The experimental data fitted very well the pseudo-second-order kinetic model. The initial sorption rate and the activation energy were also calculated. The activation energy of the sorption was calculated as 37.15 and 49.84 kJ·mol 1 for NAP and HAP, respectively. Experimental results were also analysed by the Langmuir, Freundlich and Dubinin–Redushkevich (D–R) isotherm equations at different temperatures. RL separation factor for Langmuir and the n value for Freundlich isotherm show that Fe3+ ions are favorably adsorbed by NAP and HAP. Various thermodynamic parameters such as enthalpy (ΔH), Gibbs free energy (ΔG) and entropy (ΔS) changes were computed and the results showed that the adsorption of Fe3+ ions onto NAP and HAP were spontaneous and endothermic in nature.展开更多
基金Computational Chemistry Laboratory of School of Chemical Engineering and EnvironmentNatural Science Foundationof Shanxi Province(No.2009011014)Shenzhen Strategic Emerging Industries Special Fund Program of China(No.GGJS20120619101655715)
文摘The distribution of Fe and the adsorption of NH3 in H-[Fe]MOR （mordenite） were investigated using dispersion corrected density functional theory （DFT-D2）.Based on the results,it can be found that the most favorable site for the distribution of Fe is T1O6,followed by T2O5,T4O2 and T3O1,and energy differences for Fe in different T sites are less than 0.09 eV,indicating that Fe atoms may distribute in all kinds of T sites in MOR.In addition,the adsorption energies for NH3 at each crystallographic position of H-[Fe]MOR were also determined.Finally,it can be concluded that the Br（o）nsted acid site at T2O5 is stronger than the other acid sites,and the adsorption of NH3 on Br（o）nsted acid sites is more stable than on Lewis acid sites.
基金Funded by the National Natural Science Foundation of China(Nos.51403229,21401209,and U1507104)the Foundation of Youth Innovation Promotion Association,CAS(Y310031024)+1 种基金the Natural Science Foundation of Qinghai Province(2015-ZJ-933Q)the West Light Foundation of CAS
文摘Fe3O4-octadecyltrichlorosilane（Fe3O4-OTS）was synthesized and used to remove dyes in a competitive system.Fe3O4-OTS was prepared by slow hydrolysis of OTS in cyclohexane on the surface of Fe3O4obtained through coprecipitation method.Scanning electron microscope（SEM）,energy dispersive spectrometer（EDS）,and contact angle analyzer（CA）were used to analyze the properties of Fe3O4-OTS.Methyl orange（MO）and methylene blue（MB）were selected as model molecules to study the influence mechanism of p H and ionic strength on competitive adsorption.The results of EDS and CA indicated that Fe3O4 was modified successfully with OTS on the surface.Silicon appeared and carbon content increased obviously on the surface of adsorbent.Contact angle of adsorbent increased from 0~o to 107~o after being modified by OTS.Fe3O4-OTS showed good separation for MO and MB in competitive system,which has potential to separate dyes in sewage.Separation factor（β~OB）changed from 18.724 to 0.017,when p H changed from 7 to 12,revealing that MO and MB could be separated almost thoroughly by Fe3O4-OTS.p H could change the surface charge of Fe3O4-OTS and structure of dyes,and thus change the interactions of competitive system indirectly.Even though hydrophobic interaction was enhanced,ionic strength reduced the difference of electrostatic interaction between dyes and Fe3O4-OTS.So it is unfavorable to separate dyes with opposite charges when ionic strength increases.These findings may provide theoretical guidances to separate two-component dye pollutants.
基金Funded by the Major Science and Technology Program for Water Pollution Control and Treatment(No.2013ZX07202-010)
文摘Carbon-coated Fe3O4（ Fe3O4/C） microspheres activated with 1-ethyl-3-（3-dimethylaminopropyl）-carbodiimide hydrochloride（EDC） were prepared, characterized and applied to adsorb bovine serum albumin（BSA）. The prepared magnetic microspheres had spherical core-shell structure with a uniform and continuous carbon coating coupled with activation by EDC, and possessed superparamagnetic characteristics. The experimental results showed that the adsorption amount of BSA on the EDC-activated Fe3O4/C（Fe3O4/C-EDC） microspheres was higher than that on the Fe3O4/C microspheres. The maximum adsorption of BSA on Fe3O4/C-EDC microspheres occurred at pH 4.7, which was the isoelectric point of BSA. At low concentrations（below 1.0 M）, salt had no noticeable effect on BSA adsorption. The BSA adsorption of Fe3O4/C-EDC microspheres had a better fit to the Langmuir model than the Freundlich isotherm and Temkin isotherm model, and the kinetic data were well described by the pseudo-second-order model. The adsorption equilibrium could be reached within 20 min. High desorption efficiency（97.6%） of BSA from Fe3O4/C-EDC microspheres was obtained with 0.5 M Na2HPO4（pH 9.4） as the desorbent.
基金Supported by the National Natural Science Foundation of China(No.41201487)the Natural Science Foundation of Hebei Province(No.2014202074)
文摘A facile method for synthesis of the magnetic Fe_3O_4 nanoparticles was introduced.Magnetic nanoparticles were prepared via co-precipitation method with(PMF) and without(AMF) 0.15 T static magnetic field.The effects of magnetic field on the properties of magnetic nanoparticles were studied by XRD,TEM,SEM,VSM and BET.The results showed that the magnetic field in the co-precipitation reaction process did not result in the phase change of the Fe_3O_4 nanoparticles but improved the crystallinity.The morphology of Fe_3O_4 nanoparticles was varied from random spherical particles to rod-like cluster structure.The VSM results indicated that the saturation magnetization value of the Fe_3O_4 nanoparticles was significantly improved by the magnetic field.The BET of Fe_3O_4nanoparticles prepared with the magnetic field was larger than the control by 23.5%.The batch adsorption experiments of Mn(Ⅱ) on the PMF and AMF Fe_3O_4 nanoparticles showed that the Mn(II) equilibrium capacity was increased with the pH value increased.At pH 8,the Mn(Ⅱ) adsorption capacity for the PMF and AMF Fe_3O_4 was reached at 36.81 and 28.36 mg·g^(-1),respectively.The pseudo-second-order model fitted better the kinetic models and the Freundlich model fitted isotherm model well for both PMF and AMF Fe_3O_4.The results suggested that magnetic nanoparticles prepared by the magnetic field presented a fairly good potential as an adsorbent for an efficient removal of Mn(Ⅱ) from aqueous solution.
文摘Aiming to improve the reactive adsorption desulfurization（RADS） performances of Ni/Zn O adsorbents,ZnxAly（OH）2（CO3）z·x H2 O precursor is synthesized by coprecipitation of Zn2＋,AlO-2,and CO2-3; the Zn OZn6Al2O9 composite oxides are obtained by the calcination of ZnxAly（OH）2（CO3）z·x H2 O precursor,and the Ni/Zn O-Zn6Al2O9（6.0 wt% Ni O） adsorbents are prepared by wetness impregnation method. The phase,acid strength,acid type and quantity,morphology,and thermal properties were characterized by X-ray diffraction,temperature-programmed desorption of ammonia,pyridine-adsorbed infrared spectrum,high-resolution transmission electron microscopy,and Thermo Gravimetry-Derivative Thermo Gravimetry（TG-DTG）,respectively. The breakthrough sulfur capacities of six adsorbents are between 34.2 and 47.9 mg/gcat. The kinetic studies indicated that the active energy of RADS（49.4 k J/mol） could reach nano-sized Zn O,the particle size of is about 12.0 nm. All the excellent RADS performances can be due to the high SBET. Also,there are some extents of aromatization reactions that occur,which can be contributed to the B？nsted acid rooted in Zn6Al2O9 composite oxide,and the octane number of products can be preserved well.
文摘In this study, the adsorption kinetics, equilibrium and thermodynamics of Fe3+ ions on natural (NAP) and synthetic (HAP) apaties were examined. The adsorption efficiency of Fe3+ onto the NAP and HAP was increased with increasing temperature. The kinetics of adsorption of Fe3+ ions was discussed using three kinetic models, the pseudo-first-order, the pseudo-second-order and the intra-particle diffusion model. The experimental data fitted very well the pseudo-second-order kinetic model. The initial sorption rate and the activation energy were also calculated. The activation energy of the sorption was calculated as 37.15 and 49.84 kJ·mol 1 for NAP and HAP, respectively. Experimental results were also analysed by the Langmuir, Freundlich and Dubinin–Redushkevich (D–R) isotherm equations at different temperatures. RL separation factor for Langmuir and the n value for Freundlich isotherm show that Fe3+ ions are favorably adsorbed by NAP and HAP. Various thermodynamic parameters such as enthalpy (ΔH), Gibbs free energy (ΔG) and entropy (ΔS) changes were computed and the results showed that the adsorption of Fe3+ ions onto NAP and HAP were spontaneous and endothermic in nature.
