This study describes the adsorption features of cadmium on Fe2O3 and MnO2 in alkaline saline conditions. The adsorption reached equilibrium in 6 hours under alkaline conditions. The absorption of cadmium on Fe2O3 and ...This study describes the adsorption features of cadmium on Fe2O3 and MnO2 in alkaline saline conditions. The adsorption reached equilibrium in 6 hours under alkaline conditions. The absorption of cadmium on Fe2O3 and MnO2 was consistent with Freundlich absorption isotherms, and the corresponding adsorption capacities were 16.3 and 16.7 mg·g-1, respectively. Moreover, the adsorption quantity of cadmium on Fe2O3 and MnO2 rose with increas-ing pH from acidic to neutral, and reached the maximum at pH= 9. The coexisting chlorides reduced the adsorption capacity of Fe2O3 and MnO2. The influence intensities of different cations follow the order of CaCl2>>KCl>NaCl. However, the influence of sodium salts on the capacities of Fe2O3 and MnO2 to adsorb cadmium appeared more complicated: the relatively low concentrations of sodium salts could reduce the adsorption capacity; with increasing concentrations of sodium salts, e.g. NaCl and NaNO3. the adsorption capacity decreased continually. Moreover, due to the competition adsorption and precipitation effects, the adsorption capabilities of Na2CO3, NaH2PO4 and Na2HSO4 could also be reduced and cadmium concentrations in the solution were reduced as well.展开更多
Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface ...Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface area and many acidic sites.Compared with bulk S2O82–-Fe2O3,Br?nsted acid catalysts and other reported catalysts,SFS with an Fe2O3 loading of 30%(SFS-30)exhibits an outstanding activity in the probe reaction of alcoholysis of styrene oxide by methanol with 100%yield.Moreover,SFS-30 also shows a more excellent catalytic performance than bulk S2O82–-Fe2O3 towards the alcoholysis of other ROHs(R=C2H5-C4H9).Lewis and Bronsted acid sites on the SFS-30 surfaces are confirmed by pyridine adsorbed infrared spectra.The highly efficient catalytic activity of SFS-30 may be attributed to the synergistic effect from the nano-effect of S2O82–-Fe2O3 nanoparticles and the mesostructure of SBA-15.Finally,SFS-30 shows a good catalytic reusability,providing an 84.1%yield after seven catalytic cycles.展开更多
High-purity(99%)carbon nanocoils(CNCs)have been synthesized by using porousα-Fe2O3/SnO2 catalyst.The yield of CNCs reaches 9,098%after a 6 h growth.This value is much higher than the previously reported data,indicati...High-purity(99%)carbon nanocoils(CNCs)have been synthesized by using porousα-Fe2O3/SnO2 catalyst.The yield of CNCs reaches 9,098%after a 6 h growth.This value is much higher than the previously reported data,indicating that this method is promising to synthesize high-purity CNCs on a large scale.It is considered that an appropriate proportion of Fe and Sn,proper particle size distribution,and a loose-porous aggregate structure of the catalyst are the key points to the high-purity growth of CNCs.Benefiting from the high-purity preparation,a CNC Buckypaper was successfully prepared and the electrical,mechanical,and electrochemical properties were investigated comprehensively.Furthermore,as one of the practical applications,the CNC Buckypaper was successfully utilized as an efficient adsorbent for the removal of methylene blue dye from wastewater with an adsorption efficiency of 90.9%.This study provides a facile and economical route for preparing high-purity CNCs,which is suitable for large-quantity production.Furthermore,the fabrication of macroscopic CNC Buckypaper provides promising alternative of adsorbent or other practical applications.展开更多
The adsorption of C atoms on the α-Fe2O3（001） surface was studied based on density function theory（DFT） ,in which the exchange-correlation potential was chosen as the PBE（Perdew,Burke and Ernzerhof） generalized...The adsorption of C atoms on the α-Fe2O3（001） surface was studied based on density function theory（DFT） ,in which the exchange-correlation potential was chosen as the PBE（Perdew,Burke and Ernzerhof） generalized gradient approximation（GGA） with a plane wave basis set. Upon the optimization on different adsorption sites with coverage of 1/20 and 1/5 ML,it was found that the adsorption of C atoms on the α-Fe2O3（001） surface was chemical adsorption. The coverage can affect the adsorption behavior greatly. Under low coverage,the most stable adsorption geometry lied on the bridged site with the adsorption energy of about 3.22 eV; however,under high coverage,it located at the top site with the energy change of 8.79 eV. Strong chemical reaction has occurred between the C and O atoms at this site. The density of states and population analysis showed that the s,p orbitals of C and p orbital of O give the most contribution to the adsorption bonding. During the adsorption process,O atom shares the electrons with C,and C can only affect the outermost and subsurface layers of α-Fe2O3; the third layer can not be affected obviously.展开更多
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
The activation of adsorbed CO is an important step in CO hydrogenation. The results from TPSR of pre-adsorbed CO with H2 and syngas suggested that the presence of H2 increased the amount of CO adsorption and accelerat...The activation of adsorbed CO is an important step in CO hydrogenation. The results from TPSR of pre-adsorbed CO with H2 and syngas suggested that the presence of H2 increased the amount of CO adsorption and accelerated CO dissociation. The H2 was adsorbed first, and activated to form H＊ over metal sites, then reacted with carbonaceous species. The oxygen species for CO2 formation in the presence of hydrogen was mostly OH^＊, which reacted with adsorbed CO subsequently via CO^＊＋OH^＊ → CO2^＊＋H^＊; however, the direct CO dissociation was not excluded in CO hydrogenation. The dissociation of C-O bond in the presence of H2 proceeded by a concerted mechanism, which assisted the Boudourd reaction of adsorbed CO on the surface via CO^＊＋2H^＊ → CH^＊＋OH^＊. The formation of the surface species （CH） from adsorbed CO proceeded as indicated with the participation of surface hydrogen, was favored in the initial step of the Fischer-Tropsch synthesis.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
The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al...The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al2O3 catalysts was explored in a fixed bed adsorption system. The catalysts maintain nearly 100% NO conversion efficiency at 350℃. Comprehensive tests were carried out to study the adsorption behavior of NH3 and NO over the catalysts. The desorption experiments prove that NH3 and NO are adsorbed on CuO/γ-Al2O3 catalysts. The adsorption behaviors of NH3 and NO were also studied with the in-situ diffusion reflectance infrared Fourier transform spectroscopy methods. The results show that NH3 could be strongly adsorbed on the catalysts, resulting in coordinated NH3 and NH4＋. NO adsorption leads to the formation of bridging bidentate nitrate, chelating bidentate nitrate, and chelating nitro. The interaction of NH3 and NO molecules with the Cu2＋ present on the CAl2O3 （100） surface was investigated by using a periodic density functional theory. The results show that the adsorption of all the molecules on the Cu2＋ site is energetically favorable, whereas NO bound is stronger than that of NH3 with the adsorption site, and key information about the structural and energetic properties was also addressed.展开更多
How to remove trace amount of sulfur in benzene is of significance,and deep desulfurization by Ni-containing absorbents is an efficient and promising method.In this paper,The Raney Ni/Al2 O3 adsorbent was prepared and...How to remove trace amount of sulfur in benzene is of significance,and deep desulfurization by Ni-containing absorbents is an efficient and promising method.In this paper,The Raney Ni/Al2 O3 adsorbent was prepared and its kinetic and thermodynamic characteristics on adsorptive desulfurization of benzene were studied.The results showed that Raney Ni/Al2 O3 adsorbent exhibited good adsorption performance.The equilibrium isotherms indicated that the adsorption of thiophene over the Raney Ni/Al2 O3 adsorbent complied with the Freundlich model.The results of adsorption kinetics studies showed that the pseudo-second-order kinetics equation was more advantageous than the pseudo-first-order kinetics equation in describing the adsorption kinetics of thiophene on Raney Ni/Al2 O3.The rate constant value(kp)was positively correlated with the temperature whereas the adsorption mass transfer process was mainly determined by the intraparticle and film diffusion.The adsorption thermodynamic analysis proved that△G^0<0,△H^0>0,and△S^0>0,implying that the adsorption was a spontaneous,entropy-increasing and endothermic process.展开更多
A new nanometer material, nano-Al2O3 with carbon fibre as the carrier, was employed for the removal of Cd with low concentrations from polluted water. The characterization of the material was carried out by means of S...A new nanometer material, nano-Al2O3 with carbon fibre as the carrier, was employed for the removal of Cd with low concentrations from polluted water. The characterization of the material was carried out by means of SEM and TEM. Batch adsorption and elution experiments were carried out to determine the adsorption properties of Cd on the new adsorbent. The classical Thomas model was applied to estimating the equilibrium coefficients of Cd adsorption and the saturated adsorption ability. The results show that the Thomas model is fit for describing the kinetic adsorption process, and the maximum adsorption capacity of the nanometer Al2O3/carbon is 69.29 mg/g. The resulting information also indicates that the desorption of Cd eluted with de-ionized water at a rate of 9.8 mL/min can be neglected. With the advantage of a high adsorption capacity for removing low concentration Cd, the Al2O3/carbon fibre possesses the potentiality to be an effective adsorbent for the removal of Cd from polluted water.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
The adsorption properties of atomic and molecular species on Ir4/MgO and Ir4/γ-Al2O3 have been systematically studied by means of planewave density functional theory（DFT）calculations using the periodic boundary con...The adsorption properties of atomic and molecular species on Ir4/MgO and Ir4/γ-Al2O3 have been systematically studied by means of planewave density functional theory（DFT）calculations using the periodic boundary conditions.The binding energies of these species were ordered as follows：H2O〈C2H4〈H〈OH〈S〈N〈O〈C.The adsorption energies of adatoms on Ir4/MgO were larger than those on Ir4/γ-Al2O3 except hydrogen atom,but were in reverse for the molecules calculated.In addition,the difference of adsorption energies on MgO and γ-Al2O3 supports has been elucidated by analyzing the electronic properties.A detailed investigation on state density clarifies the nature of the magnitude of adsorption energy.These calculated results are consistent well with the available experimental and theoretical results.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
基金supported by National Natural Science Foundation of China (No. 40743020 No. 40973078)Tianjin Natural Science Foundation (No. 08JCYBJC10400 and No. 06YFSZSF05100)
文摘This study describes the adsorption features of cadmium on Fe2O3 and MnO2 in alkaline saline conditions. The adsorption reached equilibrium in 6 hours under alkaline conditions. The absorption of cadmium on Fe2O3 and MnO2 was consistent with Freundlich absorption isotherms, and the corresponding adsorption capacities were 16.3 and 16.7 mg·g-1, respectively. Moreover, the adsorption quantity of cadmium on Fe2O3 and MnO2 rose with increas-ing pH from acidic to neutral, and reached the maximum at pH= 9. The coexisting chlorides reduced the adsorption capacity of Fe2O3 and MnO2. The influence intensities of different cations follow the order of CaCl2>>KCl>NaCl. However, the influence of sodium salts on the capacities of Fe2O3 and MnO2 to adsorb cadmium appeared more complicated: the relatively low concentrations of sodium salts could reduce the adsorption capacity; with increasing concentrations of sodium salts, e.g. NaCl and NaNO3. the adsorption capacity decreased continually. Moreover, due to the competition adsorption and precipitation effects, the adsorption capabilities of Na2CO3, NaH2PO4 and Na2HSO4 could also be reduced and cadmium concentrations in the solution were reduced as well.
文摘Mesoporous superacids S2O82–-Fe2O3/SBA-15(SFS)with active nanoparticles are prepared by ultrasonic adsorption method.This method is adopted to ensure a homo-dispersed nanoparticle active phase,large specific surface area and many acidic sites.Compared with bulk S2O82–-Fe2O3,Br?nsted acid catalysts and other reported catalysts,SFS with an Fe2O3 loading of 30%(SFS-30)exhibits an outstanding activity in the probe reaction of alcoholysis of styrene oxide by methanol with 100%yield.Moreover,SFS-30 also shows a more excellent catalytic performance than bulk S2O82–-Fe2O3 towards the alcoholysis of other ROHs(R=C2H5-C4H9).Lewis and Bronsted acid sites on the SFS-30 surfaces are confirmed by pyridine adsorbed infrared spectra.The highly efficient catalytic activity of SFS-30 may be attributed to the synergistic effect from the nano-effect of S2O82–-Fe2O3 nanoparticles and the mesostructure of SBA-15.Finally,SFS-30 shows a good catalytic reusability,providing an 84.1%yield after seven catalytic cycles.
基金financially supported by the National Natural Science Foundation of China(Nos.51661145025,51972039,and 51803018)
文摘High-purity(99%)carbon nanocoils(CNCs)have been synthesized by using porousα-Fe2O3/SnO2 catalyst.The yield of CNCs reaches 9,098%after a 6 h growth.This value is much higher than the previously reported data,indicating that this method is promising to synthesize high-purity CNCs on a large scale.It is considered that an appropriate proportion of Fe and Sn,proper particle size distribution,and a loose-porous aggregate structure of the catalyst are the key points to the high-purity growth of CNCs.Benefiting from the high-purity preparation,a CNC Buckypaper was successfully prepared and the electrical,mechanical,and electrochemical properties were investigated comprehensively.Furthermore,as one of the practical applications,the CNC Buckypaper was successfully utilized as an efficient adsorbent for the removal of methylene blue dye from wastewater with an adsorption efficiency of 90.9%.This study provides a facile and economical route for preparing high-purity CNCs,which is suitable for large-quantity production.Furthermore,the fabrication of macroscopic CNC Buckypaper provides promising alternative of adsorbent or other practical applications.
基金Project supported by the Foundation for Key Program of Ministry of Education (Nos.108033 and 107119)State Key Development Program for Basic Research of China (No.2009CB219801)+4 种基金the National High Technology Research and Development Program of China (No.2008AA05Z302)NNSFC (No.50976032)NSF of Beijing (No.3101001)the Specialized Basic Research Fund for Center Higher Education (No.09ZG03)Doctor Fund of North China Electric Power University (No.200822015)
文摘The adsorption of C atoms on the α-Fe2O3（001） surface was studied based on density function theory（DFT） ,in which the exchange-correlation potential was chosen as the PBE（Perdew,Burke and Ernzerhof） generalized gradient approximation（GGA） with a plane wave basis set. Upon the optimization on different adsorption sites with coverage of 1/20 and 1/5 ML,it was found that the adsorption of C atoms on the α-Fe2O3（001） surface was chemical adsorption. The coverage can affect the adsorption behavior greatly. Under low coverage,the most stable adsorption geometry lied on the bridged site with the adsorption energy of about 3.22 eV; however,under high coverage,it located at the top site with the energy change of 8.79 eV. Strong chemical reaction has occurred between the C and O atoms at this site. The density of states and population analysis showed that the s,p orbitals of C and p orbital of O give the most contribution to the adsorption bonding. During the adsorption process,O atom shares the electrons with C,and C can only affect the outermost and subsurface layers of α-Fe2O3; the third layer can not be affected obviously.
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The National Key Project for Basic Research of China(973 Project)(No.2005CB221402)China National Petroleum Corporation
文摘The activation of adsorbed CO is an important step in CO hydrogenation. The results from TPSR of pre-adsorbed CO with H2 and syngas suggested that the presence of H2 increased the amount of CO adsorption and accelerated CO dissociation. The H2 was adsorbed first, and activated to form H＊ over metal sites, then reacted with carbonaceous species. The oxygen species for CO2 formation in the presence of hydrogen was mostly OH^＊, which reacted with adsorbed CO subsequently via CO^＊＋OH^＊ → CO2^＊＋H^＊; however, the direct CO dissociation was not excluded in CO hydrogenation. The dissociation of C-O bond in the presence of H2 proceeded by a concerted mechanism, which assisted the Boudourd reaction of adsorbed CO on the surface via CO^＊＋2H^＊ → CH^＊＋OH^＊. The formation of the surface species （CH） from adsorbed CO proceeded as indicated with the participation of surface hydrogen, was favored in the initial step of the Fischer-Tropsch synthesis.
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Projects(50806025, 51021065, 50976038) supported by the National Natural Science Foundation of ChinaProject(20100480893) supported by the China Postdoctoral Science FoundationProject(1001022B) supported by the Postdoctoral Research Fund of Jiangsu Province, China
文摘The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al2O3 catalysts was explored in a fixed bed adsorption system. The catalysts maintain nearly 100% NO conversion efficiency at 350℃. Comprehensive tests were carried out to study the adsorption behavior of NH3 and NO over the catalysts. The desorption experiments prove that NH3 and NO are adsorbed on CuO/γ-Al2O3 catalysts. The adsorption behaviors of NH3 and NO were also studied with the in-situ diffusion reflectance infrared Fourier transform spectroscopy methods. The results show that NH3 could be strongly adsorbed on the catalysts, resulting in coordinated NH3 and NH4＋. NO adsorption leads to the formation of bridging bidentate nitrate, chelating bidentate nitrate, and chelating nitro. The interaction of NH3 and NO molecules with the Cu2＋ present on the CAl2O3 （100） surface was investigated by using a periodic density functional theory. The results show that the adsorption of all the molecules on the Cu2＋ site is energetically favorable, whereas NO bound is stronger than that of NH3 with the adsorption site, and key information about the structural and energetic properties was also addressed.
基金financially supported by the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions(CIT&TCD 20130325)the Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges under Beijing Municipality(IDHT20180508)。
文摘How to remove trace amount of sulfur in benzene is of significance,and deep desulfurization by Ni-containing absorbents is an efficient and promising method.In this paper,The Raney Ni/Al2 O3 adsorbent was prepared and its kinetic and thermodynamic characteristics on adsorptive desulfurization of benzene were studied.The results showed that Raney Ni/Al2 O3 adsorbent exhibited good adsorption performance.The equilibrium isotherms indicated that the adsorption of thiophene over the Raney Ni/Al2 O3 adsorbent complied with the Freundlich model.The results of adsorption kinetics studies showed that the pseudo-second-order kinetics equation was more advantageous than the pseudo-first-order kinetics equation in describing the adsorption kinetics of thiophene on Raney Ni/Al2 O3.The rate constant value(kp)was positively correlated with the temperature whereas the adsorption mass transfer process was mainly determined by the intraparticle and film diffusion.The adsorption thermodynamic analysis proved that△G^0<0,△H^0>0,and△S^0>0,implying that the adsorption was a spontaneous,entropy-increasing and endothermic process.
基金Supported by the Starting Foundation for Graduated Doctors in Jilin University(No.420010302353).
文摘A new nanometer material, nano-Al2O3 with carbon fibre as the carrier, was employed for the removal of Cd with low concentrations from polluted water. The characterization of the material was carried out by means of SEM and TEM. Batch adsorption and elution experiments were carried out to determine the adsorption properties of Cd on the new adsorbent. The classical Thomas model was applied to estimating the equilibrium coefficients of Cd adsorption and the saturated adsorption ability. The results show that the Thomas model is fit for describing the kinetic adsorption process, and the maximum adsorption capacity of the nanometer Al2O3/carbon is 69.29 mg/g. The resulting information also indicates that the desorption of Cd eluted with de-ionized water at a rate of 9.8 mL/min can be neglected. With the advantage of a high adsorption capacity for removing low concentration Cd, the Al2O3/carbon fibre possesses the potentiality to be an effective adsorbent for the removal of Cd from polluted water.
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The adsorption properties of atomic and molecular species on Ir4/MgO and Ir4/γ-Al2O3 have been systematically studied by means of planewave density functional theory（DFT）calculations using the periodic boundary conditions.The binding energies of these species were ordered as follows：H2O〈C2H4〈H〈OH〈S〈N〈O〈C.The adsorption energies of adatoms on Ir4/MgO were larger than those on Ir4/γ-Al2O3 except hydrogen atom,but were in reverse for the molecules calculated.In addition,the difference of adsorption energies on MgO and γ-Al2O3 supports has been elucidated by analyzing the electronic properties.A detailed investigation on state density clarifies the nature of the magnitude of adsorption energy.These calculated results are consistent well with the available experimental and theoretical results.
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.
