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1.
《分离科学与技术》2012,47(8):1208-1214
The FeCl3-containing Lewis-acidic ionic liquids (ILs) [C6mim]Cl/FeCl3(1:1.5), [C6mim]Cl/FeCl3(1:2), [C8mim]Cl/FeCl3(1:1.5), and [C8mim]Cl/FeCl3(1:2) were used as extractants for desulfurization of model fuel and gasoline fuel, respectively. The results demonstrate that these ILs are effective for the removal of sulfur compounds from model fuel under different mass ratio of IL to model fuel (1:1, 1:3, 1:5, 1:10) at 25°C. The extractive performance of ILs increased as the molar ratio of FeCl3 to [Cnmim]Cl(n = 6, 8) varied from 1:1 to 1:2. The selectivity of sulfur compounds by extraction process followed the order of dibenzothiophene (DBT)>benzothiophene (BT) > 4,6-dimethyldibenzothiophene (4,6-DMDBT). The sulfur removal of gasoline fuel containing sulfur content of 440.3 ppmw could be up to 85.8%; that is to say that the sulfur content of gasoline fuel varied from 440.3 ppmw to 62.4 ppmw after one extraction stage. Moreover, the [C6mim]Cl/FeCl3(1:2) can be recycled for at least 4 times with a little decrease in the desulfurization activity.  相似文献   

2.
Acidic ionic liquids (ILs) have been employed as extractant and catalyst in the oxidative desulfurization (ODS) process of fuels in recent years. Several Lewis acidic ionic liquids [C63MPy]Cl/nFeCl3 (molar fraction n = 0.5, 1, 2, 3) and [C6MIM]Cl/FeCl3 were prepared and used to remove the aromatic sulfur compounds dibenzothiophene and benzothiophene from fuels. In the ODS process, the used ILs acted as both extractant and catalyst with 30 wt % hydrogen peroxide aqueous solution as oxidant. The effects of Lewis acidity of ILs, IL's cation structure, molar ratio of O/S, reaction temperature, and different sulfur compounds on the sulfur removal of model oil were investigated. The results indicated that the sulfur removal for dibenzothiophene was affected by Lewis acidity of ILs and nearly reached 100 % by [C63MPy]Cl/FeCl3 at conditions of 298 K, IL/oil mass ratio of 1/3, O/S molar ratio of 4/1, in 20 min. The sulfur removal of real gasoline reached 99.7 % after seven ODS runs in the [C63MPy]Cl/FeCl3‐H2O2 system.  相似文献   

3.
《分离科学与技术》2012,47(9-10):2406-2433
Abstract

A composite polymer (made of gelatin and alginate) was used for the synthesis of Cyphos IL 101-immobilized resins. These resins (with varying size and different ionic liquid (IL) content) have been tested for the recovery of mercury from concentrated HCl solutions (0.1–5 M HCl concentrations). Prior to the study of sorption performance on resins, the reactivity of Cyphos IL 101 versus mercury was tested using solvent extraction methodology. These results showed that the extraction was hardly affected by the concentration of HCl and that an ion exchange mechanism was probably involved in metal recovery (binding of HgCl4 2-). The performance of these resins for Hg(II) recovery was tested through sorption isotherms and uptake kinetics, investigating the effect of resin size, ionic liquid content, metal concentration, agitation speed, and resin state (dry state versus wet state). Sorption capacity (which was proportional to the IL content) can reached up to 150 mg Hg g?1 in 1 M HCl; this sorption capacity was decreased by increasing chloride concentration. The kinetics were described well by the pseudo-second order equation and by the intraparticle diffusion equation (the so-called Crank's equation). The intraparticle diffusion coefficient was in the range of 10?11–1.2 × 10?10 m2 min?1. The kinetic profiles were controlled by the IL content, sorbent dosage, and the sorbent particle size. Drying of the resins significantly decreased diffusion rates in the resins. The presence of competitor metals did not affect sorption capacity except when stable chloro-anionic species such as in the case of Zn(II) were formed. Mercury can be desorbed using 6 M nitric acid solutions; and the sorbent can be recycled for at least six sorption/desorption cycles without significant decrease in the sorption performance.  相似文献   

4.
《分离科学与技术》2012,47(13):2028-2035
A composite magnetic sorbent with a relatively high content of humic substances (above 35% of organic carbon) was prepared by co-precipitation of Fe2+/Fe3+ salts with commercially available alkaline humate concentrate. Magnetite (Fe3O4) was identified as the main crystalline phase bearing the magnetic properties of the sorbent. Scanning electron microscope (SEM) images revealed the presence of uniform sub-micron structures on the surface of the sorbent grains. Due to the presence of humic substances, the sorbent exhibited good sorption ability towards low-polarity organic pollutants, namely chlorophenols. The sorption efficiency increased in the order of 4-mono- < 2,4-di- < 2,4,5-trichlorophenol in accordance with growing hydrophobicity of these compounds, confirming a hydrophobic nature of the interactions involved in the sorption process. Similar trends were found in the desorption study utilizing water and methanol as leachants. Some polycyclic aromatic hydrocarbons (naphthalene, anthracene, phenanthrene, fluoranthene, pyrene) were also retained on the sorbent. The chemical composition as well as the main physical characteristics (surface area, phase composition) of the sorbent remained virtually unchanged during the sorption process. The sorbent retained its magnetic properties during the sorption of organic substances from aqueous solutions, which provides an opportunity for its regeneration.  相似文献   

5.
In this research, novel nanoparticles of Kit-6 mesoporous silica magnetite were synthesized with 9.6 nm pore diameter and 241.68 m2 g?1 surface area. The synthesized mesoporous magnetite nanoparticles (MMNPs) were functionalized with amine groups. Scanning electron microscopy, powder X-ray diffraction, Fourier transform infrared spectroscopy and nitrogen adsorption–desorption method confirmed the morphology and structure of the synthesized nanoparticles. The amine functionalized MMNPs were used for sorption of toxic chromate ions from aqueous samples. The effect of various experimental parameters (four factors at three levels) on the sorption efficiency of Cr(VI) was studied and optimized via Taguchi L9 (34) orthogonal array experimental design. At optimum conditions, the sorption of the Cr(VI) was best described by a pseudo second-order kinetic model with R2 = 0.9999 and qeq = 129.8 mg g?1, suggesting chemisorption mechanism. Adsorption data were fitted well to the Langmuir isotherm and the synthesized sorbent showed complete ion removal with 185.2 mg g?1sorption capacity.  相似文献   

6.
《分离科学与技术》2012,47(6):1215-1230
Abstract

The potential to remove copper (II) ions from aqueous solutions using Na‐mordenite, a common zeolite mineral, was thoroughly investigated. The effects of relevant parameters solution pH, adsorbent dose, ionic strength, and temperature on copper (II) adsorption capacity were examined. The sorption data followed the Langmuir, Freundlich, and Dubinin‐Radushkevich (D‐R) isotherms. The maximum sorption capacity was found to be 10.69 mg/g at pH 6, initial concentration of 40 mg/dm3, and temperature of 40°C. Different thermodynamic parameters viz., changes in standard free energy (ΔG0), enthalpy (ΔH0), and entropy (ΔS0) have also been evaluated and the results show that the sorption process was spontaneous and endothermic in nature. The dynamics of the sorption process were studied and the values of rate constant of adsorption, rate constant of intraparticle diffusion were calculated. The activation energy (Ea) was found to be 11.25 kJ/mol in the present study, indicating a chemical sorption process involving weak interactions between sorbent and sorbate. The interaction between copper (II) ions and Na‐mordenite is mainly attributable to ion exchange. The sorption capacity increased with the increase of solution pH and the decrease of ionic strength and adsorbent dose. The Na‐mordenite can be used to separate copper (II) ions from aqueous solutions.  相似文献   

7.
Tetraalkyl phosphonium chloride (Cyphos IL‐101), an ionic liquid (IL), was tested for gold recovery from HCl solutions: first in liquid/liquid extraction systems (using toluene and hexane as solvent) and in a second step, after being immobilized in a biopolymer composite matrix. SEM‐EDAX analysis was used for the characterization of the resins. The sorption capacity reached up to 140 mg Au(III) g?1 in 1 M HCl solutions. Base metals that do not form anionic chlorocomplexes and nitrate or chloride ions (at 5 g L?1) did not interfere with Au(III) binding. Gold binding probably occurs through the interaction of R3R'P+ with AuCl4 ?. The kinetics of sorption was carried out varying agitation speed, metal concentration, IL content, and resin drying. Intraparticle diffusion played an important role on the control of sorption kinetics. Gold could be desorbed from the loaded IL‐impregnated resin using thiourea (in HCl solutions). The resin could be re‐used for at least 4 cycles. The resins are specially adapted for the recovery of gold from low metal concentrations.  相似文献   

8.
Three novel magnetic adsorbents were synthesized through the immobilization of di-, tri-, and tetraamine onto the surface of silica coated magnetite nanoparticles. The adsorbents were characterized by XRD patterns, FTIR spectroscopy, elemental and thermogravimetric analysis, magnetic measurements, SEM/TEM, EDX spectroscopy, and N2 adsorption/desorption isotherms. Their capacity to remove copper ions from aqueous solutions was investigated and discussed comparatively. The equilibrium data were analyzed using Langmuir and Freundlich isotherms. The kinetics was evaluated using the pseudo-first-order, pseudo-second-order, and intra-particle diffusion models. The best interpretation for the equilibrium data was given by the Langmuir isotherm for the tri- and tetraamine functionalized adsorbents, while for the diamine functionalized adsorbent the Freundlich model seemed to be better. The kinetic data were well fitted to the pseudo-second-order model. The overall rate of adsorption was significantly influenced by external mass transfer and intraparticle diffusion. It was observed that the adsorption capacity at room temperature decreased as the length of polyamine chain immobilized on the adsorbent surface increased, the maximum adsorption capacities being 52.3 mg g?1 for 1,3-diaminopropan functionalized adsorbent, 44.2 mg g?1 for diethylenetriamine functionalized adsorbent, and 39.2 mg g?1 for triethylenetetramine functionalized adsorbent. The sorption process proved to be highly dependent of pH. The results of the present work recommend these materials as potential candidates for copper removal from aqueous solutions.  相似文献   

9.
《分离科学与技术》2012,47(6):931-940
A method is described for the selective separation and extraction of cadmium-lead from aqueous solutions by tuning the pH value between 1.0 and 7.0. A modified nano-active silica sorbent was loaded with 1-butyl-3-methyl-imidazolium bis(trifluoromethylsulfonyl)imide hydrophobic ionic liquid, [Bmim+Tf2N?] and used in this work. The pH value was found to play a significant role in the sorption capacity of Cd(II) and Pb(II). In pH 1.0, the metal capacity values were characterized as 1.40 and 0.30 mmol g?1 for Cd(II) and Pb(II), respectively. In pH 7.0, Cd(II) and Pb(II) switched their capacity values to 0.65 and 1.00 mmol g?1, respectively. An anion exchange mechanism was proposed in solution with pH 1.0 for exchange of chloroanionic cadmium species by [Tf2N?]. The sorptive separation processes of Cd(II) and Pb(II) were studied and evaluated under the influence of various controlling factors. The potential applications of modified nano-silica sorbent for selective sorptive removal and separation of Cd(II) from Pb(II) in water samples was successfully accomplished by adjusting the pH value of the contact solution between 1.0 and 7.0. The results of this study indicated an efficient extraction behavior of the two examined metal ions.  相似文献   

10.
ABSTRACT

A new eco-friendly bucky gel nano sorbent consisting of magnetic grapheneoxide (MGO) and an ionic liquid (IL) was used based on dispersive extraction technique followed by cold vapor atomic absorption spectroscopy for determination of mercury in river water, milk, omega-3 supplements, and lipstick. The optimum conditions for extraction were 50 mg of sorbent (mass ratio IL/MGO: 26), 8 min vortexing, acetate buffer pH = 4, and for desorption 3 min vortexing of HNO3 (1 mL). The limits of detection, quantification, preconcentration factor and extraction recovery were found at 0.57, 1.88 µg L?1, 21 and 84%. Relative standard deviation (RSD) was 6.5% (n = 3).  相似文献   

11.
The magnetic behavior of a binary salt of tricaprylylmethylammonium tetrachloroferrate and tricaprylylmethylammonium chloride, [A336][FeCl4]0.73[Cl]0.27, was evaluated. With a magnetic susceptibility of 0.011 emu mol? 1 this binary salt exhibited a remarkable response to an external magnetic field. Dynamic light scattering (DLS) measurements allowed to study the aggregation behavior of [A336][FeCl4]0.73[Cl]0.27 as well as of further magnetic ionic liquids [PR6,6,6,14][FeCl4] and (BMIM)[FeCl4] in ethylacetate and ethanol.  相似文献   

12.
《分离科学与技术》2012,47(16):2406-2412
A new sulfonamide containing polymeric sorbent for the removal of mercury ions from waste waters was prepared starting from poly(glycidyl methacrylate)-b-poly(ethylene glycol)-b-poly(glycidyl methacrylate) (PGMA- b -PEG- b -PGMA) triblock copolymer prepared by using the ATRP method. Epoxy groups on the block copolymer were functionalized with amino groups. Ammonia-functionalized PGMA- b -PEG- b -PGMA was treated with excess of benzenesulfonyl chloride to obtain a sulfonamide-based polymeric sorbent. The sulfonamide containing the polymeric sorbent with a 3.5 mmol · g?1 total nitrogen content is able to selectively sorb mercury from aqueous solutions. The mercury sorption capacity of the resin is around 3.12 mmol g?1 under non-buffered conditions. Experiments performed in identical conditions with several metal ions revealed that Cd(II), Pb(II), Zn(II), Fe(III), and Fe(II) also were extractable in quantities (0–0.45 mmol/g). The sorbed mercury can be eluted by repeated treatment with 4 M HNO3 without hydrolysis of the sulfonamide groups.  相似文献   

13.
Magnetic ionic liquids (MIL) are extensively used in extraction and catalytic processes. Here, a series of MIL, i.e., 1‐n‐butyric acid‐3‐methylimidazolium chloride/xFeCl3 ([C3H6COOHmim]Cl/xFeCl3; x = 0.5, 1, 1.5, 2), were synthesized and characterized by infrared spectroscopy, visible absorption spectrometry, and electrospray ionization mass spectrometry. The MIL [C3H6COOHmim]Cl/2FeCl3 was found to be highly active for the extraction and catalytic oxidative desulfurization of a model oil under mild conditions. Of note, the removal of benzothiophene, which has been regarded as a refractory aromatic sulfur compound, could be achieved at up to 100 % in 10 min. After reaction, the MIL could be easily separated from the model oil by applying an external magnetic field, due to its paramagnetic properties.  相似文献   

14.
The aim of this research was to prepare magnesium ferrite (MgFe2O4) magnetic nanoparticles and to investigate their sorption characteristics towards Mn2+, Co2+, Ni2+, Cu2+ ions in aqueous solution. MgFe2O4 was synthesized by glycine-nitrate combustion method and was characterized by low crystallinity with crystallite size of 8.2?nm, particle aggregates of 13–25?nm, BET surface area of 14?m2/g and pore size of 8.0?nm. Sorption properties of MgFe2O4 towards Mn2+, Co2+, Ni2+, Cu2+ ions were studied using one-component model solutions and found to be dependent on metal ions concentration, contact time, pH and conditions of regeneration experiment. The highest sorption capacity of MgFe2O4 was detected towards Co2+ (2.30?mmol?g1) and Mn2+ (1.56?mmol?g?1) and the lowest towards Ni2+ (0.89?mmol?g?1) and Cu2+ (0.46?mmol?g?1). It was observed that sorption equilibrium occurs very quickly within 20–60?min. The pHzpc of sorbent was calculated to be 6.58. At studied pH interval (3.0–7.0) the sorption capacity of MgFe2O4 was not significantly affected. Regeneration study showed that the metal loaded sorbent could be regenerated by aqueous solution of 10?3 M MgCl2 at pH 6.0 within 120?min of contact time. Regeneration test suggested that MgFe2O4 magnetic sorbent can be efficiently used at least for four adsorption-desorption cycles. The high sorption properties and kinetics of toxic metal ion sorption indicates good prospects of developed sorbent in practice for wastewater treatment.  相似文献   

15.
Equimolar mixture of pyridine-2,6-dimethanol (PDM), and thiocyanate ion immobilized on silica serves as an efficient sorbent for selective retention of Cu(II) from other associated metal ions at µg g?1 level. The maximum sorption capacity for Cu(II) was found as 2.44 mmol g?1 at pH 6.0. The sorbed Cu(II) was completely eluted with 3 mol L?1 HNO3 and measured with a flame atomic absorption spectrometer (FAAS). The structure of the extracted Cu(II) complex was confirmed by single-crystal X-ray structure analysis and Fourier transform-infrared (FT-IR) spectroscopy. Thermogravimetric analysis (TGA) of the isolated Cu(II) complex was performed to determine its thermal stability at the extraction temperature. The three sigma detection limit (N = 15) of the method is 0.6 µ g mL?1 with a relative standard deviation (RSD) of 0.1% (N = 15). Pre-concentration factor of the method is 133. Slight interference from Mn2+ ion was eliminated by prior oxidation with potassium periodate. The developed method was tested for trace level separation and estimation of Cu(II) in certified reference materials and environmental samples.

[Supplementary materials are available for this article. Go to the publisher's online edition of Chemical Engineering Communications for the following free supplemental resources: two tables providing details of the bond lengths and bond angles of the Cu(II) complex.]  相似文献   

16.
《分离科学与技术》2012,47(13):1880-1885
The commercial NaY zeolite with the Si/Al ratio of 5:1 was selected and modified for researching the adsorptive removal of thiophene from benzene. The zeolite was ion-exchanged in Ce(NO3)3 solution and then calcined in muffle to prepare the CeY sorbent. The results show that it is a suitable method to prepare the sorbent removing thiophene from benzene that NaY zeolite is ion-exchanged by cerium in Ce(NO3)3 solution. The desulfurization efficiency of CeY sorbent increases obviously comparing with NaY zeolite. The effects of the calcination temperature, calcination time, concentration of Ce(NO3)3 solution, ion-exchange time, and ion-exchange times on the desulfurization capacity of CeY sorbent were also studied. The results show that the optimal CeY sorbent can be obtained when NaY zeolite is ion-exchanged in 0.5 mol/L Ce(NO3)3 solution at 100°C for 4 h, calcined at 700°C for 2 h, and repeated the above steps two times. The results of XRD and BET characterization indicate that those preparation conditions mainly influence on the crystallinity, specific surface area of CeY sorbent. The best CeY sorbent can remove thiophene to 136.8 mg/L from 550.0 mg/L in thiophene-benzene solution at ambient temperature and pressure with the agent-liquid ratio of 1:16 (g/mL).  相似文献   

17.
Recovery of 1-butyl-3-methylimidazolium tetrachloroferrate ([bmim]FeCl4) from its mixture with water was investigated. The [bmim]FeCl4 rich phase in the mixture forming two-phase was successfully separated, while homogeneous mixtures could not be separated. However, the concentration of the homogeneous mixture varied as a function of the magnetic field strength. Therefore, a combination of magnetic field and conventional methods to recover magnetic ILs from reaction mixtures will be very useful and have great potential.  相似文献   

18.
Here, molybdenum sulfide (MoS2) was characterized and its performance as an adsorbent for Co(II)/Ni(II) removal from water was estimated in batch experiments. The nanomaterial exhibits thin-layered structure and contains numerous hydroxyl groups. High pH enhanced Co(II)/Ni(II) sorption, while ionic strength had no effect. The chemical sorption between the binding sites of MoS2 and Co(II)/Ni(II) limited the rate. The Freundlich isotherm correlated better than Langmuir isotherm. The maximum sorption capacity for Co(II)/Ni(II) was 370.10/375.94 mg· g?1, obviously exceeding other adsorbents. Both adsorptions were endothermic and spontaneous processes. This study indicates the intrinsic value of MoS2 in removing heavy metals from water.  相似文献   

19.
《分离科学与技术》2012,47(4):923-943
Abstract

The sorption behavior of 2.7×10?5 M solution of Th(IV) ions on 1‐(2‐pyridylazo)‐2‐naphthol (PAN) loaded polyurethane foam (PUF) has been investigated. The quantitative sorption was occurred from pH 6 to 9 from acetate buffer solutions. The sorption conditions were optimized with respect to pH, shaking time, and weight of sorbent. The sorption data followed the Freundlich, Langmuir, and Dubinin‐Radushkevich (D‐R) isotherms very successfully at low metal ions concentration. The Freundlich isotherm constant (1/n) is estimated to be 0.22±0.01, and reflects the surface heterogeneity of the sorbent. The Langmuir isotherm gives the maximum monolayer coverage is to be 8.61×10?6 mol g?1. The sorption free energy of the D‐R isotherm was 17.85±0.33 kJ mol?1, suggesting chemisorption involving chemical bonding was responsible for the adsorption process. The numerical values of thermodynamic parameters such as enthalpy (ΔH), entropy (ΔS), and Gibbs free energy (ΔG) indicate that sorption is endothermic, entropy driven, and spontaneous in nature. The adsorption free energy (ΔGads) and effective free energy (ΔGeff) are also evaluated and discussed. The effect of different anions on the sorption of Th(IV) ions onto PAN loaded PUF was studied. The possible sorption mechanism on the basis of experimental finding was discussed. A new separation procedure of Th(IV) from synthetic rare earth mixture using batch, column chromatography, and squeezing techniques were reported.  相似文献   

20.
This article highlights a newly synthesized 5,11,17,23-tetra-tert.butyl-25,26,27,28-tetrakis(hydrazidecarbonylmethoxy)-calix[4]arene (3) impregnated resin 4 and it's sorption ability for the removal of selected oxoanions, i.e., (arsenate and dichromate) from aqueous environment. Resin 4 was characterized by using FT-IR spectroscopy, scanning electron microscope (SEM), elemental, and thermogravimetic (TGA) analyses techniques. Sorption study was carried out through static and dynamic methods with continuous flow operation to evaluate the potency of resin 4 under various conditions. Several parameters, such as effect of sorbent dosage, contact time, pH, and initial concentration were optimized through batch experiments. Results justify that % sorption of these oxoanions is highly dependent on pH of the solution. Equilibrium was achieved in 45 min, while sorption efficiency of resin 4 can be better explained by Langmuir and Temkin isotherm models. Furthermore, kinetically both oxoanions follow pseudo second order model. Additionally, sorption of arsenate more appropriately could be explained by Moris-Weber diffusion kinetic model. For the dynamic method, Thomas model was used to calculate the kinetic coefficient (kTH) and maximum sorption capacity (qo) of resin 4 which are 3.84 and 5.94 ml mg?1 min?1 and 0.185, 0.160 mg g?1 for As (V) and Cr (VI) respectively. Furthermore, resin 4 has been found as potential sorbent for removal of these oxoanions from contaminated surface water samples.  相似文献   

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