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1.
L. Hamon  L. Chenoy  G. De Weireld 《Adsorption》2014,20(2-3):397-408
The absolute adsorption isotherms are necessary to correctly evaluate the selectivity of the adsorbent material or to design adsorption processes at high pressure (e.g., H2 purification from syngas processes, removal of acid gas from natural gas,…). The aim of this work is thus to propose an easy method to correct the buoyancy effect of the bulk phase on the adsorbed phase volume during both pure gas and gas mixtures adsorption for pressures up to 10 MPa. The potential theory of adsorption and the Dubinin–Radushkevich relation are adapted by introducing mixing parameters based on simple Berthelot rules. The concept of internal pressure used to characterize the adsorbed phase is also adapted for mixtures. The method is then improved on a commercial activated carbon (AC), when adsorbing pure H2S and CH4, and their mixtures up to 5 MPa. The study points out the importance to carefully consider the buoyancy effect of the bulk phase on the adsorbed phase volume. Its impact on the adsorbent material selectivity at high pressures could affect the design and the performances of PSA or TSA processes. For example, only considering the excess adsorption data leads to an apparent selectivity 13 % greater than the absolute one for a concentration of 6 ppm of H2S in a CH4 matrix at 5 MPa (298 K) on the AC.  相似文献   

2.
The aim of this work was to investigate the aqueous mercury adsorption in a fixed bed of mesostructured silica SBA-15 functionalized with propylthiol by co-condensation (SBA-15-SH). Powdered synthesized adsorbents were used to prepare pellets with sizes ranging from 0.5 to 1 mm. The physicochemical properties determined from N2 adsorption and chemical analysis were compared for powder and pellets. Batch static experiments were carried out to obtain the equilibrium mercury adsorption isotherms, resulting that although the maximum adsorption capacity was reduced from powder to pellets, the materials maintained high efficiency for mercury removal even at very low aqueous metal concentration. Dynamic experiments were carried out in a fixed bed column by modifying the volumetric flow rate, bed length, inlet concentration, and amount of propylthiol groups incorporated to the adsorbent, and analyzing the temporal scale and the mercury adsorption capacities. The elution of the fixed bed was carried out chemically by circulating an aqueous 2 M hydrobromic acid stream for 2 h so achieving a complete recovery of the mercury previously adsorbed. Simplified dynamic equations of Bohart–Adams and Wolborska were used for modeling the breakthrough curves.  相似文献   

3.
A magnetic composite of silver/iron oxides/carbon nanotubes (Ag/Fe3O4/CNTs) was synthesized and used as an adsorbent for the preconcentration of mercury ions in water solutions at room temperature (25°C) in this study. The silver nanoparticles were supported on the magnetic CNTs. The modification enabled the composite had not only a high adsorption capacity for mercury ions (Hg2+) but also the magnetic isolation properties. A fast, sensitive, and simple method was successfully developed for the preconcentration and determination of trace amount of Hg2+ in water using the synthesized nanocomposite as adsorbent. The mercury concentration was determined by an atomic fluorescence spectrometer (AFS). The experimental conditions such as pH value, extraction temperature, extraction time, sample volume, eluent composition and concentration, sorbent amount, and coexisting ions were investigated for the optimization. A 500 mL of sample volume resulted in a preconcentration factor of 125. When a 200 mL of sample was employed, the limit of detection for Hg2+ was as low as 0.03 ng mL?1with relative standard deviation of 4.4% at 0.1 ng mL?1 (n = 7). The ease of synthesis and separation, the good adsorption capacity, and the satisfactory recovery will possibly make the composite an attractive adsorbent for the preconcentration of ultratrace Hg2+ in waters.  相似文献   

4.
Mixed Cu and Mg oxides on nitrogen-rich activated carbon (AC) from Nypha fruticans biomass were characterized and their CO2 adsorption performance was measured. Highly dispersed CuO and MgO nanoparticles on AC was obtained using an ultrasonic-assisted impregnation method. The optimum adsorbent is 5%CuO–25%MgO/AC having good surface properties of high surface area, pores volume and low particles agglomeration. The higher content of MgO of 5%CuO–25%MgO/AC adsorbent contributes to less metal carbide formation which increases their porosity, surface area and surface basicity. XPS analysis showed some amount of nitrogen content on the surface of the adsorbent which increased their surface basicity towards selective CO2 adsorption. The presence of moisture accelerated the CO2 chemisorption to form a hydroxyl layer on the surfaces. The 5%CuO–25%MgO/AC adsorbent successfully adsorbed CO2 via physisorption and chemisorption of 14.8 and 36.2 wt%, respectively. It was significantly higher than fresh AC with better selectivity to CO2.  相似文献   

5.
In this paper, Ce(IV)–Y, Cu(II)–Y and Cu(II)–Ce(IV)–Y adsorbents were prepared by the liquid-phase ion-exchange Y zeolites with combined Cu and Ce ions at low temperature and room pressure. The adsorbents were characterized by means of X-ray diffraction, N2-adsorption specific surface area measurements (BET), X-ray photoelectron spectroscopy, Pyridine adsorption infrared spectroscopy and Fourier transform infrared. The adsorptive desulfurization properties of these three adsorbents were studied in a fixed-bed unit through a model gasoline which made up of 1-octane solution of the refractory sulfur compounds (Such as thiophene and benzothiophene) and a certain amount of toluene or cyclohexene. The results indicate that Cu(II)–Ce(IV)–Y bind the organic sulfur compounds through two types of adsorption modes: π-complexation and direct sulfur–adsorbent interaction. The adsorption selectivity of sulfur compounds onto Cu(II)–Ce(IV)–Y decreased in the order: benzothiophene > 2,5-dimethylthiophene > 3-methylthiophene > thiophene. The effect of competition components on the metal ion-exchanged Y zeolites for sulfur removal in the order: cyclohexene > toluene. The Cu(II)–Ce(IV)–Y possesses the high sulfur adsorption capacity similar to Cu(II)–Y and high selectivity for sulfur compounds similar to Ce(IV)–Y, which can be attributed to the synergistic interaction between Cu2+ and Ce4+.  相似文献   

6.
A new solid-phase extraction method was developed for trace determination of Hg(II) by using a small amount of naked magnetite nanoparticles as an adsorbent. The magnetite nanoparticles were characterized by X-ray diffraction, scanning electron microscopy and transmission electron microscopy. The adsorbed Hg(II)-dithizone complex was eluted with 1.0 mL aliquot of an acidic 1-propanol solution prior to electrothermal atomic absorption spectrometry. A huge positive effect was found on the mercury adsorption by ionic strength. Under optimized condition, a linear calibration curve was obtained for mercury in the range of 0.2–50 ng mL?1 with relative standard deviation in the range of 0.5–2.0%. The limit of detection and enrichment factor were 0.01 ng mL?1 and 98.3, respectively. The effects of coexisting ions were studied extensively, and a new clean-up procedure was used to remove the matrix effects by using a simple sample pretreatment step using a little amount of magnetite nanoparticles. The method was successfully applied to the determination of Hg(II) in different water and human urine samples and a commercial sodium nitrate.  相似文献   

7.
The adsorption of mercury from a single/multi-solute aqueous solution by activated carbon (AC) prepared from cherry stones (CS) by chemical activation with H3PO4, ZnCl2 or KOH is studied. Three series of AC (i.e., P, H3PO4; Z, ZnCl2; K, KOH) were prepared by controlling the impregnation ratio and carbonization temperature. The textural characterization of AC was carried out by gas adsorption, mercury porosimetry and density measurements. The surface chemistry was analyzed by the pH of the point of zero charge (pHzpc), FT-IR spectroscopy and Boehm’s method. Experiments of mercury adsorption were conducted by the batch method, using aqueous solutions of mercury and of mercury, cadmium and zinc without pH adjustment. The ACs possess a wide range of pore volumes and sizes. Their microporosity is usually well developed. The meso- and macropore volumes are higher for the P carbons and K carbons, respectively. BET surface areas as a rule range between 1000 and 2000 m2?g?1. The pHzpc is much lower for the P carbons. The content of acidic oxygen surface groups is lower for the K carbons, whereas the content of basic groups is higher for these carbons. The kinetics of the adsorption process of mercury is faster for ACs with high volumes of large size pores. However, the surface groups have a marked unfavorable influence on the kinetics. The pseudo-second order rate constant (k2×10?3, g/mol?h) is higher by the order Z-4-800 (67.69)>K-3-800 (43.45)>P-3.44-400 (36.98). The incorporation of zinc and cadmium to the mercury solution usually decelerates the adsorption process for the P carbons and Z carbons and accelerates it for the K carbons. The amount adsorbed of mercury is much larger for the K carbons than for the other ACs. For the Z carbons, competition effects of zinc and cadmium on the adsorption of mercury are negligible, which indicates that mercury adsorbs specifically on surface active sites of these adsorbents.  相似文献   

8.
In this work, we compare the surface and morphometric properties of the pore networks in four silicas (code names Fr1428, Fr474, Fr1386, and MM1164) with different random porosities using the adsorption isotherms of two different probe adsorbents, nitrogen and methanol. The parent material Fr1428 was a pure silica 25 microm sample. The Fr474 sample was the same one with bonded electroneutral diol groups on its outer surface. Fr1386 was the parent material with bonded electroneutral diol groups on its outer surface and sulfonic groups on its inner surface, and the MM1164 sample was the original sample with external electroneutral diol groups and internal n-octadecyl groups. The properties examined were the specific surface area S(p) and the specific pore volume V(p), the pore connectivity c, the pore anisotropy b, the tortuosity tau, and the lacunarity lambda of the pore network as well as the percentage microporosity. These properties provide a complete characterization of complexity of the porous network. The surface areas of the solids were estimated via the traditional BET plots (S(BET)) and the I-point method (S(I)). The two sets of values S(BET) and S(I) were practically identical and they decrease as the size of the functional group increases. The values of percentage microporosity were also determined by the same I-point method using the variation of the C parameter of the BET equation. The total pore volume V(p) was found to be higher in the case of methanol adsorption, compared to nitrogen, which might be related to increase condensation. The networks of the pores were simulated using a dual site bond model (DSBM) and Monte Carlo (MC) techniques for achieving their proper arrangement into the solids. From the resulting simulating networks, the pore connectivity distributions (PCD) and their mean values c(mean) were estimated and favorably compared to the values of connectivity c(Seaton) determined according to the method of Seaton. Both values decrease with the size of the functional groups and are weakly affected by the adsorbent employed. From the simulation pore network, the mean values of tortuosity tau(mean) were also estimated and found to be lower when N2 was used as adsorbate compared to MeOH. The values of lacunarity lambda, estimated according to the method by Allain and Cloitre using the moving box technique in the DSBM/MC simulation matrix of the pore network, indicate that the distribution of the poreless mass into the matrix increases with the size of the functional group. Finally, the internal relationships observed between the pore anisotropy b and the percentage microporosity as well as between the tortuosity tau and the pore connectivity c are discussed.  相似文献   

9.
Carboxylated multi-walled carbon nanotubes (MWCNTs-COOH) were chemically modified with 3-aminopyrazole (MWCNTs-f) and applied as an efficient adsorbent to mercury and arsenic adsorption from aqueous solutions. The adsorbents were characterized by FT-IR, EDX, FE-SEM, TGA, and BET. The effects of pH, adsorbent dose, and initial ions concentration on the adsorption efficiency and the optimum conditions were investigated by central composite design. The optimum conditions were obtained at pH 7.6–7.9, adsorbent dose 20 mg, and initial ions concentration 20 ppm. So the maximum adsorption efficiencies in these conditions were 80.5 and 72.4% for the removal of Hg(II) and As(III) by MWCNTs-f, respectively. The quadratic model was used for the analysis of variance and indicated that adsorption of metal ions strongly depends on pH. Also, the pseudo-second-order model has been achieved from the adsorption kinetic studies. Furthermore, the experimental data were well fitted to the Langmuir isotherm and the maximum adsorption capacities obtained were 112 and 133 mg g?1 for the adsorption of Hg(II) and As(III) by MWCNTs-f, respectively. Moreover, a thermodynamic study revealed that the adsorption reactions were spontaneous and endothermic with the increase in randomness. In addition, a desorption study showed the favorable regeneration ability of MWCNTs-f even after three adsorption–desorption cycles. Therefore, the MWCNTs-f adsorbent has good potential for the removal of Hg(II) and As(III) pollutants from aqueous solutions.  相似文献   

10.
H2S is considered as the main gas pollutant from livestock farm and activated carbon (AC) is widely used as adsorbent for H2S. This paper focuses on the influence of modification conditions and operation conditions on the H2S adsorption performance on AC samples. The H2S adsorption performance on modified AC (MAC) samples by single and combinatory method has been investigated. It is concluded that the MAC by combinatory method of high-pressure hydrothermal method followed by alkaline solution impregnation method could promote the H2S adsorption performance remarkably. The H2S adsorption performance differs with different operation conditions. Meanwhile the samples of fresh AC and exhausted AC have been characterized using BET, FTIR, TPD and Boehm titration method. The experimental results are confirmed that the characteristics of AC have significant influence on the adsorption ability for H2S.  相似文献   

11.
Textural characterization of activated carbons prepared from palm shell by thermal activation with carbon dioxide (CO(2)) gas is reported in this paper. Palm shell (endocarp) is an abundant agricultural solid waste from palm-oil processing mills in many tropical countries such as Malaysia, Indonesia, and Thailand. The effects of activation temperature on the textural properties of the palm-shell activated carbons, namely specific surface area (BET method), porosity, and microporosity, were investigated. The activated carbons prepared from palm shell possessed well-developed porosity, predominantly microporosity, leading to potential applications in gas-phase adsorption for air pollution control. Static and dynamic adsorption tests for sulfur dioxide (SO(2)), a common gaseous pollutant, were carried out in a thermogravimetric analyzer and a packed column configuration respectively. The effects of adsorption temperature, adsorbate inlet concentration, and adsorbate superficial velocity on the adsorptive performance of the prepared activated carbons were studied. The palm-shell activated carbon was found to have substantial capability for the adsorption of SO(2), comparable to those of some commercial products and an adsorbent derived from another biomass.  相似文献   

12.
Pyrolytic tire char adsorbents either demineralized by nitric acid (purified char, PC) or activated with KOH-calcination (activated char, AC) were used for Cr(VI) removal from aquatic solutions and studied by adsorption kinetics, isotherms, and thermodynamics. Adsorbent’s physicochemical characteristics were studied by several techniques such as X-ray diffraction, porosimetry, scanning electron microscopy, elemental analysis, and Boehm titration. For PC, acid treatment leads partially to a mesoporous structure while for AC, KOH activation creates also a microporosity enhancing the specific surface area at 443 m2g?1. Cr(VI) adsorption onto both adsorbents followed better second-order kinetics and Langmuir isotherm models and it was exothermic (ΔH < 0) and spontaneous (ΔG < 0). The maximum Cr(VI) adsorption capacity for AC and PC was 114 and 79.47 mg g?1, respectively, at pH = 4. The present work reveals that AC and PC can be efficient sorbents for the removal of heavy metal ions, contributing both positively to wastewater treatment and waste tire pyrolysis plants.  相似文献   

13.
Three kinds of commercial silica gels with pore size of 2–3, 4–7 and 8–10 nm respectively are used for preparing composite adsorbents by soaking them into the aqueous solution of calcium chloride. The test result indicates that both the water uptake and adsorption rate of composite adsorbents prepared from 4–7 and 8–10 nm silica gels improve greatly compared to pure silica gels, but they do not for 2–3 nm silica gels. The silica gel with pore size of 2–3 nm is not suitable for preparing the composite adsorbent by impregnation method due to the pore blockage because of the small pore size. The SCP and COP of the adsorption chiller with sample SA50 are 128.3 Wkg?1 and 0.27 respectively at the hot source temperature of 90 °C, which are largely superior to that of SA0. Hence using the composite adsorbent instead of the pure silica gel can reduce the size of the adsorption chiller.  相似文献   

14.
Extraction, pre-concentration and determination of trace amounts of mercury ions from water samples were investigated by magnetic solid phase extraction (MSPE) method using Fe3O4 nanoparticles decorated with polythionine as an adsorbent. A simple chemical synthesis by catalytic reaction of thionine in the presence of FeCl3 and hydrogen peroxide was used for preparation of the magnetic sorbent. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, vibrating sample magnetometer analysis and Fourier transform infrared spectroscopy were used to characterise the adsorbent. Mercury ions were determined by cold vapour atomic absorption spectrometry. The parameters for MSPE procedure, such as pH of the extraction solution, adsorption time, weight adsorbent, elution conditions (type, concentration and volume of the eluent), volume of the sample solution and effects of coexisting ions were investigated. The obtained optimal conditions were: sample pH of 4; sorbent amount of 4 mg; sorption time of 20 min; elution solvent of HNO3 (0.3 mol L?1)/thiourea (2% w/v) with volume of 2 mL, and breakthrough volume of 400 mL. A good linearity in the concentration range of 0.025–40 µg L?1 (R2 > 0.999) with the pre-concentration factor of 198 was obtained. The limits of detection and quantification were achieved as 0.008 and 0.025 µg L?1, respectively. Furthermore, sea and river water samples were analysed and good recoveries (97.1–99.6%) were obtained.  相似文献   

15.
Activated carbon (AC) supported CuCl (CuCl/AC) for ethylene/ethane separation has been prepared with CuCl2 as precursor by a solid-state dispersion method. The samples are characterized by inductively coupled plasma optical emission spectrometry, X-ray diffraction, N2 adsorption/desorption and X-ray photoelectron spectroscopy, and investigated for ethylene (C2H4) and ethane (C2H6) adsorptions. The characterization results reveal that CuCl2 supported on AC can be highly dispersed on the surfaces of AC support and completely converted to CuCl after activation at 543 K in N2. The resultant adsorbent displays high ethylene adsorption capacity, high C2H4/C2H6 adsorption selectivity and excellent reversibility. The adsorption isotherms of ethylene and ethane on CuCl/AC at temperatures up to 333 K can be well fitted by the Sips models, and the corresponding isosteric heats of adsorption are calculated from the Clausius–Clapeyron equation. The value of isosteric heat of adsorption suggests that the interaction of ethylene with CuCl/AC is between physisorption and chemisorption.  相似文献   

16.
Four nanoporous carbons obtained from different polymers: polypyrrole, polyvinylidene fluoride, sulfonated styrene–divinylbenzene resin, and phenol–formaldehyde resin, were investigated as potential adsorbents for carbon dioxide. CO2 adsorption isotherms measured at eight temperatures between 0 and 60 °C were used to study adsorption properties of these polymer-derived carbons, especially CO2 uptakes at ambient pressure and different temperatures, working capacity, and isosteric heat of adsorption. The specific surface areas and the volumes of micropores and ultramicropores estimated for these materials by using the density functional theory-based software for pore size analysis ranged from 840 to 1990 m2 g?1, from 0.22 to 1.47 cm3 g?1, and from 0.18 to 0.64 cm3 g?1, respectively. The observed differences in the nanoporosity of these carbons had a pronounced effect on the CO2 adsorption properties. The highest CO2 uptakes, 6.92 mmol g?1 (0 °C, 1 atm) and 1.89 mmol g?1 (60 °C, 1 atm), were obtained for the polypyrrole-derived activated carbon prepared through a single carbonization-KOH activation step. The working capacity for this adsorbent was estimated to be 3.70 mmol g?1. Depending on the adsorbent, the CO2 isosteric heats of adsorption varied from 32.9 to 16.3 kJ mol?1 in 0–2.5 mmol g?1 range. Overall, the carbons studied showed well-developed microporosity and exceptional CO2 adsorption, which make them viable candidates for CO2 capture, and for other adsorption and environmental-related applications.  相似文献   

17.
The present work deals with uranium removal from a nitric acid raffinate (waste) solution using prepared solvent (tri-butyl phosphate, TBP) immobilizing PVC cement (SIC) as a suitable adsorbent. The studied relevant factors affecting uranium adsorption onto SIC adsorbent involved; contact time, solution molarity, initial uranium concentration and temperature. The obtained adsorption isotherm of uranium onto the SIC adsorbent was fitted to Langmuir, Freundlich and Dubinin–Radushkviech (D–R) adsorption models. The results showed that the obtained equilibrium data fitted well the Langmuir isotherm. Additionally, it was found that the adsorption process obeys the pseudo second-order kinetic model. On the other hand, the calculated theoretical capacity of our prepared SIC adsorbent reached about 17 g U/kg SIC. Uranium adsorption from the studied raffinate solution was carried out applying the attained optimum conditions. The obtained data showed that 58.4 mg U/5 g SIC were adsorbed. However, using of 2 M HNO3 solution as an eluent, 93 (54.3 mg U) from the adsorbed amount were eluted.  相似文献   

18.
《Comptes Rendus Chimie》2014,17(12):1203-1211
A thiol-functionalized hierarchical zeolite nanocomposite was synthesized and investigated with a view to remove mercury from aqueous solutions. The hierarchical zeolite was prepared by the use of a beta zeolite and of cetyltrimethylammoniumbromide (CTAB). The ligand, 3-mercaptopropyltrimethoxysilane containing thiol (–SH) groups, was then immobilized on the surface of the hierarchical zeolite through grafting with surface silanol groups. FTIR, XRD, SEM, TG-DTG, and N2 adsorption–desorption techniques were used to characterize the nanocomposite before and after functionalization. Adsorption experiments showed that this adsorbent was an excellent one to bind mercury with high selectivity; an adsorption capacity of 8.2 mequiv·g−1 of adsorbent was obtained. Furthermore, the adsorbent retained most of its capacity after regeneration with nitric acid and thiourea solutions. The adsorption data was fitted to the Freundlich isotherm.  相似文献   

19.
杂原子Y分子筛的二次合成及其吸附脱硫性能(Ⅱ)   总被引:1,自引:1,他引:0  
Breck等[1]发表了用NH4SiF6溶液对分子筛进行脱铝补硅的二次合成方法,提高了骨架的硅铝比,从而改变了分子筛的热稳定性、酸性以及催化活性.作为该方法的扩展,已有将Ti、Te、Cr、Zr、Ga等元素引入分子筛骨架的报道[2~4].目前,已经有杂原子分子筛应用到工业生产中,但采用杂原子分子筛吸附脱硫的报道还较少.前文[5]采用液-固相同晶取代反应制备了骨架含Ga的Y型分子筛,并对其吸附脱硫性能进行了初步研究.本研究进一步对[Ga]AlY的吸附脱硫机理、再生性能等方面进行了深入研究.……  相似文献   

20.
In this paper, cheap liquorice residue was used to prepare activated carbon (AC), thioacetamide (TAA) was used to modify the AC, and the adsorption experiments were conducted in the simulated acid radioactive wastewater with low uranium concentration to study the adsorption behavior and mechanism for uranium by TAA modified AC (TAA–AC). The removal efficiency by TAA–AC was 92.1–98.2% from the 1 mg L?1 uranium solution at pH 2–6. The adsorption equilibrium data were well fitted by Dubinin–Radushkevich model, and the maximum adsorption capacity was estimated to be 340 mg g?1. TAA–AC showed an enhanced selectivity for uranium in the presence of competitive ions. Furthermore, the adsorption experiments were conducted in the actual acid radioactive wastewater with low uranium concentration from an in situ leach uranium mine. The high adsorption rate (98.3%) and selectivity (Kd?=?3.78×104 mL g?1) for uranium were observed in the actual acid radioactive wastewater, and the adsorption rate was found to maintain 96.2% over six cycles of adsorption–desorption.  相似文献   

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