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1.
The sorption of Eu(III) on calcareous soil as a function of pH, humic acid (HA), temperature and foreign ions was investigated under ambient conditions. Eu(III) sorption on soil was strongly pH dependent in the observed pH range. The effect of ionic strength was significant at pH < 7, and not obvious at pH > 8. The type of salt cation used had no visible influence on Eu(III) uptake on soil, however at low pH values, the influence of anions was following the order: Cl ≈ NO3  > ClO4 . In the presence of HA, the sorption edge obviously shifted about two pH units to the lower pH, whilst in range of pH 6–7, the sorption of Eu(III) decreased with increasing pH because a considerable amount of Eu(III) was present as humate complexes in aqueous phase, then increased again at pH > 11. The results indicated that the sorption of Eu(III) on soil mainly formed outer-sphere complexes and/or ion exchange below pH ~7; whereas inner-sphere complexes and precipitation of Eu(OH)3(s) may play main role above pH ~8.  相似文献   

2.
A new chelating resin is prepared by coupling Amberlite XAD-4 with metaphenylendiamine through an azo spacer, characterized (elemental analysis, IR and thermogravimetric analysis (TGA)) and studied for preconcentration Rh (III) using Inductive Couple Plasma Atomic Emission Spectroscopy (ICP-AES) for rhodium monitoring. The optimum pH value for sorption of the metal ion was 6.5 (recovery 100%). The sorption capacity was found 0.256 mmol g− 1 of resin for Rh (III). The method has a detection limit and limit of quantification of 0.05 and 0.08 μg mL− 1 at pH 6.5, respectively. The chelating resin can be reused for 10 cycles of sorption-desorption without any significant change in sorption capacity. A recovery of 100% was obtained for the metal ion with 1.5 M HCl as eluting agent. The equilibrium adsorption data of Rh (III) on modified resin were analyzed by Langmuir and Freundlich models. Adsorption data were modeled using the pseudo-first-order, pseudo-second-order and intra-particle diffusion kinetics equations. Isotherms have also been used to obtain the thermodynamic parameters such as free energy, enthalpy and entropy of adsorption. The positive value of the enthalpy change (2.48 kJ/mol) indicates that the adsorption is an endothermic process. The method was applied for rhodium ions determination from tap water sample.  相似文献   

3.
A new aminophosphonic acid chelating resin was successfully prepared via electron beam irradiation grafting combined with chemical modification and used for the efficient removal of La(III). Firstly, glycidyl methacrylate (GMA) was grafted to polystyrene microspheres (PS) via electron beam co-radiation to obtain PS-PGMA microspheres, then followed by the amination with diethylenetriamine (DETA) to formed PS-PGMA-DETA (PGD) microspheres through nucleophilic substitution between amino and epoxy group, and finally PS-PGMA-DETA-PA (PGDP) microspheres was obtained by phosphorylation with phosphorous acid (PA). The obtained chelating resin absorbent was characterized by Fourier-transform infrared (FT-IR), thermogravimetric analysis (TGA), scanning electron microscopy (SEM), which demonstrated that the millimetric aminophosphonic acid chelating resin were successfully prepared with well-defined morphology and enhanced thermal stability. The X-ray photoelectron spectroscopy (XPS) characterization results confirmed a possible adsorption mechanism, which is mainly based on the chelation and coordination of N and O in PDGP with La(III) in the solution. A series of parameters were taken into account in the adsorption experiment, such as absorbed dose, GMA concentration, dosage of PGDP, pH, contact time, temperature, and the initial concentrations of La(III). The maximum adsorption capacity obtained from the research can be achieved 288.69 mg/g at 298.15 K, pH = 6. The kinetic sorption for for La(III) fitted the type 1 pseudo-second-order (R2 = 0.9981), which revealed that the La(III) are chemisorbed on the surface of the PGDP. It was concluded that the La(III) adsorption conformed to the Freundlich equation, indicating a multilayer adsorption process. Thermodynamic data indicated that the La(III) uptake process was a spontaneous and endothermic. In addition, this research provided a new irradiation grafting method for rare earth ions removal.  相似文献   

4.
The adsorption behavior of Eu(III) from aqueous solution to mesoporous molecular sieves (Al-MCM-41) is investigated as a function of contact time, solid content, ionic strength, pH, foreign ions and temperature by using batch technique. The experimental results show that Eu(III) adsorption is strongly dependent on pH values, but independent of ionic strength and foreign cations under our experimental conditions. The kinetic process is described by a pseudo-second-order rate model very well. The adsorption isotherms are simulated by Langmuir model very well. The thermodynamic parameters (∆G°, ∆S°, ∆H°) are calculated from the temperature dependent adsorption isotherms at 293, 313 and 333 K, respectively, and the results suggest that the adsorption of Eu(III) on Al-MCM-41 is a spontaneous and endothermic process. Desorption studies indicate that the adsorbed Eu(III) is very difficult to be desorbed from the solid surface. Al-MCM-41 is a suitable material for the preconcentration and solidification of Eu(III) from large volumes of aqueous solutions.  相似文献   

5.
A new chelating polymeric sorbent has been developed using polystyrene resin grafted with ethylenediamino tris(methylenephosphonic) acid. After characterisation by FTIR and elementary analysis, the new grafted resin has been investigated in liquid–solid extraction of uranium(VI). The influence of analytical parameters including pH, amount of resin, metal ion concentration, sample volume and ionic strength were investigated on the recovery of U(VI). Adsorption kinetic and isotherm studies were also carried out to understand the nature of the sorption of uranium(VI) by the resin. The total sorption capacity was found to be 41.76 mg/g under optimum conditions. The total desorption of the sorbed uranium ions was successfully performed with 0.1 M ammonium carbonate. Further, the effect of temperature was realized and the thermodynamic parameters were calculated.  相似文献   

6.
Effects of pH, Eu(III) concentration, ionic strength, temperature and humic acid (HA) on Eu(III) sorption to iron oxides were investigated in detail. The sorption of Eu(III) to iron oxides was significantly dependent on pH and weakly dependent on ionic strength, and higher temperature was gainful to Eu(III) sorption. In the presence of HA, Eu(III) sorption was enhanced significantly at low pH; whilst obvious negative effect was observed in higher pH range. Below 12 mg/L HA, HA could obviously enhanced Eu(III) sorption to iron oxides, nevertheless Eu(III) sorption decreased steeply with increasing HA while HA exceeded 12 mg/L. The results were helpful for understanding radionuclides behaviors in natural environment.  相似文献   

7.
史楠  高保娇  杨青 《物理化学学报》2015,30(11):2168-2176
以微米级硅胶微粒为基质, 通过接枝聚合和大分子反应, 制备了具有刷状结构的阳离子性接枝微粒, 深入研究了其对牛血清白蛋白(BSA)的强吸附能力、吸附机理和吸附热力学. 首先使含叔胺基团的单体甲基丙烯酸二甲基氨基乙酯(DMAEMA)在硅胶微粒表面发生接枝聚合, 制得接枝微粒PDMAEMA/SiO2, 然后以氯乙胺为试剂, 使接枝大分子PDMAEMA链中的叔胺基团发生季铵化反应, 获得了具有刷状结构的阳离子聚电解质的功能接枝微粒QPDMAEMA/SiO2. 测定了微粒QPDMAEMA/SiO2的zeta 电位, 实施了对BSA的等温吸附实验, 考察了介质pH值、离子强度及温度对吸附作用的影响, 研究了吸附热力学. 研究结果表明, 功能接枝微粒QPDMAEMA/SiO2 比接枝微粒PDMAEMA/SiO2 具有更高的zeta 电位, 在静电相互作用驱动下, 微粒QPDMAEMA/SiO2对BSA具有很强的吸附能力. 吸附容量随介质pH值的增大呈现先增大后减小的变化趋势,当pH值等于BSA的等电点(pI=4.7)时, 具有最高的吸附容量(高达112 mg·g-1). 以等电点为界, 离子强度对吸附容量会产生完全相反的影响作用: 当介质pH值小于BSA的等电点时, 电解质浓度增大, 吸附容量增高; 当介质pH值等于BSA的等电点时, 吸附容量几乎不随电解质的浓度发生变化. 吸附过程熵值减小而且放出热量,是一个焓驱动的吸附过程.  相似文献   

8.
Metal ions sorption can be significantly affected by the presence of other sorbates, especially of complexing ligands. In this study, the effect of Se(IV) on Eu(III) sorption onto TiO2 at different pH and Eu(III) concentration was investigated. Se(IV) was found to enhance Eu(III) sorption as a function of Se(IV) concentration. Constant capacitance model was successfully used to interpret the sorption experimental data. The solubility product of Eu2(SeO3)3 at ambient temperature was investigated to highlight the sorption mechanism of ternary sorption system. The pK sp value of Eu2(SeO3)3 was found to be 31.51 ± 0.95.  相似文献   

9.
The adsorption of Eu(III) on multiwalled carbon nanotubes (MWCNTs) as a function of pH, ionic strength and solid contents are studied by batch technique. The results indicate that the adsorption of Eu(III) on MWCNTs is strongly dependent on pH values, dependent on ionic strength at low pH values and independent of ionic strength at high pH values. Strong surface complexation and ion exchange contribute to the adsorption of Eu(III) on MWCNTs at low pH values, whereas surface complexation and surface precipitation are the main adsorption mechanism of Eu(III) on MWCNTs. The desorption of adsorbed Eu(III) from MWCNTs by adding HCl is also studied and the recycling use of MWCNTs in the removal of Eu(III) is investigated after the desorption of Eu(III) at low pH values. The results indicate that adsorbed Eu(III) can be easily desorbed from MWCNTs at low pH values, and MWCNTs can be repeatedly used to remove Eu(III) from aqueous solutions. MWCNTs are suitable material in the preconcentration and solidification of radionuclides from large volumes of aqueous solutions in nuclear waste management.  相似文献   

10.
Cellulose microsphere (CMS) adsorbent was prepared by radiation-induced grafting of dimethylaminoethyl methacrylate (DMAEMA) onto CMS followed by a protonation process. The FTIR spectra analysis proved that PDMAEMA was grafted successfully onto CMS. The adsorption of Cr(VI) onto the resulting adsorbent was very fast, the equilibrium adsorption could be achieved within 15 min. The adsorption capacity strongly depended on the pH of the solution, which was attributed to the change of both the existed forms of Cr(VI) and the tertiary-ammonium group of PDMAEMA grafted CMS with the pH. A maximum Cr(VI) uptake (ca. 78 mg g?1) was obtained as the pH was in the range of 3.0–6.0. However, even in strong acid media (pH 1.3), the adsorbents still showed a Cr(VI) uptake of 30 mg g?1. The adsorption behavior of the resultant absorbent could be described with the Langmuir mode. This adsorbent has potential application for removing heavy metal ion pollutants (e.g. Cr(VI)) from wastewater.  相似文献   

11.

The separation of americium(III) from europium(III) was achieved utilizing a bis-2,6-(5,6,7,8-tetrahydro-5,9,9-trimethyl-5,8-methano-1,2,4-benzotriazin-3-yl) pyridine (CA-BTP) chromatographic resin. The extraction chromatographic materials were prepared using various concentrations of CA-BTP. This new, hydrolytically stable extractant was impregnated on an inert polymeric support at 40% loading. The uptake of Am(III) and Eu(III) by this material from 0.1 to 4.0 M aqueous HNO3 solutions was measured. The resulting dry weight distribution ratios, D w , indicated a strong preference for Am(III) with little affinity for Eu(III). These results are similar to recently reported solvent extraction studies indicating a maximum uptake of Am(III) in the 0.5–1.0 M HNO3 range. The resin preparation, performance, and characterization of the Am/Eu separation are reported herein.

  相似文献   

12.
A new modified nanometer SiO2 using 5-sulfosalicylic acid (SSA) as a solid-phase extractant was used for separation, preconcentration and determination of Fe(III) in aqueous solutions by inductively coupled plasma atomic emission spectrometry (ICP-AES). Its adsorption and preconcentration behaviour for Fe(III) in aqueous solutions was investigated using static procedures in detail. The optimum pH value for the separation of Fe(III) on the newly designed sorbent was 3.5. Complete elution of the adsorbed Fe(III) from the nanometer SiO2-SSA was carried out using 2.0 mL of 0.01 mol L− 1 of HCl. The time of 90% sorption was less than 2 min for Fe(III) at pH 3.5. Common coexisting ions did not interfere with the separation and determination of Fe(III) at pH 3.5. The maximum static adsorption capacity of the sorbent at optimum conditions was found to be 44.01 mg of Fe(III) per gram of sorbent. The relative standard deviation (RSD) of the method under optimum conditions was 3% (n = 5). The procedure was validated by analyzing three certified reference materials (GBW 08301, GBW 08504, GBW 08511), the results obtained were in good agreement with standard values. The nanometer SiO2-SSA was successfully employed in the separation and preconcentration of the investigated Fe(III) from the biological and natural water samples yielding 100-folds concentration factor.  相似文献   

13.
For the selective extraction of Am(III) and Eu(III), quadridentate divalent phenolic Schiff bases-bis-salicylaldehyde ethylenediamine (H2salen) was investigated as a kind of extractant. The influences of alkaline cation, inorganic anion, ionic strength, pH and the concentration of H2salen on the distribution ratio of Am(III) and Eu(III) were investigated in detail. As a result, Am(III) and Eu(III) made anionic 1:1 complexes with the ligand (H2salen) and could be extracted into nitrobenzene as ion-pairs with a suitable monovalent counter anion in the aqueous solution, the extracted species were possibly of the type Am(H2salen) Eu(salen)Cl and Eu(H2salen)Cl3, respectively. The extractability of Eu(III) was significantly stronger than that of Am(III) and the maximum separation factor, SF(Am/Eu), was 96 at pH 4.0. The results indicated that H2salen had good selectivity for Am(III) and Eu(III).  相似文献   

14.
The speciation of inorganic Sb(III) and Sb(V) ions in aqueous solution was studied. The adsorption behavior of Sb(III) and Sb(V) ions were investigated as iodo and ammonium pyrollidine dithiocarbamate (APDC) complexes on a column filled with Amberlite XAD-8 resin. Sb(III) and Sb(V) ions were recovered quantitatively and simultaneously from a solution containing 0.8 M NaI and 0.2 M H2SO4 by the XAD-8 column. Sb(III) ions were also adsorbed quantitatively as an APDC complex, but the recovery of the Sb(V)-APDC complex was found to be <10% at pH 5. According to these data, the concentrations of total antimony as Sb(III)+Sb(V) ions and Sb(III) ion were determined with XAD-8/NaI+H2SO4 and XAD-8/APDC systems, respectively. The Sb(V) ion concentration was calculated by subtracting the Sb(III) concentration found with XAD-8/APDC system from the total antimony concentration found with XAD-8/NaI+H2SO4 system. The developed method was applied to determine Sb(III) and Sb(V) ions in samples of artificial seawater and wastewater.  相似文献   

15.
In order to develop a direct separation process for trivalent minor actinides from fission products in high level liquid waste (HLLW) by extraction chromatography, a novel macroporous silica-based 2,6-bis(5,6-diisohexyl)-1,2,4-triazin-3-yl)pyridine resin (isohexyl-BTP/SiO2-P resin) was prepared. The content of isohexyl-BTP extractant in the resin was as high as 33.3 wt%. The resin exhibited much higher adsorption affinity for Am(III) in 2–3 M (mol/L) HNO3 solution over U and FP which are contained in HLLW. The kinetic data were analyzed using pseudo-second-order equation. The results suggested that the Eu(III), Gd(III), and Dy(III) adsorption was well explained by the pseudo-second-order equation. Quantitative desorption for adsorbed elements was achieved by using H2O or thiourea as eluting agents. However, the kinetics of adsorption and desorption were rather slow and this drawback needs to be resolved. Stability of the resin against HNO3 was also examined. It was found that the resin was considerably stable against ≤4 M HNO3 solution for the reasons of an extremely small leakage of the extractant into the solution from the resin and the adsorption performance keeping for rare earths in 3 M HNO3 solution.  相似文献   

16.
An S‐mandelic acid imprinted chitosan resin was synthesized by cross‐linking chitosan with glutaraldehyde in 2% acetic acid solution. S‐Mandelic acid imprinted chitosan resin was used to enantioselectively separate racemic mandelic acid in aqueous medium. When keeping the pH of sample solution (100 mM Tris‐H3PO4) at 3.5 and adsorption time at 40 min, the enantiomer excess of mandelic acid in supernatant was 78.8%. The adsorption capacities of S‐mandelic acid imprinted chitosan resin for S‐ and R‐mandelic acid were determined to be 29.5 and 2.03 mg/g, respectively. While the adsorption capacities of non‐imprinted cross‐linked chitosan for S‐ and R‐mandelic acid were 2.10 and 2.08 mg/g, respectively. The result suggests that the imprinted caves in S‐mandelic acid imprinted chitosan resin are highly matched with S‐mandelic acid molecule in space structure and spatial arrangement of action sites. Interestingly, the enantiomer excess value of mandelic acid in supernatant after adsorption of racemic mandelic acid by R‐mandelic acid imprinted cross‐linked chitosan was 25.4%. The higher enantiomer excess value by S‐mandelic acid imprinted chitosan resin suggests that the chiral carbons in chitosan and the imprinted caves in S‐mandelic acid imprinted chitosan resin combine to play roles for the enantioselectivity of S‐mandelic acid imprinted chitosan resin toward S‐mandelic acid. Furthermore, the excellent enantioselectivity of S‐mandelic acid imprinted chitosan resin toward S‐mandelic acid demonstrates that using chiral chitosan as functional monomer to prepare molecularly imprinted polymers has great potential in enantioseparation of chiral pharmaceuticals.  相似文献   

17.
The effects of pH,contact time and natural organic ligands on radionuclide Eu(Ⅲ) adsorption and mechanism on titanate nanotubes(TNTs) are studied by a combination of batch and extended X-ray absorption fine structure(EXAFS) techniques.Macroscopic measurements show that the adsorption is ionic strength dependent at pH < 6.0,but ionic strength independent at pH > 6.0.The presence of humic acid(HA) /fulvic acid(FA) increases Eu(Ⅲ) adsorption on TNTs at low pH,but reduces Eu(Ⅲ) adsorption at high pH.The results of EXAFS analysis indicate that Eu(Ⅲ) adsorption on TNTs is dominated by outer-sphere surface complexation at pH < 6.0,whereas by inner-sphere surface complexation at pH > 6.0.At pH < 6.0,Eu(Ⅲ) consists of ~ 9 O atoms at REu?O ≈ 2.40  in the first coordination sphere,and a decrease in NEu-O with increasing pH indicates the introduction of more asymmetry in the first sphere of adsorbed Eu(Ⅲ).At long contact time or high pH values,the Eu(Ⅲ) consists of ~2 Eu at REu-Eu ≈ 3.60  and ~ 1 Ti at REu-Ti ≈ 4.40 ,indicating the formation of inner-sphere surface complexation,surface precipitation or surface polymers.Surface adsorbed HA/FA on TNTs modifies the species of adsorbed Eu(Ⅲ) as well as the local atomic structures of adsorbed Eu(Ⅲ) on HA/FA-TNT hybrids.Adsorbed Eu(Ⅲ) on HA/FA-TNT hybrids forms both ligand-bridging ternary surface complexes(Eu-HA/FA-TNTs) as well as surface complexes in which Eu(Ⅲ) remains directly bound to TNT surface hydroxyl groups(i.e.,binary Eu-TNTs or Eu-bridging ternary surface complexes(HA/FA-Eu-TNTs)).The findings in this work are important to describe Eu(Ⅲ) interaction with nanomaterials at molecular level and will help to improve the understanding of Eu(Ⅲ) physicochemical behavior in the natural environment.  相似文献   

18.
Batch sorption experiments were performed to remove Eu(III) ions from aqueous solutions by using attapulgite under ambient conditions. Different experimental conditions, such as contact time, solid content, foreign ions, pH, ionic strength, fulvic acid and temperature, have been investigated to study their effect on the sorption property. The results indicated that the sorption of Eu(III) onto attapulgite was strongly dependent on pH, ionic strength and temperature. The sorption increased from about 8.9 to 90% at pH ranging from 2 to 6 in 0.01 mol/L NaNO3 solution. The Eu(III) kinetic sorption on attapulgite was fitted by the pseudo-second-order model better than by the pseudo-first-order model. The sorption of Eu(III) onto attapulgite increased with increasing temperature and decreasing ionic strength. The Langmuir and Freundlich models were used to simulate the sorption isotherms, and the results indicated that the Freundlich model simulated the data better than the Langmuir model. The thermodynamic parameters (∆G o, ∆S o, ∆H o) were determined from the temperature dependent isotherms at 298.15, 318.15 and 338.15 K, and the results indicated that the sorption reaction was an endothermic and spontaneous process. The results suggest that the attapulgite is a suitable material as an adsorbent for preconcentration and immobilization of Eu(III) from aqueous solutions.  相似文献   

19.
The competitive sorption of Cu(II), Eu(III) and U(VI) ions in aqueous solutions by TiO2, has been investigated by potentiometry at I = 0.1 M NaClO4, 25 °C and under atmospheric conditions. For Cu(II) ions the investigation was performed directly by means of a Cu2+ ion selective electrode, whereas for the Eu(III) and U(VI) ions indirectly based on competition reactions between the Cu(II) ion and the Eu(III) and U(VI) ions. Numerical analysis of the experimental data supports the formation of inner-sphere surface complexes and allows the evaluation of the formation constant of the (TiO)2Cu, which is found to amount to log β* = 4.3 ± 0.4. Addition of competing Eu(III) and U(VI) ions in the aqueous system leads to replacement of the Cu(II) by the competitor metal ion. Evaluation of the potentiometric data obtained from competition experiments indicates on an ion exchange mechanism. The formation constant of the Eu(III) and U(VI) species adsorbed on TiO2 is found to be log β* = 4.4 ± 0.7 and 4.8 ± 0.8, respectively. The relative affinity of the TiO2 surface for the metal ions under investigation is U(VI) > Eu(III) > Cu(II).  相似文献   

20.
Eu(III) adsorption on rutile was investigated as a function of contact time, pH, ionic strength and Eu(III) concentration by using a batch experimental method. The effects of carbonate, sulfate, and phosphate were also studied. It was found that the kinetics of Eu(III) adsorption on rutile could be described by a pseudo-second-order model. The adsorption of Eu(III) on rutile is strongly pH-dependent, but relatively insensitive to ionic strength. A double layer model (DLM) with two inner-sphere Eu(III) surface complexes was applied to quantitatively interpret the adsorption of Eu(III) on rutile. There were no apparent effects of carbonate and sulfate on Eu(III) adsorption, whereas the presence of phosphate promoted Eu(III) adsorption on rutile. The surface complexes of Eu(III) on rutile were evidenced by X-ray photoelectron spectroscopy (XPS).  相似文献   

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