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1.
2.
Adsorption and desorption of uranium(VI) from dilute aqueous solutions by Eucalyptus citriodora distillation sludge was studied in a batch mode. The potential of Eucalyptus citriodora distillation sludge to remove uranium(VI) from aqueous solutions has been investigated at different conditions of solution pH, metal ion concentrations, biosorbent dosage, biosorbent particle size, contact time and temperature. The results indicated that biosorption capacity of Eucalyptus citriodora distillation sludge was strongly affected by the medium pH, the biosorbent dose, metal ion concentrations and medium temperature. Reduction in particle size increased the biosorption capacity. Langmuir and Freundlich isotherm models were applied to biosorption data to determine the biosorption characteristics. An optimum biosorption capacity (57.75 mg/g) was achieved with pH 4.0, particle size 0.255 mm, biosorbent dose 0.5 g/100 mL and initial uranium(VI) concentration of 100 mg/L. Uranium(VI) removal by Eucalyptus citriodora distillation sludge was rapid, the equilibrium was established within 60 min and pseudo-second-order model was found to fit with the experimental data. The biosorption process decreased with an increase in the temperature indicating its exothermic nature. Pretreatments of biomass with different reagents affected its biosorption capacity. A significant increase (34 %) in biosorption capacity (83.25 mg/g) was observed with benzene treatment. Fourier-transform infra-red studies showed the involvement of carbonyl, carboxyl and amide groups in the biosorption process. The results indicated that sulfuric acid had the best effects as an eluent showing 93.24 % desorption capacity.  相似文献   

3.
An iron (III)-impregnated sorbent was prepared from sugarcane bagasse and ferric chloride solution via carbonization/activation in a muffle furnace at 500?°C for 4?h. The adsorption removal of chromium (VI) from aqueous solution by the iron (III)-impregnated sorbent was then studied in a batch system. With increasing initial chromium (VI) concentration from 25 to 130?mg/L at an adsorbent dose of 300?mg/50?mL, the amount of adsorbed chromium (VI) increased from 4.15 to 12.20?mg/g at 20?°C, from 4.16 to 12.50?mg/g at 30?°C, and from 4.16 to 13.72?mg/g at 40?°C. The dynamical data fit very well with the pseudo-second-order kinetic model, and the calculated adsorption capacities of 4.16, 8.37, and 13.37?mg/g were equal to the actual values of the experiments at the initial chromium (VI) concentrations of 25, 50, and 100?mg/L, respectively. The Langmuir isotherm could yield better fits than the Freundlich isotherm. The calculated isotherm parameters confirmed the favorable adsorption of chromium (VI) on the iron (III)-impregnated sorbent.  相似文献   

4.
To assess the dynamics of microbially mediated U-clay redox reactions, we examined the reduction of iron(III)-rich nontronite NAu-2 and uranium(VI) by Shewanella oneidensis MR-1. Bioreduction experiments were conducted with combinations and varied concentrations of MR-1, nontronite, U(VI) and the electron shuttle anthraquinone-2,6-disulfonate (AQDS). Abiotic experiments were conducted to quantify U(VI) sorption to NAu-2, the reduction of U(VI) by chemically-reduced nontronite-Fe(II), and the oxidation of uraninite, U(IV)O2(s), by nontronite-Fe(III). When we incubated S. oneidensis MR-1 at lower concentration (0.5 × 108 cell mL−1) with nontronite (5.0 g L−1) and U(VI) (1.0 mM), little U(VI) reduction occurred compared to nontronite-free incubations, despite the production of abundant Fe(II). The addition of AQDS to U(VI)- and nontronite-containing incubations enhanced both U(VI) and nontronite-Fe(III) reduction. While U(VI) was completely reduced by S. oneidensis MR-1 at higher concentration (1.0 × 108 cell mL−1) in the presence of nontronite, increasing concentrations of nontronite led to progressively slower rates of U(VI) reduction. U(VI) enhanced nontronite-Fe(III) reduction and uraninite was oxidized by nontronite-Fe(III), demonstrating that U served as an effective electron shuttle from S. oneidensis MR-1 to nontronite-Fe(III). The electron-shuttling activity of U can explain the lack or delay of U(VI) reduction observed in the bulk solution. Little U(VI) reduction was observed in incubations that contained chemically-reduced nontronite-Fe(II), suggesting that biologic U(VI) reduction drove U valence cycling in these systems. Under the conditions used in these experiments, we demonstrate that iron-rich smectite may inhibit or delay U(VI) bioreduction.  相似文献   

5.
A hydrophilic kapok fiber was prepared by a chemical process of the Fenton reaction and used as an adsorbent to remove Pb(II) from aqueous solution. The effects of experimental parameters including pH, contact time, Pb(II) concentration, and coexisting heavy metals were estimated as well as evaluated. The optimum concentrations of FeSO4 and H2O2 for the Fenton reaction-modified kapok fiber (FRKF) were 0.5 mol L?1 and 1 mol L?1, respectively. The adsorption kinetic models and isotherm equations of Langmuir and Freundlich were conducted to identify the most optimum adsorption rate and adsorption capacity of Pb(II) on FRKF. The FRKF displayed an excellent adsorption rate for Pb(II) in single metal solution with the maximum adsorption capacity of 94.41?±?7.56 mg g?1 at pH 6.0. Moreover, the FRKE still maintained its adsorption advantage of Pb(II) in the mixed metal solution. The FRKF exhibited a considerable potential in removal of metal content in wastewater streams.  相似文献   

6.
The removal of the chromium (VI) ion from aqueous solutions with the Lewatit FO36 ion-exchange resin is described at different conditions. The effects of adsorbent dose, initial metal concentration, contact time and pH on the removal of chromium (VI) were investigated. The batch ion exchange process was relatively fast and it reached equilibrium after about 90 min of contact. The ion exchange process, which is pH dependent showed maximum removal of chromium (VI) in the pH range 5.0–8.0 for an initial chromium (VI) concentration of 0.5 mg/dm3. The equilibrium related to Lewatit FO36 ion- exchange capacity and the amounts of the ion exchange were obtained using the plots of the Langmuir adsorption isotherm. It was observed that the maximum ion exchange capacity of 0.29 mmol of chromium (VLVg for Lewatit FO36 was achieved at optimum pH value of 6.0. The ion exchange of chromium (VI) on this cation-exchange resin followed first-order reversible kinetics.  相似文献   

7.
Potato starch and dextrins resulting from thermolysis of potato starch in the absence of reagents and presence of -amino acids are promising depressants for separation of lead and copper minerals present in the Polish industrial copper concentrates. The polysaccharides were used for differential xanthate flotation of the final industrial concentrates produced by flotation with sulfhydryl collectors in the absence of depressants. The polysaccharides depressed galena and provided froth concentrate rich in chalcocite and other copper minerals as well as cell product containing lead minerals. The best results of separation were obtained in the presence of plain dextrin prepared by a thermal degradation of potato starch. The industrial concentrate containing 18.5% Cu and 5.5% Pb was divided into a froth product containing 38.1% Cu with 77% recovery of copper and a cell product assaying 7.3% Pb with 83% recovery of lead. It was accomplished using 2500 g/t of dextrin, 50g/t of potassium ethyl xanthate, and 50 g/t of frother (α-terpineol). The pH of flotation was 8.0–8.2.  相似文献   

8.
Iron oxides may undergo structural transformations when entering an anoxic environment. These transformations were investigated using the isotopic exchange between aqueous Fe(II) and iron oxides in experiments with 55Fe-labelled iron oxides. 55Fe was incorporated congruently into a ferrihydrite, two lepidocrocites (#1 and #2), synthesised at 10°C and 25°C, respectively, a goethite and a hematite. The iron oxides were then submerged in Fe2+ solutions (0-1.0 mM) with a pH of 6.5. In the presence of aqueous Fe2+, an immediate and very rapid release of 55Fe was observed from ferrihydrite, the two lepidocrocites and goethite, whereas in the absence of Fe2+ no release was observed. 55Fe was not released from hematite, even at the higher Fe2+ concentration. The release rate is mainly controlled by characteristics of the iron oxides, whereas the concentration of Fe2+ only has minor influence. Ferrihydrite and 5-nm-sized lepidocrocite crystals attained complete isotopic equilibration with aqueous Fe(II) within days. Within this timeframe ferrihydrite transformed completely into new and more stable phases such as lepidocrocite and goethite. Lepidocrocite #2 and goethite, having larger particles, did not reach isotopic equilibrium within the timeframe of the experiment; however, the continuous slow release of 55Fe suggests that isotopic equilibrium will ultimately be attained.Our results imply a recrystallization of solid Fe(III) phases induced by the catalytic action of aqueous Fe(II). Accordingly, iron oxides should properly be considered as dynamic phases that change composition when exposed to variable redox conditions. These results necessitate a reevaluation of current models for the release of trace metals under reducing conditions, the sequestration of heavy metals by iron oxides, and the significance of stable iron isotope signatures.  相似文献   

9.
Reduction of U(VI) under iron reducing conditions was studied in a model system containing the dissimilatory metal-reducing bacterium Shewanella putrefaciens and colloidal hematite. We focused on the competition between direct enzymatic uranium reduction and abiotic reduction of U(VI) by Fe(II), catalyzed by the hematite surface, at relatively low U(VI) concentrations (< 0.5 μM) compared to the concentrations of ferric iron (> 10 mM). Under these conditions surface catalyzed reduction by Fe(II), which was produced by dissimilatory iron reduction, was the dominant pathway for uranium reduction. Reduction kinetics of U(VI) were identical to those in abiotic controls to which soluble Fe(II) was added. Strong adsorption of U(VI) at the hematite surface apparently favored the abiotic pathway by reducing the availability of U(VI) to the bacteria. In control experiments, lacking either hematite or bacteria, the addition of 45 mM dissolved bicarbonate markedly slowed down U(VI) reduction. The inhibition of enzymatic U(VI) reduction and abiotic, surface catalyzed U(VI) reduction by the bicarbonate amendments is consistent with the formation of aqueous uranyl-carbonate complexes. Surprisingly, however, more U(VI) was reduced when dissolved bicarbonate was added to experimental systems containing both bacteria and hematite. The enhanced U(VI) reduction was attributed to the formation of magnetite, which was observed in experiments. Biogenic magnetite produced as a result of dissimilatory iron reduction may be an important agent of uranium immobilization in natural environments.  相似文献   

10.
A novel polyurethane foam/organobentonite/iron oxide nanocomposite adsorbent was successfully prepared via in situ polymerization of toluene diisocyanate and polyol in presence of 5 wt% organobentonite/iron oxide. The obtained nanocomposite was characterized in detail, and the results revealed that the clay layers are exfoliated and/or intercalated in the polymer matrix forming a nanocomposite structure. The application of the prepared nanocomposite for adsorption of cadmium ions from aqueous solution was tested as a function of various experimental parameters using batch procedures. Adsorptive removal of Cd(II) onto the nanocomposite attained maximum at adsorbent content 1.5 g/L, pH 6, and the equilibrium was established within 60 min. Kinetic studies showed that the experimental data fit very well to pseudo-second-order model, and the adsorption process proceeds through three steps. It was found that external liquid film and intraparticle diffusion steps deeply affect the rate of Cd2+ ions adsorption onto the synthesized nanocomposite. Langmuir isotherm model fitted the adsorption data better than Freundlich with a maximum adsorption capacity (q m) for Cd(II) equal to 78 mg/g under the specified experimental conditions. The synthesized nanocomposite afforded effective extraction for Cd2+ ions from natural water samples and excellent reusability feature. This study declares the potential efficiency of a new clay/polymer nanocomposite as alternative for wastewater remediation.  相似文献   

11.
A mixing of metal-loaded acid mine drainage with shallow groundwater or surface waters usually initiates oxidation and/or hydrolysis of dissolved metals such as iron (Fe) and aluminum (Al). Colloidal particles may appear and agglomerate with increasing pH. Likewise chemical conditions may occur while flooding abandoned uranium mines. Here, the risk assessment of hazards requires reliable knowledge on the mobility of uranium (U). A flooding process was simulated at mesocosm scale by mixing U-contaminated acid mine water with near-neutral groundwater under oxic conditions. The mechanism of U-uptake by fresh precipitates and the molecular structure of U bonding were determined to estimate the mobility of U(VI). Analytical and spectroscopic methods such as Extended X-ray Absorption Fine-Structure (EXAFS) spectroscopy at the Fe K-edge and the U LIII-edge, and Attenuated Total Reflectance Fourier Transform Infrared (ATR-FTIR) spectroscopy were employed. The freshly formed precipitate was identified as colloidal two-line ferrihydrite. It removed U(VI) from solution by sorption processes, while surface precipitation or structural incorporation of U was not observed. EXAFS data suggest a mononuclear inner-sphere, edge-sharing complex of U(VI) with ferrihydrite in the absence of dissolved carbonate. By employing a novel EXAFS analysis method, Monte Carlo Target Transformation Factor Analysis, we could for the first time ascertain a 3-D configuration of this sorption complex without the necessity to invoke formation of a ternary complex. The configuration suggests a slightly tilted position of the adsorbed unit relative to the edge-sharing Fe(O, OH)6 octahedra. In the presence of dissolved carbonate and at pH ∼8.0, a distal carbonate O-atom at ∼4.3 Å supports formation of ternary U(VI)-carbonato surface complexes. The occurrence of these complexes was also confirmed by ATR-FTIR. However, in slightly acidic conditions (pH 5-6) in equilibrium with atmospheric CO2, the U(VI) sorption on ferrihydrite was dominated by the binary complex species Fe(O)2UO2, whereas ternary U(VI)-carbonato surface complexes were of minor relevance. While sulfate and silicate were also present in the mine water, they had no detectable influence on U(VI) surface complexation. Our experiments demonstrate that U(VI) forms stable inner-sphere sorption complexes even in the presence of carbonate and at slightly alkaline pH, conditions which previously have been assumed to greatly accelerate the mobility of U(VI) in aqueous environments. Depending on the concentrations of U(VI) and carbonate, the type of surface complexes may change from binary uranyl-ferrihydrite to ternary carbonato-uranyl-ferrihydrite complexes. These different binding mechanisms are likely to influence the binding stability and retention of U(VI) at the macroscopic level.  相似文献   

12.
Dry lakes, degraded sandy grasslands, abandoned farmland and mobile dunes which are widely distributed throughout the arid areas of northern China have been investigated in this work. Gain-size distribution of the surface sediments of Manas lake in Junggar basin, Juyan lake in the Alxa plateau, Zhuye lake in Minqin basin and most deserts (such as Mu Us desert, Otindag desert, Horqin desert and Hulun Buir desert) in China have been analyzed. The results show clay with particle sized <10 μm on the surface sediments of dry lakebed and sandy grassland developed from dry lakebed, respectively, account for >60% and ∼50% of the total mass. Since the tiny particles on the surface of abandoned farmland are blown away easily and rapidly, the content of clay particles in Minqin basin is <14%. The grain-size distribution of mobile dunes in northern China mainly consists of particles >63 μm and few particles <10 μm. Consequently, although sand/dust storms originate primarily in the western deserts, the gobi areas of the Alxa plateau, the north and east of Hexi Corridor and in central Mongolia, the widely distributed dry lakebeds, sandy grasslands and abandoned farmland adjacent to the deserts also contribute to aeolian dusts. Hence, the material sources for sand dust storm in East Asia include inland deserts, but also dry lakes, sandy grasslands and abandoned farmland, which are widely distributed throughout the arid inlands of northern China.  相似文献   

13.
Recent studies of uranium(VI) geochemistry have focused on the potentially important role of the aqueous species, CaUO2(CO3)32− and Ca2UO2(CO3)30(aq), on inhibition of microbial reduction and uranium(VI) aqueous speciation in contaminated groundwater. However, to our knowledge, there have been no direct studies of the effects of these species on U(VI) adsorption by mineral phases. The sorption of U(VI) on quartz and ferrihydrite was investigated in NaNO3 solutions equilibrated with either ambient air (430 ppm CO2) or 2% CO2 in the presence of 0, 1.8, or 8.9 mM Ca2+. Under conditions where the Ca2UO2(CO3)30(aq) species predominates U(VI) aqueous speciation, the presence of Ca in solution lowered U(VI) adsorption on quartz from 77% in the absence of Ca to 42% and 10% at Ca concentrations of 1.8 and 8.9 mM, respectively. U(VI) adsorption to ferrihydrite decreased from 83% in the absence of Ca to 57% in the presence of 1.8 mM Ca. Surface complexation model predictions that included the formation constant for aqueous Ca2UO2(CO3)30(aq) accurately simulated the effect of Ca2+ on U(VI) sorption onto quartz and ferrihydrite within the thermodynamic uncertainty of the stability constant value. This study confirms that Ca2+ can have a significant impact on the aqueous speciation of U(VI), and consequently, on the sorption and mobility of U(VI) in aquifers.  相似文献   

14.
A new spectrophotometric method for the microdetermination of uranium(VI) from phosphorites in the presence of commonly occurring metal ions has been developed. Uranium is extracted from chloroform solution of N-phenyl-2-naphtho-hydroxamic acid (N-P-2-NHA) at pH 4.0–4.5. The orange-red extract has the maximum absorption at 515 nm. The extraction was quantitative and obeys Beer's law at 515 nm.  相似文献   

15.
Amorphous tin(VI) hydrogen phosphate (ATHP) was synthesized using the liquid phase precipitation method and served as an adsorbent to remove Pb(II), Cu(II), and Zn(II) from aqueous solutions. The ATHP was characterized by powder X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption–desorption techniques. Adsorption properties were evaluated as a function of pH, reaction time, concentration of reactants, and salinity. Their equilibrium adsorption data were modeled using Freundlich, Langmuir, and Dubinin–Kaganer–Radushkevich isotherms, respectively. The results revealed that adsorption equilibrium reached within 180 min. ATHP indicated good adsorption even below the pHZPC, and best adsorption at pH 5 for Pb(II) and Cu(II) and at pH 5.5 for Zn(II) was observed. Equilibrium data fitted better to the Langmuir model for Pb(II) and Cu(II) and fitted better to the Freundlich model for Zn(II). The saturated adsorption capacities deduced from the Langmuir model were 2.425, 1.801, and 0.600 mmol/g for Cu(II), Pb(II), and Zn(II), respectively, indicating an adsorption affinity order of Cu > Pb > Zn. There is a negative correlation between the concentration of NaCl and adsorption capacity of ATHP, yet ATHP still exhibited excellent adsorption having an adsorption capacity of 19.35, 15.16, 6.425 mg/g when the concentration of NaCl was 0.6 mol/L. The free energy (E) was 12.33, 10.70, and 14.74 kJ/mol for Pb(II), Cu(II), and Zn(II), respectively. An adsorption mechanism based on ion exchange between heavy metal ions and H+ in the ATHP is proposed. Furthermore, the used ATHP was regenerated by HCl solution and the adsorbent was used repeatedly.  相似文献   

16.
《Geochimica et cosmochimica acta》1999,63(19-20):2919-2928
Construction of the entrance tunnel to the Äspö Hard Rock Laboratory, a prototype repository in Sweden for research into the geological disposal of spent nuclear fuel, has resulted in increased transport of organic carbon from the surface into the groundwater. This increased input of organic matter has induced accelerated oxidation of organic carbon associated with reduction of iron(III) minerals as the terminal electron acceptor in microbial respiration. Hydrochemical modeling of major solute ions at the site indicates an apparent first-order decay constant for organic carbon of 3.7 ± 2.6/yr. This rapid turnover is not accompanied by an equivalent mobilization of ferrous iron. Thermodynamic calculation of iron mineral solubility suggests that ferrous clay minerals may form in hydraulically transmissive fractures. The conditional potentials for the oxidation–reduction of such phases coincide with measured redox potentials at the site. The calculated potential is sufficiently low so that such phases would provide reducing capacity against future intrusion of O2 into the groundwater, thus buffering a repository against oxic corrosion of the engineered barriers.  相似文献   

17.
Structural Fe(II) has been shown to reduce several oxidized environmental contaminants, including NO3, chlorinated solvents, Cr(VI), and U(VI). Studies investigating reduction of U(VI) by soils and sediments, however, suggest that abiotic reduction of U(VI) by Fe(II) is not significant, and that direct enzymatic reduction of U(VI) by metal-reducing bacteria is required for U(VI) immobilization as U(IV). Here evidence is presented for abiotic reduction and immobilization of U(VI) by structural Fe(II) in a redoximorphic soil collected from a hillside spring in Iowa. Oxidation of Fe(II) in the soil after reaction with U(VI) was demonstrated by Mössbauer spectroscopy and reduction of U(VI) by the pasteurized soil using U LIII-edge X-ray absorption spectroscopy (XAS). XAS indicates that both reduced U(IV) and oxidized U(VI) or U(V) are present after U(VI) interaction with the Fe(II) containing soil. The EXAFS data show the presence of a non-uraninite U(IV) phase and evidence of the oxidized U(V) or U(VI) fraction being present as a non-uranyl species. Little U(VI) reduction is observed by soil that has been exposed to air and oxidation of Fe(II) to goethite has occurred. Soil characterization based on chemical extractions, Mössbauer spectroscopy, and Fe K-edge XAS indicate that the majority of Fe(II) in the soil is structural in nature, existing in clay minerals and possibly a green rust-like phase. These data provide compelling evidence for abiotic reduction of U(VI) by structural Fe(II) from soil near Fe-rich oxic–anoxic boundaries in natural environments. The work highlights the potential for abiotic reduction of U(VI) by Fe(II) in reduced, Fe-rich environments.  相似文献   

18.
Uranium(VI), which is often elevated in granitoidic groundwaters, is known to adsorb strongly to Fe (hydr)oxides under certain conditions. This process can be used in water treatment to remove U(VI). To develop a consistent geochemical model for U(VI) adsorption to ferrihydrite, batch experiments were performed and previous data sets reviewed to optimize a set of surface complexation constants using the 3-plane CD-MUSIC model. To consider the effect of dissolved organic matter (DOM) on U(VI) speciation, new parameters for the Stockholm Humic Model (SHM) were optimized using previously published data. The model, which was constrained from available X-ray absorption fine structure (EXAFS) spectroscopy evidence, fitted the data well when the surface sites were divided into low- and high-affinity binding sites. Application of the model concept to other published data sets revealed differences in the reactivity of different ferrihydrites towards U(VI). Use of the optimized SHM parameters for U(VI)-DOM complexation showed that this process is important for U(VI) speciation at low pH. However in neutral to alkaline waters with substantial carbonate present, Ca–U–CO3 complexes predominate. The calibrated geochemical model was used to simulate U(VI) adsorption to ferrihydrite for a hypothetical groundwater in the presence of several competitive ions. The results showed that U(VI) adsorption was strong between pH 5 and 8. Also near the calcite saturation limit, where U(VI) adsorption was weakest according to the model, the adsorption percentage was predicted to be >80%. Hence U(VI) adsorption to ferrihydrite-containing sorbents may be used as a method to bring down U(VI) concentrations to acceptable levels in groundwater.  相似文献   

19.
In recent years, the need for safe and economical methods to eliminate heavy metals from contaminated waters has necessitated research on the production of low-cost alternatives to commercially available activated carbon. In the present work, in order to enhance the removal of heavy metals from contaminated water, Zizyphus vulgaris wastes were modified chemically to produce an adsorbent rich in carboxylic groups to enhance the removal of heavy metals from contaminated water. Adsorption of Zn(II) ions on the produced adsorbent was then optimized. The optimal ratio for esterification involved the treatment of Z. vulgaris wastes (1 g) with 0.0037 mmol malic acid in the presence of a very small amount of water for 2 h at 140 °C. The maximum values for adsorption capacity, q max, were 28.7 and 164.6 mg/g on native and modified Z. vulgaris wastes, respectively, at pH 5 and 30 °C with a contact time 2 h and an initial metal ion concentration of 400 mg/L. The equilibrium data were well fitted by the Langmuir and Freundlich adsorption models and demonstrated the significant capacity for Z. vulgaris wastes in the removal of Zn(II) ions from aqueous solutions.  相似文献   

20.
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