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1.
Yolcubal I  Akyol NH 《Chemosphere》2008,73(8):1300-1307
The transport and fate of arsenate in carbonate-rich soil under alkaline conditions was investigated with multiple approaches combining batch, sequential extraction and column experiments as well as transport modeling studies. Batch experiments indicated that sorption isotherm was nonlinear over a wide range of concentration (0.1-200 mg L(-1)) examined. As(V) adsorption to the calcareous soil was initially fast but then continued at a slower rate, indicating the potential effect of rate-limited sorption on transport. Column experiments illustrated that transport of As(V) was significantly retarded compared to a non-reactive tracer. The degree of retardation decreased with increasing As(V) concentration. As(V) breakthrough curves exhibited nonideal transport behavior due to the coupled effects of nonlinear and rate-limited sorption on arsenate transport, which is consistent with the results of modeling studies. The contribution of nonlinear sorption to the arsenate retardation was negligible at low concentration but increased with increasing As(V) concentration. Sequential extraction results showed that nonspecifically sorbed (easily exchangeable, outer sphere complexes) fraction of arsenate is dominant with respect to the inner-sphere surface bound complexes of arsenate in the carbonate soil fraction, indicating high bioavailability and transport for arsenate in the carbonate-rich soils of which Fe and Al oxyhydroxide fractions are limited.  相似文献   

2.
Arsenic contamination of groundwater is a major threat to human beings globally. Among various methods available for arsenic removal, adsorption is fast, inexpensive, selective, accurate, reproducible and eco-friendly in nature. The present paper describes removal of arsenate from water on zirconium oxide-coated sand (novel adsorbent). In the present work, zirconium oxide-coated sand was prepared and characterised by infrared and X-ray diffraction techniques. Batch experiments were performed to optimise different adsorption parameters such as initial arsenate concentration (100–1,000 μg/L), dose (1–8 g/L), pH of the solution (2–14), contact time (15–150 min.), and temperature (20, 30, 35 and 40 °C). The experimental data were analysed by Langmuir, Freundlich, Temkin and Dubinin–Radushkevich isotherm models. Furthermore, thermodynamic and kinetic parameters were evaluated to know the mode of adsorption between ZrOCMS and As(V). The maximum removal of arsenic, 97 %, was achieved at initial arsenic concentration of 200 μg/L, after 75 min at dosage of 5.0 g/L, pH?7.0 and 27?±?2 °C. For 600 μg/L concentration, the maximum Langmuir monolayer adsorption capacity was found to be 270 μg/g at 35 °C. Kinetic modelling data indicated that adsorption process followed pseudo-second-order kinetics. The mechanism is controlled by liquid film diffusion model. Thermodynamic parameter, ΔH°, was ?57.782, while the values of ΔG° were ?9.460, ?12.183, ?13.343 and ?13.905 kJ/mol at 20, 30, 35 and 40 °C, respectively, suggesting exothermic and spontaneous nature of the process. The change in entropy, ΔS°?=??0.23 kJ/mol indicated that the entropy decreased due to adsorption of arsenate ion onto the solid adsorbent. The results indicated that the reported zirconium oxide-coated marine sand (ZrOCMS) was good adsorbent with 97 % removal capacity at 200 μg/L concentration. It is interesting to note that the permissible limit of arsenic as per World Health Organization is 10 μg/L, and in real situation, this low concentration can be achieved through this adsorbent. Besides, the adsorption capacity showed that this adsorbent may be used for the removal of arsenic from any natural water resource.  相似文献   

3.
Bagasse fly ash (BFA, a sugar industrial waste) was used as low-cost adsorbent for the uptake of arsenate and arsenite species from water. The optimum conditions for the removal of both species of arsenic were as follows: pH 7.0, concentration 50.0 μg/L, contact time 50.0 min, adsorbent dose 3.0 g/L, and temperature 20.0 °C, with 95.0 and 89.5 % removal of arsenate and arsenite, respectively. The Langmuir, Freundlich, Temkin, and Dubinin–Radushkevich adsorption isotherms were used to analyze the results. The results of these models indicated single-layer uniform adsorption on heterogeneous surface. Thermodynamic parameters, i.e., ΔG°, ΔH°, and ΔS°, were also calculated. At 20.0 to 30.0 °C, the values of ΔG° lie in the range of ?4,722.75 to ?4,878.82 and ?4,308.80 to ?4,451.73 while the values of ΔH° and ΔS° were ?149.90 and ?121.07, and 15.61 and 14.29 for arsenate and arsenite, respectively, indicating that adsorption is spontaneous and exothermic. Pseudo-first-order kinetics was followed. In column experiments, the adsorption decreased as the flow rate increased with the maximum removal of 98.9 and 95.6 % for arsenate and arsenite, respectively. The bed depth service time and Yoon and Nelson models were used to analyze the experimental data. The adsorption capacity (N o) of BFA on column was 3.65 and 2.98 mg/cm3 for arsenate and arsenite, respectively. The developed system for the removal of arsenate and arsenite species is economic, rapid, and capable of working under natural conditions. It may be used for the removal of arsenic species from any contaminated water resources.  相似文献   

4.
Activated natural siderite (ANS) was used to investigate its characteristics and mechanisms of As(V) adsorption from aqueous solution. Batch tests were carried out to determine effects of contact time, initial As(V) concentration, temperature, pH, background electrolyte, and coexisting anions on As(V) adsorption. Arsenic(V) adsorption on ANS well-fitted pseudo-second-order kinetics. ANS showed a high-adsorption capacity of 2.19 mg/g estimated from Langmuir isotherm at 25 °C. Thermodynamic studies indicated that As(V) adsorption on ANS was spontaneous, favorable, and endothermic. ANS adsorbed As(V) efficiently in a relatively wide pH range between 2.0 and 10.0, although the removal efficiency was slightly higher in acidic conditions than that in basic conditions. Effects of background electrolyte and coexisting anions were not significant within the concentration ranges observed in high As groundwater. Results of XRD and Fe K-edge XANES analysis suggested ANS acted as an Fe(II)/(III) hybrid system, which was quite effective in adsorbing As from aqueous solution. There was no As redox transformation during adsorption, although Fe(II) oxidation occurred in the system. Two infrared bands at 787 and 872 cm?1 after As(V) adsorption suggested that As(V) should be predominantly adsorbed on ANS via inner-sphere bidendate binuclear surface complexes.  相似文献   

5.
Dong H  Guan X  Wang D  Li C  Yang X  Dou X 《Chemosphere》2011,85(7):1115-1121
Batch experiments were carried out to investigate the influences of H2O2/Fe(II) molar ratio, pH, sequence of pH adjustment, initial As(V) concentration, and interfering ions on As(V) removal in H2O2-Fe(II) process from synthetic acid mine drainage (AMD). The optimum H2O2/Fe(II) molar ratio was one for arsenate removal over the pH range of 4-7. Arsenate removal at pH 3 was poor even at high Fe(II) dosage due to the high solubility of Fe(III) formed in situ. With the increase of Fe(II) dosage, arsenate removal increased progressively before a plateau was reached at pH 5 as arsenate concentration varied from 0.05 to 2.0 mg L−1. However, arsenate removal was negligible at Fe/As molar ratio <3 and then experienced a striking increase before a plateau was reached at pH 7 and arsenate concentration ≥1.0 mg L−1. The co-occurring ions exerted no significant effect on arsenate removal at pH 5. The experimental results with synthetic AMD revealed that this method is highly selective for arsenate removal and the co-occurring ions either improved arsenate removal or slightly depressed arsenate removal at pH 5-7. The extended X-ray absorption fine structure (EXAFS) derived As-Fe length, 3.27-3.30 Å, indicated that arsenate was removed by forming bidentate-binuclear complexes with FeO(OH) octahydra. The economic analysis revealed that the cost of the H2O2-Fe(II) process was only 17-32% of that of conventional Fe(III) coagulation process to achieve arsenate concentration below 10 μg L−1 in treated solution. The results suggested that the H2O2-Fe(II) process is an efficient, economical, selective and practical method for arsenate removal from AMD.  相似文献   

6.
Liang J  Xu R  Jiang X  Wang Y  Zhao A  Tan W 《Chemosphere》2007,67(10):1949-1955
The effect of arsenate on Cd(II) adsorption in two variable charge soils and the desorption of Cd(II) pre-adsorbed in the presence of arsenate were studied. The batch type experiments showed, the presence of arsenate led to increase in Cd(II) adsorption and the desorption of pre-adsorbed Cd(II). Further it was observed that the extent of adsorption and desorption of Cd(II) was greatly influenced by the initial concentrations of arsenate and Cd(II), the solution pH, and the nature of the soils. In general the increase in arsenate concentration and pH favored the uptake of Cd(II). Moreover, the arsenate concentration influenced more in Hyper-Rhodic Ferralsol than Rhodic Ferralsol at least for the Cd(II) adsorption/desorption. This may be due to the content of Fe/Al oxides in these soils. The larger the content of Fe/Al oxides, the more the adsorption of arsenate by the soil, hence greater the uptake of Cd(II). It can be assumed that the enhanced Cd(II) adsorption was mainly due to the increase in net negative surface charge of the soil induced by the adsorption of arsenate, because the presence of arsenate led to the decrease in zeta potential of these soil suspensions. The increase of electrostatically adsorbed Cd(II) was responsible for the increase in the desorption of Cd(II) pre-adsorbed in the presence of arsenate.  相似文献   

7.
Red mud-modified biochar (RM-BC) has been produced to be utilized as a novel adsorbent to remove As because it can effectively combine the beneficial features of red mud (rich metal oxide composition and porous structure) and biochar (large surface area and porous structure properties). SEM-EDS and XRD analyses demonstrated that red mud had loaded successfully on the surface of biochar. With the increasing of pH in solution, arsenate (As(V)) adsorption on RM-BC decreased while arsenite (As(III)) increased. Arsenate adsorption kinetics process on RM-BC fitted the pseudo-second-order model, while that of As(III) favored the Elovich model. All sorption isotherms produced superior fits with the Langmuir model. RM-BC exhibited improved As removal capabilities, with a maximum adsorption capacity (Qmax) for As(V) of 5923 μg g?1, approximately ten times greater than that of the untreated BC (552.0 μg g?1). Furthermore, it has been indicated that the adsorption of As(V) on RM-BC may be strongly associated with iron oxides (hematite and magnetite) and aluminum oxides (gibbsite) by X-ray absorption near-edge spectroscopy (XANES), which was possibly because of surface complexation and electrostatic interactions. RM-BC may be used as a valuable adsorbent for removing As in the environment due to the waste materials being relatively abundant.  相似文献   

8.
Representative duplicate fly ash samples were obtained from the stacks of 400- and 385-MW utility boilers (Unit A and Unit B, respectively) using a modified U.S. Environmental Protection Agency (EPA) Method 17 sampling train assembly as they burned 0.9 and 0.3 wt % S residual (No. 6 fuel) oils, respectively, during routine power plant operations. Residual oil fly ash (ROFA) samples were analyzed for Ni concentrations and speciation using inductively coupled plasma-atomic emission spectroscopy, X-ray absorption fine structure (XAFS) spectroscopy, and X-ray diffraction (XRD). ROFA deionized H2O extraction residues were also analyzed for Ni speciation using XAFS and XRD. Total Ni concentrations in the ROFAs were similar, ranging from 1.3-1.5 wt%; however, stack gas Ni concentrations in the Unit A were 0.990 microg/Nm3 compared with 0.620 microg/Nm3 for Unit B because of the greater residual oil feed rates employed at Unit A to attain higher 400-MW load conditions with a lower heating value oil. Ni speciation analysis results indicated that ROFAs from Unit A contain approximately 3 wt % NiSO4 x xH2O (where x is assumed to be 6 for calculation purposes) and appoximately 4.5 wt% of a Ni-containing spinel compound, similar in composition to (Mg,Ni)(Al,Fe)2O4. ROFAs from Unit B contain on average 2 wt% NiSO4 x 6 H20 and 1.1 wt% NiO. XAFS and XRD analyses did not detect any nickel sulfide compounds, including carcinogenic nickel subsulfide (Ni3S2) (XAFS detection limit is 5% of the total Ni concentration). In addition, XAFS measurements indicated that inorganic sulfate and organic thiophene species accounted for > 97% of the total S in the ROFAs. Unit A ROFAs contained much lower thiophene proportions because cyclone-separated ROFA reinjection is employed on this unit to collect and reburn the larger carbonaceous particles.  相似文献   

9.
An attempt has been made to elucidate the effects of soil properties on arsenate adsorption by modeling the relationships between adsorption capacity and the properties of 16 Chinese soils. The model produced was validated against three Australian and three American soils. The results showed that nearly 93.8% of the variability in arsenate adsorption on the low-energy surface could be described by citrate-dithionite extractable Fe (Fe(CD)), clay content, organic matter content (OM) and dissolved organic carbon (DOC); nearly 87.6% of the variability in arsenate adsorption on the high-energy surface could be described by Fe(CD), DOC and total arsenic in soils. Fe(CD) exhibited the most important positive influence on arsenate adsorption. Oxalate extractable Al (Al(OX)), citrate-dithionite extractable Al (Al(CD)), extractable P and soil pH appeared relatively unimportant for adsorption of arsenate by soils.  相似文献   

10.
A facile one-pot process has been proposed to prepare the novel ethylenediaminetetraacetic acid (EDTA)-modified magnetite nanoparticles (EDTA-MNPs). The bared Fe3O4 magnetite nanoparticles and EDTA-MNPs were characterized using FTIR spectroscopy, TEM, VSM, and X-ray diffraction. The application of the modified magnetite nanoparticles for metal ion uptake was studied using Ni2+ as a model. The adsorption was fast and the equilibrium was established within 5 min, and the adsorption kinetics of Ni2+ onto EDTA-MNPs followed the pseudo second-order chemisorption mechanism. Maximum adsorption capacity for Ni2+ reached as high as 41.3 mg/g at pH 6. The successive adsorption–desorption studies indicated that the EDTA-MNPs kept the adsorption and desorption efficiencies constant over ten cycles. Importantly, EDTA-MNPs were able to remove nearly 100 % of Ni2+ from real water.  相似文献   

11.
Zhang FS  Itoh H 《Chemosphere》2006,65(1):125-131
Photocatalytic oxidation of arsenite and simultaneous removal of the generated arsenate from aqueous solution were investigated. The whole process was performed using an adsorbent developed by loading iron oxide and TiO2 on municipal solid waste melted slag. The loading was carried out through chemical reactions and high-temperature process. In the removal process, arsenite was first oxidized to arsenate, and then was removed by adsorption. The oxidation of arsenite was rapid, but the adsorption of the generated arsenate was slow. A concentration of 100 mg l(-1) arsenite could be entirely oxidized to arsenate within 3 h in the presence of the adsorbent and under UV-light irradiation, but the equilibrium adsorption of the generated arsenate needed 10 h. Arsenite could also be oxidized to arsenate only by UV-light, but the reaction rate was approximately 1/3 of that of the photocatalyzed reaction. Both acidic and alkaline conditions were favorable for the oxidation reaction, and the optimum pH value for the oxidation and adsorption was proposed to be around 3. To oxidize and remove original 20 mg l(-1) or 50 mg l(-1) arsenite from aqueous solution, the necessary adsorbent amount was 2 g l(-1) or 5 g l(-1), respectively. Furthermore, the surface properties of the adsorbent were examined and the oxidation mechanism of arsenite was discussed. It is believed that the adsorbent developed in this study is efficient, cost-effective and environment-friendly for application in arsenic-contaminated wastewater treatment.  相似文献   

12.
The aim of this study is to highlight the possibility of using powder magnetite adsorption-Fenton oxidation as a method for removal of azo dye acid red B (ARB) from water. The adsorption properties of magnetite powder towards ARB were studied. The oxidation of adsorbed ARB and regeneration of magnetite adsorbent at the same time by Fenton reagent (hydrogen peroxide [H2O2] + iron (II) [Fe2+]) in another treatment unit with a smaller volume was also investigated. The efficiency of Fenton oxidation of ARB was compared for the reaction carried out in solution and on magnetite. The magnetic separation method was used to recover magnetite after adsorption or regeneration. The results indicated that the adsorption rate was fast. The capacity was strongly dependent on pH and inorganic anions, and pH 3.8 was optimal for the adsorption of ARB. The adsorption can be described well using the Langmuir model. The oxidation was more efficient for ARB adsorbed on magnetite than in solution. The adsorption capacity of magnetite increased significantly after regeneration, which was the result of an increase in surface area of the adsorbent and change of elemental ratio (oxygen:iron [O:Fe]) on the surface. The maximum adsorption capacity for ARB was 32.4 mg/g adsorbent.  相似文献   

13.
The marine macroalga, Ulva lactuca, has been exposed to different concentrations of antifouling paint particles (4–200 mg L?1) in the presence of a fixed quantity of clean estuarine sediment and its photosynthetic response and accumulation of Cu and Zn monitored over a period of 2 days. An immediate (<2 h) toxic effect was elicited under all experimental conditions that was quantitatively related to the concentration of contaminated particles present. Likewise, the rate of leaching of both Cu and Zn was correlated with the concentration of paint particles added. Copper accumulation by the alga increased linearly with aqueous Cu concentration, largely through adsorption to the cell surface, but significant accumulation of Zn was not observed. Thus, in coastal environments where boat maintenance is practiced, discarded antifouling paint particles are an important source of Cu, but not Zn, to U. lactuca.  相似文献   

14.
A thin-film continuous flow-through reactor was used to investigate reactions between aqueous Cr(VI) and two iron oxides, geothite and magnetite. Delayed effluent breakthrough of Cr(VI) indicated significant uptake by both oxides. Accumulation and remobilization of Cr(VI) depends on pH and the redox properties of the surface. For geothite the surface was quickly saturated and no further adsorption observed. Chromate anion (CrO42−) exhibited Langmuir-type adsorption. For magnetite, a significant slow steady-state rate of Cr(VI) uptake was observed. We propose two different mechanisms of chromium uptake: surface complexation of Cr(VI) species on geothite, and reductive precipitation of Cr(VI) at Fe(II) sites on magnetite.  相似文献   

15.
A novel method of preconcentration of trace arsenite and arsenate by using titanium dioxide nanoparticles as adsorbent was described. The concentrations of preconcentrated arsenite and arsenate were determined by a silver diethyldithiocarbamate spectrophotometric method without desorption. Batch adsorption experiments were carried out as a function of the pH, contact time, amount of titanium dioxide nanoparticles, and solution volume. In the pH range 5 to 6, adsorption rates of arsenite and arsenate were higher than 98%. The calibration coefficient was 0.9991, and the linear range was 0 to 100 microg/L. The developed method was precise, with the relative standard deviation <5% at concentration level of 10 microg/L, with a detection limit (3sigma, n=6) of 0.44 microg/L. The accuracy of the method for total arsenic was validated by standard reference materials (SRM 3103a) (National Institute of Standards and Technology, Gaithersburg, Maryland). The method was also applied to the analysis of arsenite and arsenate in natural water samples to verify the accuracy. The recovery values remained in a narrow range, from 95 to 103%.  相似文献   

16.
Iron hydroxide supported onto porous diatomite (D-Fe) is a low-cost material with potential to remove arsenic from contaminated water due to its affinity for the arsenate ion. This affinity was tested under varying conditions of pH, contact time, iron content in D-Fe and the presence of competitive ions, silicate and phosphate. Batch and column experiments were conducted to derive adsorption isotherms and breakthrough behaviours (50 μg L?1) for an initial concentration of 1,000 μg L?1. Maximum capacity at pH 4 and 17 % iron was 18.12–40.82 mg of arsenic/g of D-Fe and at pH 4 and 10 % iron was 18.48–29.07 mg of arsenic/g of D-Fe. Adsorption decreased in the presence of phosphate and silicate ions. The difference in column adsorption behaviour between 10 % and 17 % iron was very pronounced, outweighing the impact of all other measured parameters. There was insufficient evidence of a correlation between iron content and arsenic content in isotherm experiments, suggesting that ion exchange is a negligible process occurring in arsenate adsorption using D-Fe nor is there co-precipitation of arsenate by rising iron content of the solute above saturation.  相似文献   

17.
Laboratory batch experiments were carried out to study the adsorption of arsenate on 16 Chinese soils with different physicochemical properties. Wide differences in arsenate adsorption were observed, and the Jiangxi and Hubei soils were more effective sorbents for arsenate than other soils. The Langmuir one-surface and two-surface equations were used to model the arsenate adsorption data. Except for the Jiangxi and Hubei soils, the Langmuir one-surface equation gave reasonably good fits to the arsenate adsorption data. However, the Langmuir two-surface equation generally provided a better fit than the Langmuir one-surface equation. For soils with relative high organic matter (OM), dissolved organic carbon (DOC) or extractable phosphate, the Langmuir one-surface and two-surface equations described the adsorption isotherms similarly. In contrast, for soils with relatively low contents of OM, DOC or extractable phosphate, the Langmuir two-surface equation gave the better fit to the arsenate adsorption data.  相似文献   

18.

Purpose

Arsenic, a toxic metalloid in drinking water, has become a major threat for human beings and other organisms. In the present work, attempts have been made to remove arsenate from the synthetic as well as natural water of Ballia district, India by electrocoagulation method. Efforts have also been made to optimize the various parameters such as initial arsenate concentration, pH, applied voltage, processing time, and working temperature.

Method

Electrocoagulation is a fast, inexpensive, selective, accurate, reproducible, and eco-friendly method for arsenate removal from groundwater. The present paper describes an electrocoagulation method for arsenate removal from groundwater using iron and zinc as anode and cathode, respectively.

Results

The maximum removal of arsenate was 98.8% at 2.0?mg?L?1, 7.0, 3.0?V, 10.0?min, and 30°C as arsenate concentration, pH, applied voltage, processing time, and working temperature, respectively. Relative standard deviation, coefficient of determination (r 2), and confidence limits were varied from 1.50% to 1.59%, 0.9996% to 0.9998%, and 96.0% to 99.0%, respectively. The treated water was clear, colorless, and odorless without any secondary contamination. The developed and validated method was applied for arsenate removal of two samples of groundwater of Ballia district, U.P., India, having 0.563 to 0.805?mg?L?1, arsenate concentrations.

Conclusions

The reported method is capable for the removal of arsenate completely (100% removal) from groundwater of Ballia district. There was no change in the groundwater quality after the removal of arsenate. The treated water was safe for drinking, bathing, and recreation purposes. Therefore, this method may be the choice of arsenate removal from natural groundwater.  相似文献   

19.

Purpose

Owing to the present complexity and difficulty of concentrated dye wastewater treatment, this work aimed to synthesize a reproducible waste-sorbing material for the treatment of wastewater by forming the dye-conjugating complex hybrid.

Methods

The inorganic/organic hybridization was applied to prepare the objective material by immobilizing waster dye-Mordant blue 9 (MB) with barium sulfate (BaSO4). The composition and pattern of the formed material were determined by spectrometry and characterized by SEM and XRD, and their formation process was clarified. The adsorption of cationic dye-basic blue BO (BB) and copper ion was investigated..

Results

The hybrid of MB alone into growing BaSO4 formed the pineapple-like particles while that of the MB/BB-conjugating complex was the rhombus material. The adsorption of BB on the MB–BaSO4 hybrid was probably attributed to ion-pair equilibrium and that of Cu2+ may result from the complexation. The treatment of dye and heavy metal wastewaters indicated that the MB hybrid material removed 99.8% BB and 97% Cu2+ and the dye-conjugating hybrid with growing BaSO4 100% MB, 99.5% BB, and 44% Cu2+.

Conclusion

The waste MB–BaSO4 hybrid material is efficient to treat cationic dye and Cu2+ wastewater. The dye-conjugating hybridization method is the first to be advanced for in situ wastewater treatment, and it showed a combined effect for the removal of both organic dyes and heavy metals.  相似文献   

20.
以可溶性淀粉为原料,在反相悬浮体系中合成N,N′-亚甲基双丙烯酰胺交联淀粉微球为载体,研究了新型吸附材料淀粉微球(cross-linked starch microsphere,CSMs)对Mn+(Cu2+、Cr3+、Pb2+)的静态吸附行为。利用扫描电镜、X射线衍射仪和红外光谱仪对微球及其吸附产物进行表征,分析讨论了3种金属原子结构,研究了吸附机理。结果表明:308K时,Cu2+、Pb2+和Cr3+的饱和吸附量分别是2.43、0.30和0.27 mmol/g,CSMs对Cu2+离子吸附能力最强,并且其通过物理吸附、配位吸附方式吸附Mn+,并得出引起微球吸附能力大小可能与金属离子电荷、离子半径和外层电子排布的差异因素有关。  相似文献   

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