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1.
Solidification/stabilization (S/S) of hazardous iron oxide coated cement (IOCC) spent adsorbent containing arsenic (As(III)) was investigated in the present study. Cement and lime-based S/S effectiveness was evaluated by performing semi-dynamic leach tests. The S/S effectiveness was evaluated by measuring effective diffusion coefficients (D(e)) and leachability indices (LX). It was found that though cement or lime alone were efficient in preventing arsenic leaching (D(e) being in range of 10(-10) to 10(-12) for all the matrices) from the solidified matrices, the best combination for arsenic containment in the matrix was obtained when a mixture of cement and lime was used. The LX values for all the matrices were higher than 10, suggesting that the S/S treated arsenic sludge are acceptable for "controlled utilization". Calcite formation along with precipitation and conversion into non-soluble forms (calcium arsenite, calcium hydrogen arsenate hydrates, calcium hydrogen arsenates, etc.) were found to be the responsible mechanism for low leaching of arsenic from the solidified/stabilized samples. A linear relationship between cumulative fraction (CFR) of arsenic leached and square root of leach time (R(2) ranging from 0.90 to 0.94) suggested that the diffusion is the responsible mechanism for arsenic leaching. Thus, cement and lime show effective containment of the As(III) within the matrix thus indicating S/S by cement and lime, which is also a low-cost option, as a suitable management option for the toxic As(III) sludge.  相似文献   

2.
3.
A simple and robust on-line sequential injection system based on solid phase extraction (SPE) coupled to a flow injection hydride generation atomic absorption spectrometer (FI-HGAAS) with a heated quartz tube atomizer (QTA) was developed and optimized for the determination of As(III) in groundwater without any kind of sample pretreatment. The method was based on the selective retention of inorganic As(V) that was carried out by passing the filtered original sample through a cartridge containing a chloride-form strong anion exchanger. Thus the most toxic form, inorganic As(III), was determined fast and directly by AsH(3) generation using 3.5 mol L(-1) HCl as carrier solution and 0.35% (m/v) NaBH(4) in 0.025% NaOH as the reductant. Since the uptake of As(V) should be interfered by several anions of natural occurrence in waters, the effect of Cl(-), SO(4)(2-), NO(3)(-), HPO(4)(2-), HCO(3)(-) on retention was evaluated and discussed. The total soluble inorganic arsenic concentration was determined on aliquots of filtered samples acidified with concentrated HCl and pre-reduced with 5% KI-5% C(6)H(8)O(6) solution. The concentration of As(V) was calculated by difference between the total soluble inorganic arsenic and As(III) concentrations. Detection limits (LODs) of 0.5 μg L(-1) and 0.6 μg L(-1) for As(III) and inorganic total As, respectively, were obtained for a 500 μL sample volume. The obtained limits of detection allowed testing the water quality according to the national and international regulations. The analytical recovery for water samples spiked with As(III) ranged between 98% and 106%. The sampling throughput for As(III) determination was 60 samplesh(-1). The device for groundwater sampling was especially designed for the authors. Metallic components were avoided and the contact between the sample and the atmospheric oxygen was carried to a minimum. On-field arsenic species separation was performed through the employ of a serial connection of membrane filters and anion-exchange cartridges. Advantages derived from this approach were evaluated. HPLC-ICPMS was employed to study the consistency of the analytical results.  相似文献   

4.
Recent evidence suggests that the oxidation of arsenite by zero-valent sulfur (S(0)) may produce stable aqueous arsenate species under highly reducing conditions. The speciation of arsenic (As) in reducing soils, sediments and aquifers may therefore be far more complex than previously thought. We illustrate this by presenting updated E(h)-pH diagrams of As speciation in sulfidic waters that include the most recently reported formation constants for sulfide complexes of As(III) and As(V). The results show that the stability fields of As(III) and As(V) (oxy)thioanions cover a large pH range, from pH 5 to 10. In particular, As(V)-S(-II) complexes significantly enhance the predicted solubility of As under reducing conditions. Equilibrium calculations further show that, under conditions representative of sulfidic pore waters and in the presence of solid-phase elemental sulfur, the S(0)((aq))/HS(-) couple yields a redox potential (E(h))~ 0.1 V higher than the SO(4)(2-)/HS(-) couple. S(0) may thus help stabilize aqueous As(V) not only by providing an electron acceptor for As(III) but also by contributing to a more oxidizing redox state.  相似文献   

5.
Oxidation of arsenic bearing fly ash as pretreatment before solidification.   总被引:2,自引:0,他引:2  
When a waste fly ash, containing large amounts of As(2)O(3), is solidified using cement and lime, the arsenic concentration in the leachate (extraction test DIN 38 414 S4) is determined by the solubility of CaHAsO(3) and can be lowered to a value of ca. 5 mg/l, in a saturated solution of Ca(OH)(2). One of the criteria for landfilling of hazardous waste is, however, that the arsenic concentration in the leachate must be lower than 1 mg/l. In this paper, it is shown that oxidation of the waste before solidification, whereby As(III) is oxidised to As(V) using H(2)O(2), lowers the leaching of arsenic, and other contaminants, from the solidified product. With the speciation program MINTEQA2, it is calculated that the solubility of As(V) in the presence of a pure Ca(3)(AsO(4))(2) precipitate is lower than the solubility of As(III) in the presence of a pure CaHAsO(3) precipitate. The arsenic concentration in the presence of both a Ca(OH)(2) and a Ca(3)(AsO(4))(2) precipitate can even be lowered to 0.47 mg/l (pH 12.5). The As concentration in the leachate of the extraction test on an oxidised S/S sample was indeed lowered to ca. 0.5 mg/l, which is a reduction by a factor of 10 compared to the concentration of ca. 5 mg/l, obtained in the leachate of the extraction test on a non-oxidised S/S sample. This is in very good agreement with the calculated value of 0.47 mg/l. Also, the pretreatment decreased the cumulative fraction of arsenic released over the entire test period of a semi-dynamic leach test by a factor of 7. At all times during the test, the As concentration did not exceed the norm of 1 mg/l.  相似文献   

6.
Removal of arsenic from water by zero-valent iron   总被引:8,自引:0,他引:8  
Batch and column experiments were conducted to investigate the effect of dissolved oxygen (DO) and pH on arsenic removal with zero-valent iron [Fe(0)]. Arsenic removal was dramatically affected by the DO content and the pH of the solution. Under oxic conditions, arsenate [As(V)] removal by Fe(0) filings was faster than arsenite [As(III)]. Greater than 99.8% of the As(V) was removed whereas 82.6% of the As(III) was removed at pH 6 after 9h of mixing. When the solution was purged with nitrogen gas to remove DO, less than 10% of the As(III) and As(V) was removed. High DO content and low solution pH also increased the rate of iron corrosion. The removal of arsenic by Fe(0) was attributed to adsorption by iron hydroxides generated from the oxic corrosion of Fe(0). The column results indicated that a filtration system consisting of an iron column and a sand filter could be used for treatment of arsenic in drinking water.  相似文献   

7.
Chen D  Huang C  He M  Hu B 《Journal of hazardous materials》2009,164(2-3):1146-1151
A simple and sensitive method using micro-column packed with 3-(2-aminoethylamino) propyltrimethoxysilane (AAPTS) modified ordered mesoporous silica combined with inductively coupled plasma optical emission spectrometry (ICP-OES) for the speciation of inorganic arsenic (As(III) and As(V)) has been developed. The adsorption behaviors of As(III) and As(V) on AAPTS modified ordered mesoporous silica were investigated. It was found that As(V) can be selectively adsorbed on the micro-column within pH of 3-9, while As(III) could not be retained in the studied pH range and passed through the micro-column directly. Total inorganic arsenic was extracted after the oxidation of As(III) to As(V) with 50.0 micromol L(-1) KMnO(4). The assay of As(III) was based on subtracting As(V) from total As. The effect of various parameters on the separation/preconcentration of As(III) and As(V) have been investigated and the optimal experimental conditions were established. The adsorption capacity of AAPTS modified ordered mesoporous silica for As(V) was found to be 10.3 mg g(-1). The detection limit of the method for As(V) was 0.05 microg L(-1) with an enrichment factor of 100, and the relative standard deviation (R.S.D.) was 5.7% (n=7, C=1.0 microg L(-1)). In order to validate the developed method, a certified reference material GSBZ50004-88 environmental water sample was analyzed and the determined values were in good agreement with the certified values. The proposed method was successfully applied to the speciation analysis of inorganic arsenic in natural water samples.  相似文献   

8.
Removal of As(V) and As(III) by reclaimed iron-oxide coated sands   总被引:1,自引:1,他引:0  
This paper aims at the feasibility of arsenate and arsenite removal by reclaimed iron-oxide coated sands (IOCS). Batch experiments were performed to examine the adsorption isotherm and removal performance of arsenic systems by using the IOCS. The results show that the pH(zpc) of IOCS was about 7.0 +/- 0.4, favoring the adsorption of As(V) of anion form onto the IOCS surface. As the adsorbent dosage and initial arsenic concentration were fixed, both the As(V) and As(III) removals decrease with increasing initial solution pH. Under the same initial solution pH and adsorbent dosage, the removal efficiencies of total arsenic (As(V) and As(III)) were in the order as follows: As(V)>As(V)+As(III)>As(III). Moreover, adsorption isotherms of As(V) and As(III) fit the Langmuir model satisfactorily for the four different initial pH conditions as well as for the studied range of initial arsenic concentrations. It is concluded that the reclaimed IOCS can be considered as a feasible and economical adsorbent for arsenic removal.  相似文献   

9.
Arsenic-contaminated mountain tap water supply in Ron Phibun District, Nakorn Si Thammarat Province, Thailand poses a health hazard. Arsenic was removed using a constructed wetland (CW) system, in which the treated contaminated tap water was sedimented in 3 consecutive ponds before entering into the CW ponds, containing either Cyperus spp. or Colocasia esculenta. Following 1 year of operation both plants had similar ability to remove arsenic from mountain tap water. Arsenic was mostly concentrated at the roots of both plants. Arsenic in C. esculenta leaves was allowed to leach out in freshwater for 149 days, but the level (0.05 mg L(-1)) was much lower than standard guidelines for industrial discharge. For Cyperus spp., young shoots were utilized as ornamental plants. As the sediments contained high arsenic levels, they were converted by a solidification/stabilization (S/S) system into cement-containing blocks, which after curing for 21 days produced arsenic leaching at levels that did not require a secure landfill for storage. The success of this study demonstrated that CW combined with appropriate S/S system is a suitable approach for Thailand in removing arsenic from contaminated water.  相似文献   

10.
This paper deals with the experimental investigation related to removal of arsenic from a simulated contaminated ground water by the adsorption onto Fe(3+) impregnated granular activated carbon (GAC-Fe) in presence of Fe(2+), Fe(3+), and Mn(2+). Similar study has also been done with granular activated carbon (GAC) for comparison. The effects of shaking time, pH, and temperature on the percentage removal of As(T), As(III), As(V), Fe(2+), Fe(3+), and Mn have been discussed. The shaking time for optimum removal of arsenic species has been noted as 8h for GAC-Fe and 12h for GAC, respectively. As(T) removal was less affected by the change in pH within the pH range of 2-11. Maximum removal of As(V) and As(III) was observed in the pH range of 5-7 and 9-11, respectively, for both the adsorbents. Under the experimental conditions at 30 degrees C, the optimum removal of As(T), As(III), As(V), Fe, and Mn are 95.5%, 93%, 98%, 100%, and 41%, respectively, when GAC-Fe is used. For GAC these values are 56%, 41%, 71%, 99%, and 98%. The adsorbent dose (AD) and its particle size (PS) for both GAC and GAC-Fe were 30 g/l and 125-150 mum, respectively. The initial arsenic concentration in the synthetic water sample was 200 ppb.  相似文献   

11.
Guo H  Li Y  Zhao K  Ren Y  Wei C 《Journal of hazardous materials》2011,186(2-3):1847-1854
Synthetic siderite has been used as adsorbent for As(III) removal in this study. Effects of contact time, temperature, pH, co-existing anions on As(III) adsorption were intensively investigated. Adsorption mechanisms were also studied using the X-ray absorption technique. Results show that the maximum adsorption capacity is up to 9.98 mg g(-1) at 25°C at a siderite dosage of 2 g L(-1). Adsorption kinetics agrees with the Lagergren pseudo-second order model. Arsenic(III) adsorption can be better described by Langmuir isotherm model for As(III) adsorption at 55°C, indicating that the coverage of the adsorption sites is in the form of monolayer, although Freundlich isotherm yields a better fit to the experimental data at 25, 35 and 45°C. Thermodynamic study indicates that As(III) adsorption on the synthetic siderite is spontaneous and endothermic in nature. The adsorption capacity is enhanced with the increase in reaction temperature. The adsorption is independent on solution pH between 3.0 and 9.6. The presence of NO(3)(-), SO(4)(2-), PO(4)(3-) or SiO(3)(2-) with element concentrations less than 20 mg L(-1) does not have adverse effect on As(III) adsorption. XANES spectra indicate that As mainly occurs as As(V) in the As adsorbed-materials, and the fraction of oxidized As(III) increases with the decrease in As(III) concentration. The formation of Fe hydroxide minerals (such as lepidocrocite and goethite) followed by As(III) oxidation and adsorption is shown to be the main mechanism of As(III) removal by the synthetic siderite.  相似文献   

12.
Contamination of potable groundwater with arsenic is a serious health hazard, which calls for proper treatment before its use as drinking water. The objective of the present study is to assess the effectiveness of iron oxide coated cement (IOCC) for As(III) adsorption from aqueous solution. Batch studies were conducted to study As(III) adsorption onto IOCC at ambient temperature as a function of adsorbent dose, pH, contact time, initial arsenic concentration and temperature. Kinetics reveal that the uptake of As(III) ion is very rapid and most of fixation occurs within the first 20 min of contact. The pseudo-second order rate equation successfully described the adsorption kinetics. Langmuir, Freundlich, Redlich-Peterson (R-P), and Dubinin-Radushkevich (D-R) models were used to describe the adsorption isotherms at different initial As(III) concentrations and at 30 g l(-1) fixed adsorbent dose. The maximum adsorption capacity of IOCC for As(III) determined from the Langmuir isotherm was 0.69 mg g(-1). The mean free energy of adsorption (E) calculated from the D-R isotherm was found to be 2.86 kJ mol(-1) which suggests physisorption. Thermodynamic parameters indicate an exothermic nature of adsorption and a spontaneous and favourable process. The results suggest that IOCC can be suitably used for As(III) removal from aqueous solutions.  相似文献   

13.
In this paper, a system of flow injection (FI) capillary microextraction (CME) on line coupled with inductively plasma mass spectrometry (ICP-MS) was proposed for simultaneous separation and speciation of inorganic As(III)/As(V) and Cr(III)/Cr(VI) in natural waters. Ordered mesoporous Al2O3 coating was prepared by sol-gel technology and used as CME coating material. Various experimental parameters affecting the capillary microextraction of inorganic arsenic and chromium species have been investigated and optimized. Under the optimized conditions, the limits of detection were 0.7 and 18 ng L(-1) for As(V) and Cr(VI), 3.4 and 74 ng L(-1) for As(III) and Cr(III), respectively, with an enrichment factor of 5 and a sampling frequency of 8h(-1). The relative standard deviations (R.S.D.) were 3.1, 4.0, 2.8 and 3.9% (C=1 ng mL(-1), n=7) for As(V), As(III), Cr(VI) and Cr(III), respectively. The proposed method was successfully applied for the analysis of inorganic arsenic and chromium species in mineral water, tap water and lake water with the recovery of 94-105%. In order to verify the accuracy of the method, two certified reference of GSBZ50027-94 and GSBZ50004-88 water samples were analyzed and the results obtained were in good agreement with the certified values. The ordered mesoporous Al2O3 coated capillary showed an excellent solvent and thermal stability and could be re-used for more than 30 times without decreasing extraction efficiency.  相似文献   

14.
Batch studies were conducted to examine the adsorption kinetics and adsorption capacity of iron oxide-coated biomass (IOCB) for As(III) and As(V). The optimum pH for As(V) and As(III) removal was found to be 6. The equilibrium time for removal of arsenic was found to be approximately 7 h. The adsorption of As(V) on IOCB was rapid compared to that of As(III) adsorption. An increase in temperature (from 5 to 30 °C) was found to increase As(III) removal, whereas in the case of As(V), the removal increased with temperature from 5 to 10 °C, but remained relatively constant thereafter up to 30 °C. The pseudo-second order rate equation was found to describe better the kinetics of arsenic adsorption than other equations. The isotherm data for As(V) removal fitted better with the Langmuir equation compared with other tested models and the isotherm data for As(III) removal fitted better with Redlich–Peterson equation than other tested models. Iron oxide-coated fungal biomass (A. niger) was found to be efficient in removing arsenic from an aqueous solution.  相似文献   

15.
A novel hydride generation (HG) interface for coupling capillary electrophoresis (CE) with inductively coupled plasma mass spectrometry (ICPMS) is presented in this work. The CE-HG-ICPMS interface was applied to the separation and quantitation of common arsenic species. Lack of a commercially available HG interface for CE-ICPMS led to a three concentric tube design allowing alleviation of back pressure commonly observed in CE-HG-ICPMS. Due to the high sensitivity and element-specific detection of ICPMS, quantitative analysis of As(III), As(V), monomethylarsonic acid, and dimethylarsinic acid was achieved. Optimization of CE separation conditions resulted in the use of 20 mmol L(-1) sodium borate with 2% osmotic flow modifier (pH 9.0) and -20 kV applied potential for baseline resolution of each arsenic species in the shortest time. Hydride generation conditions were optimized through multiple electrophoretic separation analyses with 5% HCl and 3% NaBH(4) (in 0.2% NaOH) determined to be the optimum conditions. After completion of system optimization, detection limits obtained for the arsenic species were less than 40 ng L(-1) with electromigration time precision less than 1% within a total analysis time of 9.0 min. Finally, the interface was used for speciation analysis of arsenic in river and tap water samples.  相似文献   

16.
Brine disposal is a serious challenge of arsenic (V) removal from drinking water using ion-exchange (IX). Although arsenic removal with ferric chloride (FeCl(3)) from drinking waters is well documented, the application of FeCl(3) to remove arsenic (V) from brines has not been thoroughly investigated. In contrast to drinking water, IX brines contain high ionic strength, high alkalinity, and high arsenic concentrations; these factors are known to influence arsenic removal by FeCl(3). Surface complexation modeling and experimental coagulation tests were performed to investigate the influence of ionic strength, pH, Fe/As molar ratios, and alkalinity on the removal of arsenic from IX brines. The model prediction was in good agreement with the experimental data. Optimum pH range was found to be between 4.5 and 6.5. The arsenic removal efficiency slightly improved with higher ionic strength. The Fe/As ratios needed to treat brines were significantly lower than those used to treat drinking waters. For arsenic (V) concentrations typical in IX brines, Fe/As molar ratios varying from 1.3 to 1.7 were needed. Sludge solid concentrations varying from 2 to 18 mg L(-1) were found. The results of this research have direct application to the treatment of residual wastes brines containing arsenic.  相似文献   

17.
Yan XP  Yin XB  He XW  Jiang Y 《Analytical chemistry》2002,74(9):2162-2166
A flow injection on-line sorption preconcentration and separation in a knotted reactor (KR) was coupled to hydride generation atomic fluorescence spectrometry (HG-AFS) for speciation of inorganic arsenic in natural water samples. The method involved on-line formation of the As(III)-pyrrolidinedithiocarbamate (PDC) complex over a sample acidity of 0.001-0.1 mol L(-1) HCl, its adsorption onto the inner walls of the KR made from 150-cm long x 0.5-mm i.d. PTFE tubing, elution withmol L(-1) HCl, and detection by HG-AFS. Total inorganic arsenic was determined after prereduction of As(V) to As(III) with 1% m/v L-cysteine. The concentration of As(V) was calculated by the difference of the total inorganic arsenic and As(III). A 1 mol L(-1) concentration of HCl was employed not only as the efficient eluent but also as the required medium for subsequent hydride generation. Potential factors that affect adsorption, rinsing, elution, and hydride generation were investigated in detail. The low cost, easy operation, and high sensitivity are the obvious advantages of the present system. With consumption of a 6 mL sample solution, an enhancement factor of 11 and a detection limit (3s) of 0.023 microg L(-1) As(III) were obtained at a sample throughput of 32 h(-1). The precision for 14 replicate measurements of 1 microg L(-1) As(III) was 1.3% (RSD). The recoveries from natural water samples varied from 96.7 to 105% for 2 microg L(-1) of As(III) spike and from 97.1 to 107% for 2 microg L(-1) of As(V) spike. The analytical results obtained by the present method for total arsenic in the certified reference materials, SLRS-4 (river water) and NASS-5 (seawater), agreed well with the certified values. The developed method was also successfully applied to the speciation of inorganic arsenic in local natural water samples.  相似文献   

18.
This paper presents the observations on the bio-removal of arsenic from contaminated water by using Ralstonia eutropha MTCC 2487 and activated carbon in a batch reactor. The effects of agitation time, pH, type of granular activated carbon (GAC) and initial arsenic concentration (As(o)) on the % removal of arsenic have been discussed. Under the experimental conditions, optimum removal was obtained at the pH of 6-7 with agitation time of 100 h. The % removal of As(T) increased initially with the increase in As(o) and after attaining the maximum removal (~86%) at the As(o) value of around 15 ppm, it started to decrease. Simultaneous adsorption bioaccumulation (SABA) was observed, when fresh GAC was used as supporting media for bacterial immobilization. In case of SABA, the % removal of As(III) was almost similar (only ~1% more) to the additive values of individual removal of As(III) obtained by only adsorption and only bio-adsorption. However, for As(V) the % removal was less (~8%) than the additive value of the individual % removals obtained by only adsorption and bio-adsorption. Percentage removal of Fe, Mn, Cu and Zn were 65.17%, 72.76%, 98.6% and 99.31%, respectively. Maximum regeneration (~99.4%) of the used bio-adsorbent was achieved by the treatment with 5NH(2)SO(4) followed by 1N NaOH and 30% H(2)O(2) in HNO(3). The fitness of the isotherms to predict the specific uptake for bio-adsorption/accumulation process has been found to decrease in the following order: Temkin isotherm>Langmuir isotherm>Freundlich isotherm. For the adsorption process with fresh GAC the corresponding order is Freundlich isotherm>Langmuir isotherm>Temkin isotherm for As(V) and As(T). However, for As(III) it was Langmuir>Temkin>Freundlich.  相似文献   

19.
Arsenic (V) is known to form heteropolyacid with ammonium molybdate in acidic aqueous solutions, which can be quantitatively extracted into certain organic solvents. In the present work, 12-molybdoarsenic acid extracted in butan-1-ol is used for quantification of As (V). Total arsenic is estimated by converting arsenic (III) to arsenic (V) by digesting samples with concentrated nitric acid before extraction. Concentration of As (III) in the sample solutions could be calculated by the difference in total arsenic and arsenic (V). The characterization of arsenic was carried out by GFAAS using Pd as modifier. Optimization of the experimental conditions and instrumental parameters was investigated in detail. Recoveries of (90-110%) were obtained in the spiked samples. The detection limit was 0.2 microg l(-1). The proposed method was successfully applied for the determination of trace amount of arsenic (III) and arsenic (V) in process water samples.  相似文献   

20.
Arsenic removal by adsorption on iron(III) phosphate   总被引:1,自引:0,他引:1  
Under natural conditions, arsenic is often associated with iron oxides and iron(III) oxidative capacity towards As(III) is well known. In this study, As(III) and As(V) removal was performed using synthesised iron(III) phosphate, either amorphous or crystalline. This solid can combine (i) As(III) oxidation by iron(III) and (ii) phosphate substitution by As(V) due to their similar properties. Results showed that adsorption capacities were higher towards As(III), leading to Fe2+ and HAsO4(2-) leaching. Solid dissolution and phosphate/arsenate exchange led to the presence of Fe3+ and PO4(3-) in solution, therefore various precipitates involving As(V) can be produced: with Fe2+ as Fe3(AsO4)2.8H2O(s) and with Fe3+ as FeAsO4.2H2O(s). Such formations have been assessed by thermodynamic calculations. This sorbent can be a potential candidate for industrial waste treatment, although the high release of phosphate and iron will exclude its application in drinking water plants.  相似文献   

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