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1.
Recently, nano zero-valent iron (nZVI) has emerged as an effective adsorbent for the removal of arsenic from aqueous solutions. However, its use in various applications has suffered from reactivity loss resulting in a decreased efficiency. Thus, the aim of this study was to develop an effective arsenic adsorbent as a core/shell structural nZVI/manganese oxide (or nZVI/Mn oxide) to minimize the reactivity loss of the nZVI. As the major result, the arsenic adsorption capacities of the nZVI/Mn oxide for As(V) and As(III) were approximately two and three times higher than that of the nZVI, respectively. In addition, the As(V) removal efficiency of the nZVI/Mn oxide was maintained through 4 cycles of regeneration whereas that of the nZVI was decreased significantly. The enhanced reactivity and reusability of the nZVI/Mn oxide can be successfully explained by the synergistic interaction of the nZVI core and manganese oxide shell, in which the manganese oxides participate in oxidation reactions with corroded Fe2+ and subsequently retard the release of aqueous iron providing additional surface sites for arsenic adsorption. In summary, this study reports the successful fabrication of a core/shell nZVI/Mn oxide as an effective adsorbent for the removal of arsenic from aqueous solutions.  相似文献   

2.
A study was conducted to explore some of the basic processes of polychlorinated biphenyl (PCB) destruction by a new technology termed electrochemical peroxidation process (ECP). ECP represents an enhancement of the classic Fenton reaction (H2O2 + Fe2+) in which iron is electrochemically generated by steel electrodes. Focus was on the extent of adsorption of a mixture of Aroclor 1248 on steel electrodes in comparison to iron filings. Commercially available zero-valent iron filings rapidly adsorbed PCBs from an aqueous solution of Aroclor 1248. Within 4 h, all the PCBs were adsorbed at 1%, 5%, and 10% Fe0 (w/v) concentrations. Little difference in adsorption was found between acidic (2.3) and unamended solutions (pH 5.5), even though significant differences in iron oxidation state and Fe2+ concentrations were measured in solution. PCB adsorption also occurs on steel electrodes regardless of the pH or electric current applied (AC or DC), suggesting the combination of oxidizing (free radical-mediated reactions) and reducing (dechlorination reactions) iron-mediated degradation pathways may be possible. Extraction of the iron powder after 48 h of contact time yielded the progressive recovery of biphenyl with increasing Fe mass(from 0.4% to 3.5%) and changes of the PCB congener-specific pattern as a consequence of dechlorination. A variety of daughter congeners similar to those accumulated during anaerobic microbial dechlorination of Aroclor 1248 in contaminated sediments indicate preferential removal of meta- and para-chlorines.  相似文献   

3.
改性沸石处理高铁锰地下水   总被引:3,自引:1,他引:2  
采用不同方法对天然沸石改性,并用改性后沸石进行了静态和动态除铁锰实验。结果表明,采用NaCl、HCl、微波方法对沸石改性,以NaCl改性效果最好。经浓度为25%的NaCl改性后的沸石铁去除率提高了13.81%,锰去除率提高了26.4%。沸石改性可以同步提高其除铁、除锰效果,且除锰效果提高更多。铁或锰的存在都能使对方单一被沸石吸附效果下降。用沸石滤柱处理高铁锰地下水,在停留时间1.0 h时,铁最高去除率为62.3%,锰最高去除率为58.3%。  相似文献   

4.
Two types of nano-pore substrates, waste-reclaimed (WR) and soil mineral (SM) with the relatively low density, were modified by the reaction with irons (i.e. Fe(II):Fe(III) = 1:2) and the applicability of the modified substrates (i.e. Fe-WR and Fe-SM) on cyanide removal was investigated. Modification (i.e. Fe immobilization on substrate) decreased the BET surface area and PZC of the original substrates while it increased the pore diameter and the cation exchange capacity (CEC) of them. XRD analysis identified that maghemite (γ-Fe2O3) and iron silicate composite ((Mg, Fe)SiO3) existed on Fe-WR, while clinoferrosilite (FeSiO3) was identified on Fe-SM. Cyanide adsorption showed that WR adsorbed cyanide more favorably than SM. The adsorption ability of both original substrates was enhanced by the modification, which increased the negative charges of the surfaces. Without the pH adjustment, cyanide was removed as much as 97% by the only application of Fe-WR, but the undesirable transfer to hydrogen cyanide was possible because the pH was dropped to around 7.5. With a constant pH of 12, only 54% of cyanide was adsorbed on Fe-WR. On the other hand, the pH was kept as 12 without adjustment in Fe-WR/H2O2 system and cyanide was effectively removed by not only adsorption but also the catalytic oxidation. The observed first-order rate constant (kobs) for cyanide removal were 0.49 (±0.081) h−1. Moreover, the more cyanate production with the modified substrates indicated the iron composites, especially maghemite, on substrates had the catalytic property to increase the reactivity of H2O2.  相似文献   

5.
《Chemosphere》2013,90(11):1450-1456
Two types of nano-pore substrates, waste-reclaimed (WR) and soil mineral (SM) with the relatively low density, were modified by the reaction with irons (i.e. Fe(II):Fe(III) = 1:2) and the applicability of the modified substrates (i.e. Fe-WR and Fe-SM) on cyanide removal was investigated. Modification (i.e. Fe immobilization on substrate) decreased the BET surface area and PZC of the original substrates while it increased the pore diameter and the cation exchange capacity (CEC) of them. XRD analysis identified that maghemite (γ-Fe2O3) and iron silicate composite ((Mg, Fe)SiO3) existed on Fe-WR, while clinoferrosilite (FeSiO3) was identified on Fe-SM. Cyanide adsorption showed that WR adsorbed cyanide more favorably than SM. The adsorption ability of both original substrates was enhanced by the modification, which increased the negative charges of the surfaces. Without the pH adjustment, cyanide was removed as much as 97% by the only application of Fe-WR, but the undesirable transfer to hydrogen cyanide was possible because the pH was dropped to around 7.5. With a constant pH of 12, only 54% of cyanide was adsorbed on Fe-WR. On the other hand, the pH was kept as 12 without adjustment in Fe-WR/H2O2 system and cyanide was effectively removed by not only adsorption but also the catalytic oxidation. The observed first-order rate constant (kobs) for cyanide removal were 0.49 (±0.081) h−1. Moreover, the more cyanate production with the modified substrates indicated the iron composites, especially maghemite, on substrates had the catalytic property to increase the reactivity of H2O2.  相似文献   

6.
A batch adsorption process was applied to investigate the removal of manganese from aqueous solution by oxidized multiwalled carbon nanotubes (MWCNTs). In doing so, the thermodynamic, adsorption isotherm, and kinetic studies were also carried out. MWCNT with 5–10-nm outer diameter, surface area of 40–600 m2/g, and purity above 95 % was used as an adsorbent. A systematic study of the adsorption process was performed by varying pH, ionic strength, and temperature. Manganese-adsorbed MWCNT was characterized by Raman, FTIR, X-ray diffraction, XPS, SEM, and TEM. The adsorption efficiency could reach 96.82 %, suggesting that MWCNT is an excellent adsorbent for manganese removal from water. The results indicate that second-order kinetics model was well suitable to model the kinetic adsorption of manganese. Equilibrium data were well described by the typical Langmuir adsorption isotherm. Thermodynamic studies revealed that the adsorption reaction was spontaneous and endothermic process. The experimental results showed that MWCNT is an excellent manganese adsorbent. The MWCNTs removed the manganese present in the water and reduced it to a permissible level making it drinkable.  相似文献   

7.
The combination of zero-valent iron (Fe0) and iron oxide-coated sand (IOCS) was used to remove Cr(VI) and As(V) from groundwater in this study. The efficiency and the removal mechanism of Cr(VI) and As(V) by using this combination, with the influence of humic acid (HA), were investigated using batch experiments. Results showed that, compared to using Fe0 or IOCS alone, the Fe0-IOCS can perform better on the removal of both Cr(VI) and As(V). Metal extraction studies showed that As(V) was mainly removed by IOCS and iron corrosion products while Cr(VI) was mainly removed by Fe0 and its corrosion products. Competition was found between Cr(VI) and As(V) for the adsorption sites on the iron corrosion products. HA had shown insignificant effects on Cr(VI) removal but some effects on As(V) removal kinetics. As(V) was adsorbed on IOCS at the earlier stage, but adsorbed/coprecipitated with the iron corrosion products at the later stage.  相似文献   

8.
Three treatment cells were operated at a site near Durango, CO. One treatment cell operated for more than 3 years. The treatment cells were used for passive removal of contamination from groundwater at a uranium mill tailings repository site. Zero-valent iron [Fe(0)] that had been powdered, bound with aluminosilicate and molded into plates was used as a reactive material in one treatment cell. The others used granular Fe(0) and steel wool. The treatment cells significantly reduced concentrations of As, Mn, Mo, Se, U, V and Zn in groundwater that flowed through it. Zero-valent iron [Fe(0)], magnetite (Fe3O4), calcite (CaCO3), goethite (FeOOH) and mixtures of contaminant-bearing phases were identified in the solid fraction of one treatment cell. A reaction progress approach was used to model chemical evolution of water chemistry as it reacted with the Fe(0). Precipitation of calcite, ferrous hydroxide [Fe(OH)2] and ferrous sulfide (FeS) were used to simulate observed changes in major-ion aqueous chemistry. The amount of reaction progress differed for each treatment cell. Changes in contaminant concentrations were consistent with precipitation of reduced oxides (UO2, V2O3), sulfides (As2S3, ZnS), iron minerals (FeSe2, FeMoO4) and carbonate (MnCO3). Formation of a free gas phase and precipitation of minerals contributed to loss of hydraulic conductivity in one treatment cell.  相似文献   

9.
Xu X  Zhou H  Zhou M 《Chemosphere》2006,62(5):847-852
Chemical treatment of para-nitrochlorobenzene (p-NCB) by palladium/iron (Pd/Fe) bimetallic particles represents one of the latest innovative technologies for the remediation of contaminated soil and groundwater. The amination and dechlorination reaction is believed to take place predominantly on the surface site of the Pd/Fe catalysts. The p-NCB was first transformed to p-chloroaniline (p-CAN) then quickly reduced to aniline. 100% of p-NCB was removed in 30 min when bimetallic Pd/Fe particles with 0.03% Pd at the Pd/Fe mass concentration of 3g 75 ml(-1) were used. The p-NCB removal efficiency and the subsequent dechlorination rate increased with the increase of bulk loading of palladium and Pd/Fe. As expected, p-NCB removal efficiency increased with temperature as well. In particular, the removal efficiency of p-NCB was measured to be 67%, 79%, 80%, 90% and 100% for reaction temperature 20, 25, 30, 35 and 40 degrees C, respectively. Our results show that no other intermediates were generated besides Cl(-), p-CAN and aniline during the catalytic amination and dechlorination of p-NCB.  相似文献   

10.
Removal of arsenic from water by electrocoagulation   总被引:16,自引:0,他引:16  
In the present study electrocoagulation (EC) has been evaluated as a treatment technology for arsenite [As(III)] and arsenate [As(V)] removal from water. Laboratory scale experiments were conducted with three electrode materials namely, iron, aluminum and titanium to assess their efficiency. Arsenic removal obtained was highest with iron electrodes. EC was able to bring down aqueous phase arsenic concentration to less than 10 microgl(-1) with iron electrodes. Current density was varied from 0.65 to 1.53 mAcm(-2) and it was observed that higher current density achieved rapid arsenic removal. Experimental results at different current densities indicated that arsenic removal was normalized with respect to total charge passed and therefore charge density has been used to compare the results. Effect of pH on arsenic removal was not significant in the pH range 6-8. Comparative evaluation of As(III) and As(V) removal by chemical coagulation (with ferric chloride) and electrocoagulation has been done. The comparison revealed that EC has better removal efficiency for As(III), whereas As(V) removal by both processes was nearly same. The removal mechanism of As(III) by EC seems to be oxidation of As(III) to As(V) and subsequent removal by adsorption/complexation with metal hydroxides generated in the process.  相似文献   

11.
A combined chemical and biological treatment scheme was evaluated in this study aiming at obtaining the simultaneous removal of metalloid arsenic and cationic heavy metals from contaminated soils. The treatment involved the use of the iron reducing microorganism Desulfuromonas palmitatis, whose activity was combined with the chelating strength of EDTA. Taking into consideration that soil iron oxides are the main scavengers of As, treatment with iron reducing microorganisms aimed at inducing the reductive dissolution of soil oxides and thus obtaining the release of the retained As. The main objective of using EDTA was the removal of metal contaminants, such as Pb and Zn, through the formation of soluble metal chelates. Experimental results however indicated that EDTA was also indispensable for the biological reduction of Fe(III) oxides. The bacterial activity was found to have a pronounced positive effect on the removal of arsenic, which increased from the value of 35% obtained during the pure chemical treatment up to 90% in the presence of D. palmitatis. In the case of Pb, the major part, i.e. approximately 85%, was removed from soil with purely chemical mechanisms, whereas the biological activity slightly improved the extraction, increasing the final removal up to 90%. Co-treatment had negative effect only for Zn, whose removal was reduced from 80% under abiotic condition to approximately 50% in the presence of bacteria.  相似文献   

12.
Hsia T. H.  S. L. Lo  C. F. Lin 《Chemosphere》1992,25(12):1825-1837
The adsorption of As(V) by amorphous iron oxide was investigated at 25°C, 0.01 M NaNO3 background electrolyte as a function of solution pH(4–10) at three initial As(V) concentrations and two Fe(III) concentrations. As(V) adsorption increased with decreasing pH. A modified Langmuir isotherm has been used for describing an equilibrium partition existing between solid and liquid phases. The triple-layer model was used for simulating As(V) adsorption on iron oxide surface. This model was able to describe As(V) adsorption over the pH range 4–10, all at the concentrations of As(V) and Fe(III) studied. =Fe(H2AsO4)0, = Fe(HAsO4) and = Fe(AsO4)2− have been shown through simulation with inner-sphere complexation products to be more consistent with experimental adsorption observations than complexation with other surface species.  相似文献   

13.
Iron oxide-loaded slag for arsenic removal from aqueous system   总被引:5,自引:0,他引:5  
Zhang FS  Itoh H 《Chemosphere》2005,60(3):319-325
An effective adsorbent for arsenic removal from aqueous system was synthesized by loading iron(III) oxide on municipal solid waste incinerator melted slag. The loading was accomplished via chemical processes and thermal coating technique. The key point of the technique was the simultaneous generation of amorphous FeOOH sol and silica sol in-situ and eventually led to the formation of Fe-Si surface complexes which combined the iron oxide with the melted slag tightly. The surface morphology of the iron oxide-loaded slag was examined and the loading mechanisms were discussed in detail. The adsorbent was effective for both arsenate and arsenite removal and its removal capabilities for As(V) and As(III) were 2.5 and 3 times of those of FeOOH, respectively. Both affinity adsorption and chemical reactions contributed to arsenic removal. The effects of solution pH, contact time, arsenic concentration and adsorbent dosage on arsenic removal were examined and the optimum removal conditions were established. Furthermore, leaching of hazardous elements such as Cr(VI), As, Se, Cd and Pb from the adsorbent at a pH range of 2.5-12.5 was below the regulation values. Accordingly, it is believed that the iron oxide-loaded slag developed in this study is environmentally acceptable and industrially applicable for wastewater treatment.  相似文献   

14.
The contamination of fresh water with pharmaceutical and personal care products (PPCPs) has risen during the last few years. The adsorption of some PPCPs namely, Diclofenac-Na, Naproxen, Gemfibrozil and Ibuprofen from aqueous solution has been studied, magnetic nanoparticles coated zeolite (MNCZ) has been used as the adsorbent. Batch adsorption experiment was conducted to study the influences of different adsorption parameters such as contact time, solution pH and PPCPs concentrations in order to optimize the reaction conditions. The removal was favored at low pH values. Thus, as pH turns from acidic to basic conditions these compounds were less efficiently removed. The initial concentration does not appear to exert a noticeable effect on the removal efficiency of the studied PPCPs at low concentrations, but it showed less removal efficiency during high concentration of PPCPs especially for Ibuprofen. The removal of Diclofenac-Na was independent on time, while the contact time was of significant effect on the adsorption of Naproxen, Gemfibrozil and Ibuprofen even though these compounds were removed up to 95% during 10 min using MNCZ. From the isotherm adsorption study, the adsorption of PPCPs studied on MNCZ was best fitted with Freundlich isotherm equation. Pseudo-second order model providing the best fit model with the experimental data. Column adsorption study was conducted to compare the removal efficiency of MNCZ with other processes used at drinking water treatment plants (DWTPs), MNCZ showed high removal efficiency (>99%) than other used processes at DWTPs.  相似文献   

15.
Remediating dicamba-contaminated water with zerovalent iron   总被引:1,自引:0,他引:1  
Dicamba (3,6-dichloro-2-methoxybenzoicacid) is a highly mobile pre- and post-emergence herbicide that has been detected in ground water. We determined the potential of zerovalent iron (Fe0) to remediate water contaminated with dicamba and its common biological degradation product, 3,6-dichlorosalicylic acid (DCSA). Mixing an aqueous solution of 100 microM dicamba with 1.5% Fe0 (w/v) resulted in 80% loss of dicamba within 12 h. Solvent extraction of the Fe0 revealed that dicamba removal was primarily through adsorption; however when the Fe0 was augmented with Al or Fe(III) salts, dicamba was dechlorinated to an unidentified degradation product. In contrast to dicamba, Fe0 treatment of DCSA resulted in removal with some dechlorination observed. When DCSA was treated with Fe0 plus Al or Fe(III) salts, destruction was 100%. Extracts of this Fe0 treatment contained the same HPLC degradation peak observed with the Fe0 + Al or Fe(III) salt treatment of dicamba. Molecular modeling suggests that differences in removal and dechlorination rates between dicamba and DCSA may be related to the type of coordination complex formed on the iron surface. Experiments with 14C-labeled dicamba confirmed that Fe-adsorbed dicamba residues are available for subsequent biological mineralization (11% after 125 d). These results indicate that Fe0 could be potentially used to treat dicamba and DCSA-contaminated water.  相似文献   

16.
Bio-reduction of arsenate using a hydrogen-based membrane biofilm reactor   总被引:1,自引:0,他引:1  
Chung J  Li X  Rittmann BE 《Chemosphere》2006,65(1):24-34
Arsenate (As(V)) is a carcinogen and a significant problem in groundwater in many parts of the world. Since As(III) is generally more mobile and more toxic than As(V), the reduction of As(V) to As(III) is not a conventional treatment goal. However, reducing As(V) to As(III) may still be a means for decontamination, because As(III) can be removed from solution by precipitation or complexation with sulfide or by adsorption to Fe(II)-based solids. A promising approach for reducing oxidized contaminants is the H2-based membrane biofilm reactor (MBfR). In the case of arsenate, the MBfR allows bio-reduction of As(V) to As(III) and sulfate to sulfide, thereby giving the potential for As removal, such as by precipitation of As2S3(s) or formation of Fe(II)-based solids. When As(V) was added to a denitrifying MBfR, As(V) was reduced immediately to As(III). Decreasing the influent sulfate loading increased As(V) reduction for a fixed H2 pressure. A series of short-term experiments elaborated on how As(V) loading, nitrate and sulfate loadings, and H2 pressure controlled As(V) reduction. Lower nitrate loading and increased As(V) loading increased the extent of As(V) reduction, but increased H2 pressure did not increase As(V) reduction. As(V) reduction was sensitive to sulfate loading, with a maximum As(V)-removal percentage and flux with no addition of sulfate. As(III) could be precipitated with sulfide or adsorbed to Fe(II) solids, which was verified by scanning electron microscopy and energy dispersive X-ray analysis.  相似文献   

17.
The present work investigates the impacts and mechanisms associated with natural organic matter (NOM) in the Fe0 treatment system of Cu2+ and Zn2+ under roof runoff conditions. The NOM in runoff waters was characterized using XAD-4/8 adsorption resins, copper complexation, acidic capacity and liquid chromatography with online carbon detection. Batch kinetic experiments and flow-through configurations were performed and the results of metal removal were elucidated taking into account the characteristics of NOM. Based on the findings, it is shown that NOM influences the removal of metals through several complex pathways. At an un-favored condition for adsorption of metals, i.e., on iron corrosion products, at pH相似文献   

18.
Chemical reaction between nitric oxide (NO) andzero valent iron (ZVI) was studied in a packed-bed column process with high temperatures based on ZVI strong reducing abilities. For six controlled temperatures of 523-773 K and 400 ppm of NO (typical flue gas temperature and concentration), under short empty bed contacttime ([EBCT] 0.0226-0.0679 sec), NO was completely removed for temperature of 573-773 K but not for 523 K. Break-through curves were conducted for the five working temperatures, and the results indicated that NO reductions by ZVI were varied from 2 to 26.7 mg NO/g ZVI. Higher temperature and longer EBCT achieved better NO removal efficiency. X-ray diffraction (XRD) and electron spectroscopy for chemical analysis (ESCA) were conducted to analyze the crystal structure and oxidation state of the reacted ZVI. Three layers of iron species were detected by XRD: ZVI, Fe3O4, and Fe2O3. ZVI was the most prevalent species, and Fe3O4 and Fe2O3 were less from the XRD analysis. By ESCA, the oxidation state on the reacted ZVI surface was determined, and the species was identifled as Fe2O3, which is the most oxidizing species for iron. Therefore, three layers from the ZVI core to the ZVI surface can be identified: ZVI, Fe3O4, and Fe2O3. Combining the results from XRD and ESCA, the mechanisms for ZVI and NO can be proposed as two consecutive reactions from lower oxidation state (ZVI) in the core to higher oxidation state on the iron surface (Fe2O3): 3Fe + 4NO<--(high temperature)-->Fe3O4 + 2N2 (A1), 4Fe3O4 + 2NO<--(high temperature)-->6Fe2O3 + N2* (A2) Because there was only <5% ZVI used to remove NO comparing to theoretical ZVI used based on the proposed stoichiometry, it can be concluded that the heterogeneous reaction only occurred on the ZVI surface instead of on bulk of the ZVI.  相似文献   

19.
Mak MS  Lo IM 《Chemosphere》2011,84(2):234-240
This study investigated the removal kinetics and mechanisms of Cr(VI) and As(V) by Fe(0) in the presence of fulvic acid (FA) and humic acid (HA) by means of batch experiments. The focus was on the involvements of FA and HA in redox reactions, metal complexation, and iron corrosion product aggregation in the removal of Cr(VI) and As(V) removal by Fe(0). Synthetic groundwater was used as the background electrolyte to simulate typical groundwater. The results showed faster Cr(VI) removal in the presence of HA compared to FA. Fluorescence spectroscopy revealed that no redox reaction occurred in the FA and HA. The results of the speciation modeling indicate that the free Fe(II) concentration was higher in the presence of HA, resulting in a higher removal rate of Cr(VI). However, the removal of As(V) was inhibited in the HA solution. Speciation modeling showed that the concentration of dissolved metal-natural organic matter (metal-NOM) complexes significantly affected the aggregation of the iron corrosion products which in turn affected the removal of As(V). The aggregation was found to be induced by gel-bridging of metal-NOM with the iron corrosion products. The effects of metal-NOM on the aggregation of the iron corrosion products were further confirmed by TEM studies. Larger sizes of iron corrosion products were formed in the FA solution compared to HA solution. This study can shed light on understanding the relationships between the properties of NOM (especially the content of metal-binding sites) and the removal of Cr(VI) and As(V) by Fe(0).  相似文献   

20.
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   

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