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1.
The optimization of TiO2-impregnated chitosan beads (TICB) as an arsenic adsorbent is investigated to maximize the capacity and kinetics of arsenic removal. It has been previously reported that TICB can 1) remove arsenite, 2) remove arsenate, and 3) oxidize arsenite to arsenate in the presence of UV light and oxygen. Herein, it is reported that adsorption capacity for TICB is controlled by solution pH and TiO2 loading within the bead and enhanced with exposure to UV light. Solution pH is found to be a critical parameter, whereby arsenate is effectively removed below pH 7.25 and arsenite is effectively removed below pH 9.2. A model to predict TICB capacity, based on TiO2 loading and solution pH, is presented for arsenite, arsenate, and total arsenic in the presence of UV light. The rate of removal is increased with reductions in bead size and with exposure to UV light. Phosphate is found to be a direct competitor with arsenate for adsorption sites on TICB, but other relevant common background groundwater ions do not compete with arsenate for adsorption sites. TICB can be regenerated with weak NaOH and maintain full adsorption capacity for at least three adsorption/desorption cycles.  相似文献   

2.
The toxic and carcinogenic properties of inorganic and organic arsenic species make their determination in natural water vitally important. Determination of individual inorganic and organic arsenic species is critical because the toxicology, mobility, and adsorptivity vary substantially. Several methods for the speciation of arsenic in groundwater, surface-water, and acid mine drainage sample matrices using field and laboratory techniques are presented. The methods provide quantitative determination of arsenite [As(III)], arsenate [As(V)], monomethylarsonate (MMA), dimethylarsinate (DMA), and roxarsone in 2-8 min at detection limits of less than 1 microg arsenic per liter (microg As L(-1)). All the methods use anion exchange chromatography to separate the arsenic species and inductively coupled plasma-mass spectrometry as an arsenic-specific detector. Different methods were needed because some sample matrices did not have all arsenic species present or were incompatible with particular high-performance liquid chromatography (HPLC) mobile phases. The bias and variability of the methods were evaluated using total arsenic, As(III), As(V), DMA, and MMA results from more than 100 surface-water, groundwater, and acid mine drainage samples, and reference materials. Concentrations in test samples were as much as 13,000 microg As L(-1) for As(III) and 3700 microg As L(-1) for As(V). Methylated arsenic species were less than 100 microg As L(-1) and were found only in certain surface-water samples, and roxarsone was not detected in any of the water samples tested. The distribution of inorganic arsenic species in the test samples ranged from 0% to 90% As(III). Laboratory-speciation method variability for As(III), As(V), MMA, and DMA in reagent water at 0.5 microg As L(-1) was 8-13% (n=7). Field-speciation method variability for As(III) and As(V) at 1 microg As L(-1) in reagent water was 3-4% (n=3).  相似文献   

3.
In the acid stream (pH 2.5-4.7) originating from the Carnoulès mine tailings, the acidophilic protozoan Euglena mutabilis grows with extremely high sulfate (1.9-4.9 g/l), iron (0.7-1.7 g/l) and arsenic concentrations (0.08-0.26 g/l). Strong variations in flow rate and high sulfate concentrations (up to 4.9 g/l) have been registered in early winter and might be the reason for the reduction in cell number of the protozoan from October to December 2001. No relation was established between arsenic concentration and/or speciation and abundance of the protozoan in the stream. Arsenite, which is the most toxic form, predominates in water. The oxidation of arsenite to arsenate occurred within a few days in laboratory experiments when E. mutabilis was present in Reigous Creek water and synthetic As(III)-rich culture medium. Methylated compounds (MMA, DMA) were not identified in the culture media. The protozoan bioaccumulated As in the cell (336 +/- 112 microg As/g dry wt.) as inorganic arsenite (105 +/- 52 microg As/g dry wt.) and arsenate (231 +/- 112 microg As/g dry wt.). Adsorption of As at the cell surface reached 57 mg/g dry wt. in the As(V) form for E. mutabilis grown in 250 mg/l As(III) synthetic medium. Both intracellular accumulation and adsorption at the cell surface increased for increasing As(III) concentration in the medium but the concentration factor in the cell relative to soluble As decreased.  相似文献   

4.
The effect of Zn2+ on both the kinetic and equilibrium aspects of arsenic adsorption to magnetite nanoparticles was investigated at pH 4.5-8.0. At pH 8.0, adsorption of both arsenate and arsenite to magnetite nanoparticles was significantly enhanced by the presence of small amount of Zn2+ in the solution. With less than 3 mg/L of Zn2+ added to the arsenic solution prior to the addition of magnetite nanoparticles, the percentage of arsenic removal by magnetite nanoparticles increased from 66% to over 99% for arsenate, and from 80% to 95% for arsenite from an initial concentration of ∼100 μg/L As at pH 8.0. Adsorption rate also increased significantly in the presence of Zn2+. The adsorption-enhancement effect of Zn2+ was not observed at pH 4.5-6.0, nor with ZnO nanoparticles, nor with surface-coated Zn-magnetite nanoparticles. The enhanced arsenic adsorption in the presence of Zn2+ cannot be due to reduced negative charge of the magnetite nanoparticles surface by zinc adsorption. Other cations, such as Ca2+ and Ag+, failed to enhance arsenic adsorption. Several potential mechanisms that could have caused the enhanced adsorption of arsenic have been tested and ruled out. Formation of a ternary surface complex by zinc, arsenic and magnetite nanoparticles is a possible mechanism controlling the observed zinc effect. Zinc-facilitated adsorption provides further advantage for magnetite nanoparticle-enhanced arsenic removal over conventional treatment approaches.

Synopsis

Arsenic adsorption to magnetite nanoparticles at neutral or slightly basic pH can be significantly enhanced with trace amount of Zn2+ due to the formation of a ternary complex.  相似文献   

5.
The most frequently encountered forms of organic arsenic, namely, dimethylarsinic acid, monomethylarsonic acid, arsenobetaine, arsenocholine and Roxarsone (4-hydroxy-3-nitrobenzene arsonic acid) were tested for toxicity either by using the Microtox bioassay, based on the rapid (within 15 min) fading of luminescence emitted by Vibrio fischeri marine bacteria, or by monitoring growth rate of the same bacteria for 3 days. Organic arsenic was generally found to be less toxic to these biological models than inorganic arsenic. In many cases, EC50 values for DMA, MMA or HNAA when using luminescence or growth inhibition assays could not be determined because of the low toxicity of the compounds. Nevertheless, results from the luminescence inhibition assay, which was found to be more sensitive than the growth inhibition assay, allowed to rank toxicity as follows: arsenate at pH 8>HNAA at pH 5>arsenate at pH 5>MMA at pH 5>HNAA at pH 8>DMA at pH 5. Arsenobetaine and monomethylarsonic acid were unexpectedly found to stimulate bacterial growth (hormesis effect). pH was found to have a strong influence on the observed toxicity as a consequence of the pH-induced changes in the chemical speciation of the tested molecules. In most cases it appeared that negatively charged forms were less toxic than the uncharged ones.  相似文献   

6.
Arsenic speciation in river and estuarine waters from southwest Spain   总被引:1,自引:0,他引:1  
An arsenic speciation survey was carried out in water samples from the Tinto and Odiel Rivers (southwest of Spain), as well as their common estuary. Both rivers are affected by acid mine drainage (AMD) and represent an input of heavy metals into the estuary, which also suffers from industrial water discharges. Samples were taken in December 2000 and July 2001. The arsenic species considered were arsenite (As(III)), arsenate (As(V)), monomethylarsonic (MMA) and dimethylarsinic (DMA) ions using coupled high-performance liquid chromatography-hydride generation-inductively coupled plasma-mass spectrometry (HPLC-HG-ICP-MS) for their determination. Parameters such as pH, salinity, redox potential and dissolved O2 were also measured. The results revealed that the acid mine drainage originating mainly during winter along the upper part of the Tinto River course causes high inorganic concentrations of dissolved arsenic, up to 600 microg l(-1) of As(III) and 200 microg l(-1) of As(V). In summer, As(III) levels decreased due to the diminution of the input from acid mine drainage and also because of oxidation, with a corresponding increase of As(V) level. Furthermore, the extreme acidic conditions of this river (pH 2.3-2-6) do not allow biological activity sufficient to produce significant concentrations of methylated arsenic species. The arsenic concentrations in the nearby Odiel River were always 5-10 times lower than in the Tinto River, with arsenic levels usually below 100 microg l(-1), dominated by As(V), indicating that it is less affected by acid mine drainage. The highest inorganic arsenic species concentrations were found where the river crosses a mining site, which corresponds to the highest As(III) values. Significant biological activity in this river produced methylated species that were detected along the water-course, with the highest concentrations at the lower course of the river, accounting for up to 53-61% of the total dissolved arsenic. At the common estuary formed by both rivers, only arsenate was detected in most samples at lower concentrations than in the riverine water samples. The tidal cycle showed a similar pattern of dilution of the arsenate when seawater comes into the estuary. Methylated species were not found either in summer or winter, at least at the 0.1 microg l(-1) level, possibly because of the high turbidity of the waters, producing an inhibition of the phytoplankton activity. In addition to the riverine inputs into the common estuary, industrial activity also represents an important source of arsenic as the discharge from a Cu smelter produced the highest arsenate level of all samples in estuary and also the only sample with significant arsenite concentration. Furthermore, the underlying iron-oxide-rich sediments represent an importance source of arsenic into the water column. In three nearby estuaries not affected by industrial activity or acid mine drainage, arsenic levels remained below detection limits.  相似文献   

7.
Arsenic-associated health complications are reported worldwide. Arsenic is a documented toxic element in drinking water. Removing arsenic from drinking water is widely dependent on iron-based techniques. Although inorganic arsenic has long been known to be toxic to humans, little is known about the toxic effect of the interaction between arsenic and iron. We investigated the effect of arsenic plus iron on the liver of rats. We gave rats sodium arsenite, iron, or sodium arsenite plus iron. Neither the arsenic-alone nor the iron-alone treatments altered their serum aspartate or alanine transaminase levels. However, a combination of non-toxic doses of arsenite and iron synergistically increased serum aspartate and alanine transaminase levels and lipid peroxidation in liver tissue. Therefore, we hypothesize that arsenic plus iron synergistically induces hepatic damage mediated through oxidative stress in rats. Our study indicates an important public health issue: using iron precipitants to remove arsenic from water may cause oxidative hepatic damage in humans.  相似文献   

8.
Lin TF  Wu JK 《Water research》2001,35(8):2049-2057
Equilibrium and kinetic adsorption of tri-valent (arsenite) and penta-valent (arsenate) arsenic to activated alumina is elucidated. The properties of activated alumina, including porosity, specific surface area, and skeleton density were first measured. A batch reactor with temperature control was employed to determine both adsorption capacity and adsorption kinetics for arsenite and arsenate to activated-alumina grains. The Freundlich and Langmuir isotherm equations were then used to describe the partitioning behavior for the system at different pH. A pore diffusion model, coupled with the observed Freundlich or Langmuir isotherm equations, was used to interpret an observed experimental adsorption kinetic curve for arsenite at one specific condition. The model was found to fit with the experimental data fairly well, and pore diffusion coefficients can be extracted. The model, incorporated with the interpreted pore diffusion coefficient, was then employed to predict the experimental data for arsenite and arsenate at various conditions, including different initial arsenic concentrations, grain sizes of activated alumina, and system pHs. The model predictions were found to describe the experimental data fairly well, even though the tested conditions substantially differed from one another. The agreement among the models and experimental data indicated that the adsorption and diffusion of arsenate and arsenite can be simulated by the proposed model.  相似文献   

9.
Adsorption of arsenite and arsenate on amorphous iron hydroxide   总被引:12,自引:0,他引:12  
Adsorption isotherms in solutions with ionic strengths of 0.01 at 25°C were measured over the arsenite and arsenate concentration range 10−7−10−3 M and the pH range 4–10. At low concentrations, these isotherms obeyed equations of the Langmuir type. At higher concentrations the adsorption isotherms were linear, indicating the existence of more than one type of surface site on the amorphous iron hydroxide adsorbent. Removal of arsenite and arsenate by amorphous iron hydroxide throughout the concentration range were determined as a function of pH. By careful selection of the relative concentration of arsenic and amorphous iron hydroxide and pH, removals on the order of 92% can be achieved.  相似文献   

10.
Levels of arsenic in water from Meager Creek hot springs, British Columbia, Canada, were found to be naturally elevated. Biota including microbial mats, green algae, sedge, cedar, fleabane, monkey flower, moss, mushrooms and lichens, that were expected to be impacted by the water, were analyzed for total levels of arsenic and for arsenic species. The major arsenic species extracted from all samples were arsenate and arsenite, which are toxic forms of arsenic. Additionally, small amounts of arsenosugars X and XI were detected in microbial mats and green algae, implying that cyanobacteria/bacteria, and possibly green algae are capable of synthesizing arsenosugars from arsenate. Low to trace amounts of arsenosugars X and XI were detected in lichens and the fungus Tarzetta cupularis. A large fraction (on average, greater than 50%) of arsenic was not extracted by using methanol/water (1:1) and the chemical and toxicological significance of this arsenic remains unknown.  相似文献   

11.
Cellulose and orange waste were chemically modified by means of phosphorylation. The chemically modified gels were further loaded with iron(III) in order to create a suitable chelating environment for arsenate and arsenite removal. The loading capacity for iron(III) on the gel prepared from orange waste (POW) was 1.21 mmol g−1 compared with 0.96 mmol g−1 for the gel prepared from cellulose (PC). Removal tests of arsenic with the iron(III)-loaded gel were carried out batchwise and by using a column. Arsenite removal was favored under alkaline condition for both PC and POW gels, however, the POW gel showed some removal capability even at neutral pH. On contrary, arsenate removal took place under acidic conditions at pH=2–3 and 2–6 for the PC and POW gels, respectively. Since iron(III) loading is higher on the POW gel than on the PC gel greater arsenic removal has been achieved by the POW gel compared with the PC gel. It can be concluded that the POW gel can be used for the removal and recovery of both arsenite and arsenate from arsenic contaminated wastewater.  相似文献   

12.
Arsenic speciation and distribution in an arsenic hyperaccumulating plant   总被引:31,自引:0,他引:31  
Arsenic-contaminated soil is one of the major arsenic sources for drinking water. Phytoremediation, an emerging, plant-based technology for the removal of toxic contaminants from soil and water, has been receiving renewed attention. Although a number of plants have been identified as hyperaccumulators for the phytoextraction of a variety of metals, and some have been used in field applications, no hyperaccumulator for arsenic had been previously reported until the recent discovery of Brake fern (Pteris vittata), which can hyperaccumulate arsenic from soils. This finding may open a door for phytoremediation of arsenic-contaminated soils. Speciation and distribution of arsenic in the plant can provide important information helpful to understanding the mechanisms for arsenic accumulation, translocation, and transformation. In this study, plant samples after 20 weeks of growth in an arsenic-contaminated soil were used for arsenic speciation and distribution study. A mixture of methanol/water (1:1) was used to extract arsenic compounds from the plant tissue. Recoveries of 85 to 100% were obtained for most parts of the plant (rhizomes, fiddle heads, young fronds and old fronds) except for roots, for which extraction efficiency was approximately 60%. The results of this study demonstrate the ability of Brake fern as an arsenic hyperaccumulator. It transfers arsenic rapidly from soil to aboveground biomass with only minimal arsenic concentration in the roots. The arsenic is found to be predominantly as inorganic species; and it was hypothesized that the plant uptakes arsenic as arsenate [As(V)I and arsenate was converted to arsenite [As(III)] within the plant. The mechanisms of arsenic uptake, translocation, and transformation by this plant are not known and are the objectives of our on-going research.  相似文献   

13.
Niu CH  Volesky B  Cleiman D 《Water research》2007,41(11):2473-2478
Highly toxic arsenate occurs naturally in some well water as well as in industrial wastewaters. Removal of arsenate (As(V)) by biosorption with acid-washed crab shells (AWCS) is very sensitive to solution pH. It greatly increased when the solution pH was lowered from 3.44+/-0.07 to 2.51+/-0.02, but it was reduced at pH below 1.99+/-0.01. Change of solution pH not only affected the charged functional groups on AWCS but also the speciation of arsenate in solution. Increasing ionic strength of solution negatively affected the arsenic uptake. At ionic strength 0.1M, arsenic uptake was seriously depressed. Arsenic biosorption with AWCS was mainly through arsenate binding on the amide groups in the AWCS. AWCS has a dense structure and low extent of swelling in aqueous solutions. This might prevent effective arsenate access to the functional groups in AWCS.  相似文献   

14.
The retention capacity for arsenic species of new nanomaterials based on tin(II) inorganic oxides or hybrid (inorganic and organic) materials was studied. The synthesis of a polymer-metal complex was performed with poly(acrylic acid) and tin(II) chloride. Poly(AA)-Sn(II) with 10 and 20 wt% of tin and a structure with a mol ratio tin:carboxylate group of 1:1, were characterized. These compounds with 10 and 20 wt% of tin content were used to compare the arsenic removal capability through the liquid-phase polymer-based retention, (LPR), technique. Also, tin oxide was prepared by adding alkaline solution to tin(II) chloride salt. The intermediate tin compound was studied by UV-Vis spectroscopy at different pH values and quantified by potentiometric titration. The solid structure is characterized by Fourier transformed infrared spectroscopy, X-ray diffraction, and specific area BET (N2). Removal of arsenite and arsenate species from solution by hydrolysated tin was carried out by LPR technique with ultrafiltration membranes and a fixed-bed column unsupported or supported on SiO2. In all these cases, a washing method at constant pH was applied. The arsenic retention ability depended on the class of tin compounds prepared, with a higher efficiency for arsenic being observed at basic pH for soluble complex poly(AA)-Sn(II) than that for tin hydroxide or hydrolysate of Sn+2.  相似文献   

15.
Mixed metal oxide impregnated chitosan beads (MICB) containing nanocrystalline Al2O3 and nanocrystalline TiO2 were successfully developed. This adsorbent exploits the high capacity of Al2O3 for arsenate and the photocatalytic activity of TiO2 to oxidize arsenite to arsenate, resulting in a removal capacity higher than that of either metal oxide alone. The composition of the beads was optimized for maximum arsenite removal in the presence of UV light. The mechanism of removal was investigated and a mode of action was proposed wherein TiO2 oxidizes arsenite to arsenate which is then removed from solution by Al2O3. Pseudo-second order kinetics were used to validate the proposed mechanism. MICB is a more efficient and effective adsorbent for arsenic than TiO2-impregnated chitosan beads (TICB), previously reported on, yet maintains a desirable life cycle, free of complex synthesis processes, toxic materials, and energy inputs.  相似文献   

16.
Sorption materials for arsenic removal from water: a comparative study   总被引:4,自引:0,他引:4  
Daus B  Wennrich R  Weiss H 《Water research》2004,38(12):2948-2954
Five different sorption materials were tested in parallel for the removal of arsenic from water: activated carbon (AC), zirconium-loaded activated carbon (Zr-AC), a sorption medium with the trade name 'Absorptionsmittel 3' (AM3), zero-valent iron (Fe(0)), and iron hydroxide granulates (GIH). Batch and column tests were carried out and the behavior of the two inorganic species (arsenite and arsenate) was investigated separately. The sorption kinetics of arsenate onto the materials followed the sequence Zr-AC > GIH = AM3 > Fe(0) > AC. A different sequence was obtained for arsenite (AC > Zr-AC = AM3 = GIH = Fe(0)). AC was found to enhance the oxidation reaction of arsenite in anaerobic batch experiments. The linear constants of the sorption isotherms were determined to be 377, 89 and 87 for Zr-AC, AM3 and GIH, respectively. The uptake capacities yielded from the batch experiment were about 7gl(-1) for Zr-Ac and 5gl(-1) for AM3. Column tests indicated that arsenite was completely removed. The best results were obtained with GIH, with the arsenate not eluting before 13100 pore volumes (inflow concentration 1 mg l(-1) As) which corresponds to a uptake capacity of 2.3 mg g(-1) or 3.7 g l(-1).  相似文献   

17.
Kale, lettuce, carrots and potatoes were grown in 20 experimental plots surrounding a wood preservation factory, to investigate the amount and pathways for plant uptake of arsenic and chromium. Arsenate used in the wood preservation process is converted to the more toxic arsenite by incineration of waste wood and is emitted into the atmosphere. Elevated concentrations of inorganic arsenic and chromium were found both in the test plants and in the soil around the factory. Multivariate statistical analysis of the results indicated that the dominating pathway of arsenic and chromium from the factory to the leafy vegetables grown nearby was by direct atmospheric deposition, while arsenic in the root crops originated from both the soil and the atmosphere. Consumption of vegetables grown near the source would result in an increased intake of inorganic arsenic, but the intake via the total diet was estimated to be below the provisional tolerable daily intake for inorganic arsenic established by FAO/WHO.  相似文献   

18.
Many Bangladeshi suffer from arsenic-related health concerns. Most mitigation activities focus on identifying contaminated wells and reducing the amount of arsenic ingested from well water. Food as a source of arsenic exposure has been recently documented. The objectives of this study were to measure the main types of arsenic in commonly consumed foods in Bangladesh and estimate the average daily intake (ADI) of arsenic from food and water. Total, organic and inorganic, arsenic were measured in drinking water and in cooked rice and vegetables from Bangladeshi households. The mean total arsenic level in 46 rice samples was 358 microg/kg (range: 46 to 1,110 microg/kg dry weight) and 333 microg/kg (range: 19 to 2,334 microg/kg dry weight) in 39 vegetable samples. Inorganic arsenic calculated as arsenite and arsenate made up 87% of the total arsenic measured in rice, and 96% of the total arsenic in vegetables. Total arsenic in water ranged from 200 to 500 microg/L. Using individual, self-reported data on daily consumption of rice and drinking water the total arsenic ADI was 1,176 microg (range: 419 to 2,053 microg), 14% attributable to inorganic arsenic in cooked rice. The ADI is a conservative estimate; vegetable arsenic was not included due to limitations in self-reported daily consumption amounts. Given the arsenic levels measured in food and water and consumption of these items, cooked rice and vegetables are a substantial exposure pathway for inorganic arsenic. Intervention strategies must consider all sources of dietary arsenic intake.  相似文献   

19.
Mobile arsenic species in unpolluted and polluted soils   总被引:1,自引:0,他引:1  
The fate and behaviour of total arsenic (As) and of As species in soils is of concern for the quality of drinking water. To estimate the relevance of organic As species and the mobility of different As species, we evaluated the vertical distribution of organic and inorganic As species in two uncontaminated and two contaminated upland soils. Dimethylarsinic acid (up to 6 ng As g(-1)), trimethylarsine oxide (up to 1.5 ng As g(-1)), 4 unidentified organic As species (up to 3 ng As g(-1)) and arsenobetaine (up to 15 ng As g(-1)), were detected in the forest soils. Arsenobetaine was the dominant organic As species in both unpolluted and polluted forest soils. No organic As species were detected in the contaminated grassland soil. The organic As species may account for up to 30% of the mobile fraction in the unpolluted forest floor, but never exceed 9% in the unpolluted mineral soil. Highest concentrations of organic As species were found in the forest floors. The concentrations of extractable arsenite were highest in the surface horizons of all soils and may represent up to 36% of total extractable As. The concentrations of extractable arsenate were also highest in the Oa layers in the forest soils and decreased steeply in the mineral soil. In conclusion, the investigated forest soils contain a number of organic As species. The organic As species in forest soils seem to result from throughfall and litterfall and are retained mostly in the forest floor. The relative high concentrations of extractable arsenite, one of the most toxic As species, and arsenate in the forest floor point to the risk of their transfer to surface water by superficial flow under heavy rain events.  相似文献   

20.
Arsenic removal by iron-modified activated carbon   总被引:6,自引:0,他引:6  
Iron-impregnated activated carbons have been found to be very effective in arsenic removal. Oxyanionic arsenic species such as arsenate and arsenite adsorb at the iron oxyhydroxide surface by forming complexes with the surface sites. Our goal has been to load as much iron within the carbon pores as possible while also rendering as much of the iron to be available for sorbing arsenic. Surface oxidation of carbon by HNO3/H2SO4 or by HNO3/KMnO4 increased the amount of iron that could be loaded to 7.6-8.0%; arsenic stayed below 10 ppb until 12,000 bed volumes during rapid small-scale tests (RSSCTs) using Rutland, MA groundwater (40-60 ppb arsenic, and pH of 7.6-8.0). Boehm titrations showed that surface oxidation greatly increased the concentration of carboxylic and phenolic surface groups. Iron impregnation by precipitation or iron salt evaporation was also evaluated. Iron content was increased to 9-17% with internal iron-loading, and to 33.6% with both internal and external iron loading. These iron-tailored carbons reached 25,000-34,000 bed volumes to 10 ppb arsenic breakthrough during RSSCTs. With the 33.6% iron loading, some iron peeled off.  相似文献   

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