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1.
To determine the relative importance of the physical and chemical factors that influence the movement of heavy metals through soils, leaching experiments were carried out under conditions of constant molarity during unsaturated steady-state water flow through a Manawatu fine sandy loam (a Dystric Fluventic Eutochrept). The movement and exchange of copper was studied in a binary Cu-Ca system. The movement of the associated anions, namely chloride and sulfate, was also monitored. The measurements were compared with predictions from the convection-dispersion equation (CDE), linked with cation exchange theory. The agreement between the measured and predicted breakthrough of sulfate and copper was good. This indicates that copper retardation in the Manawatu soil is closely related to the cation exchange capacity, and that exchange between Ca and Cu is the main process of Cu retardation in the Manawatu soil. However, copper appeared slightly later in the effluent than predicted, indicating that non-exchange processes are also involved in copper transport. Measurements of suction cups could also be used to obtain the parameters for the CDE to describe sulfate movement through the soil. Time domain reflectometry (TDR) measurements of the bulk-soil electrical conductivity could be used to monitor the movement of both sulfate and copper. This indicates that TDR can also be used to monitor cation transport and exchange through the soil, provided the percolating solution causes a sufficient change in the electrical conductivity.  相似文献   

2.
利用厌氧颗粒污泥对烟气中SO2吸收生成的硫酸盐或亚硫酸盐废水进行处理,考察起始SO4^2-质量浓度、初始COD/SO4^2-、初始pH、接种污泥质量、亚铁离子等限制性生态因子对硫酸盐还原的影响。结果表明:在起始SO4^2-质量浓度800mg/L,初始COD/SO4^2-为3.0,pH值为7.0,接种污泥质量为31.10gVSS/L,添加亚铁离子的条件下,进行半连续试验,硫酸根去除率可迭70%。表明在COD/SO4^2-较低的条件下,各生态因子综合作用下,硫酸盐还原可得较好效果。  相似文献   

3.
This study investigated the interaction between microbial growth and cell elution, and their influence on resultant microbial distribution between the aqueous and solid phases during solute transport in a sandy, low-organic-carbon-content porous medium. Miscible displacement experiments were conducted with salicylate as the model compound, and with different initial conditions (e.g., substrate concentrations and cell densities) to attain various degrees of microbial growth. For each experiment, salicylate and dissolved oxygen concentrations as well as cell densities were monitored in the column effluent. Cell densities were also measured in the porous medium at the beginning and end of each experiment. Total microbial growth was determined in two ways, one based on a cell mass balance for the system and the other based on total amount of salicylate degraded. For conditions yielding a considerable amount of microbial growth, the majority of the biomass was associated with the aqueous phase (68-90%). Conversely, under minimal-growth conditions, most cells (approximately 60-70%) were attached to particle surfaces. Significant cell elution was observed for most conditions, the rate of which increased in the presence of the substrate. The results suggest that the increase in aqueous-phase cells observed for the experiments exhibiting the greatest growth is associated with the production of new cells, and that under appropriate conditions aqueous-phase biomass can contribute significantly to contaminant biodegradation.  相似文献   

4.
If volatile organoselenides are to be analyzed for their stable Se isotope composition to elucidate sources and formation processes, organoselenides need to be trapped quantitatively to avoid artificial Se isotope fractionation. We developed an efficient trap of organoselenides to be used in microcosms designed to determine the Se isotope fractionation by microbial transformation of inorganic Se to volatile organoselenides. The recoveries of volatilized dimethyldiselenide (DMDSe) from aqueous standard solutions by activated charcoal and alkaline peroxide solution with subsequent freeze-drying and purification via a cation exchange resin were tested. Microcosm experiments with the Se-methylating fungus in a growth medium were conducted, and tightness of the microcosm was assessed by comparing mass balances of total Se of the fungus, medium, and trapped organoselenides with the supplied Se mass. At the end of the experiment, we calculated δSe values of the whole microcosm and compared them with the δSe value of supplied Se(IV) and Se(VI). Our results demonstrated that activated charcoal cannot be used for quantitative trapping of organoselenides because generally <64% of the outgassed DMDSe were recovered. The mean recovery of Se volatilized from an aqueous DMDSe standard trapped in alkaline peroxide, in contrast, was 96 ± 11% (SD) after 2 h ( = 4). The mass balances of total Se in microcosm experiments with alkaline peroxide traps run for 11 to 15 d were 96 ± 15 and 102 ± 2.4% for Se(IV) and Se(VI) ( = 3), respectively. The mass-weighted mean δSe values for the Se(IV) and Se(VI) batch experiments were -0.31 ± 0.05‰ ( = 3) and -0.76 ± 0.07‰ ( = 3), compared with -0.20 ± 0.10‰ and -0.69 ± 0.10‰ in the supplied Se oxyanions, respectively. We conclude that the alkaline peroxide trap can reliably be used to determine the Se isotope composition of organoselenides.  相似文献   

5.
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7.
Effective and low-cost strategies for remediating chromium (Cr)-contaminated soil are needed. Chromium(VI) leaching from contaminated soil into ground water and surface water threatens water supplies and the environment. This study tested indigenous Cr(VI) microbial transformation in batch systems at 10 degrees C in the presence of various electron acceptors. The effects of carbon addition, spiked Cr(VI), and mixing highly contaminated soil with less contaminated soil were investigated. The results indicated that Cr(VI) can be biotransformed in the presence of different electron acceptors including oxygen, nitrate, sulfate, and iron. Sugar addition had the greatest effect on enhancing Cr(VI) removal. Less dissolved organic carbon (DOC) was consumed per amount of Cr(VI) transformed under anaerobic conditions [0.8-93 mg DOC/mg Cr(VI)] compared with aerobic conditions [1.4-265 mg DOC/mg Cr(VI)]. Toxicity of high concentrations (< 160 mg/L) of spiked Cr(VI) were not evident. At Cr(VI) concentrations > 40 mg/L, aerobic conditions promoted faster Cr(VI) reduction than anaerobic conditions with nitrate or sulfate present. Biotransformation of Cr(VI) in highly contaminated soil (22,000 mg Cr/kg) was facilitated by mixing with less-contaminated soil. The study results provide a framework for evaluating indigenous Cr(VI) microbial transformation and enhance the ability to develop strategies for soil treatment.  相似文献   

8.
This work reveals levels of corrosion rate and polarization behavior of carbon steel immersed in aqueous solutions of monoethanolamine (MEA) used in the absorption-based carbon dioxide (CO2) capture process for greenhouse gas reduction from industrial flue gas streams. Such information was obtained from electrochemical-based corrosion experiments under a wide range of the CO2 capture process conditions. The corrosion of carbon steel was evaluated in respect to process parameters including partial pressure of oxygen (O2), CO2 loading in solution, solution velocity, solution temperature, MEA concentration and metal surface condition. Results show that the aqueous MEA solution containing CO2 provides a favorable condition for the corrosion of carbon steel to proceed. Corrosion rate is increased by all tested process parameters. These parametric effects were explained by the electrochemical kinetic data obtained from polarization curves and by the thermodynamic data obtained from Pourbaix diagram.  相似文献   

9.
The persistence and degradation of endosulfan isomers and their primary degradation product, endosulfan-sulfate, were studied in a clay soil from cotton farms of western Queensland. Endosulfan degradation in relation to soil moisture, temperature, day and night temperature fluctuation, waterlogging and re-application were studied. The results show that the degradation rates of both endosulfan isomers were greatly affected by changes in soil water content and temperature. Under a high water content-high temperature regime the concentration of alpha-endosulfan in the soil fell rapidly during the first 4 weeks of application, followed by a prolonged period of slower rate of degradation. Alpha endosulfan showed a bi-exponential form of degradation for all water content-temperature experiments except for extremes in both these two factors. In the submerged soils (and also in low-water content, low temperature, non-submerged experiments) no such rapid initial degradation of alpha-endosulfan was observed, and a single first-order rate equation describes the data. Degradation of beta-endosulfan was significantly slower than for the alpha-isomer under all conditions studied. A half-life of more than a year was recorded for the beta-isomer when both water content and temperature were low. The degradation of beta-endosulfan showed no sign of the bi-exponential function observed for alpha-isomer, and a single first order rate equation described the data obtained for each factor studied. Endosulfan-sulfate was the major degradation product in all non-submerged experiments. Its build up in the soil very closely followed the disappearance of alpha-endosulfan. Its highest build-up was in the high water content-low temperature experiments, but its persistence was primarily influenced by soil temperature. Both alpha and beta-isomers, and endosulfan sulfate, persisted longer in the submerged soil. Re-application of endosulfan, and day and night fluctuation of temperature had contrasting effects on the degradation of the two isomers. Both factors slowed down the degradation of alpha-endosulfan and enhanced that of beta-endosulfan, but their net effect was to prolong the overall persistence of this chemical in the soil. Submerged conditions reduced the net formation of endosulfan-sulfate and enhanced its degradation rate.  相似文献   

10.
Arsenic remobilization in a shallow lake: the role of sediment resuspension   总被引:1,自引:0,他引:1  
Oxic resuspension occurs regularly in shallow lakes, yet its role as a mechanism for contaminant remobilization remains ill defined. This study investigated contaminant remobilization during sediment resuspension and determined whether changes in contaminant sediment partitioning reflected the mechanisms controlling remobilization. Arsenic-contaminated sediment from a shallow wetland was subjected to simulated resuspension under a range of differing initial pH conditions. The effect of resuspension on As partitioning was evaluated using a fractionation scheme targeting the dissolved, ion exchangeable, carbonate, organic, amorphous iron oxide, crystalline iron oxide, and apatite fractions. Rate investigations demonstrated that arsenic remobilization occurred on timescales similar to resuspension events, with concentrations reaching steady state within 24 h. The sediment also buffered slurry pH to 8.3 in experiments where the initial pH was between 4 and 10. This pH regulation was attributed to carbonate dissolution or acid-base equilibria of surface base functional groups, although iron oxide and organic matter dissolution did occur in experiments with an initial pH outside this range. Remobilization caused losses in arsenic associated with the ion exchangeable, organic, and amorphous iron fractions but changes in initial pH have a negligible effect on arsenic remobilization or partitioning within the well-buffered region. Resuspension released approximately 20% of the total sediment arsenic, although calculations indicated that a single resuspension event would not significantly change water column arsenic concentrations. While not conclusively proving the mechanisms of remobilization, fractionation gave valuable insight into the effect of sediment resuspension on contaminant remobilization.  相似文献   

11.
Soils are contaminated with potentially toxic iron-cyanide complexes by some industrial activities. The influence of sulfate on the sorption of the iron-cyanide complexes ferricyanide, [Fe(CN)6]3-, and ferrocyanide, [Fe(CN)6]4-, on goethite was investigated in batch experiments. The experiments were conducted as influenced by pH and varying sulfate/iron-cyanide complex concentration ratios. Furthermore, the desorption of iron-cyanide complexes sorbed on goethite was studied using phosphate and chloride solutions as influenced by pH and anion concentration. Over the whole pH range (pH 3.5 to 8), ferricyanide and sulfate showed similar affinities for the goethite surface. The extent of ferricyanide sorption strongly depended on sulfate concentrations and vice versa. In contrast, ferrocyanide sorption was only decreased (approximately 12%) by sulfate additions at pH 3.5. Ferricyanide was completely desorbed by 1 M chloride, ferrocyanide not at all. Unbuffered phosphate solutions (pH 8.3) desorbed both iron-cyanide complexes completely. Even in 70-fold excess, pH-adjusted phosphate solutions could not desorb ferrocyanide completely at pH 3.5. For ferricyanide we propose a sorption mechanism that is similar to the sulfate sorption mechanism, including outer-sphere and weak inner-sphere surface complexes on goethite. Ferrocyanide appears to form inner-sphere surface complexes. Additionally, we assume that ferrocyanide precipitates probably as a Berlin Blue-like phase at pH 3.5. Hence, ferrocyanide should be less mobile in the soil environment than ferricyanide or sulfate.  相似文献   

12.
The boreal forest is subject to natural and anthropogenic disturbances, but the production of greenhouse gases as a result of flooding for hydroelectric power generation has received little attention. It was hypothesized that flooded soil would result in greater CO(2) and CH(4) emissions and carbon (C) fractionation compared with non-flooded soil. To evaluate this hypothesis, soil C and nitrogen (N) dynamics, CO(2) and CH(4) mean production rates, and (13)C fractionation in laboratory incubations at 14 and 21 degrees C under non-flooded and flooded conditions and its effect on labile and recalcitrant C sources were determined. A ferro-humic Podzol was collected at three different sites at the Experimental Lakes Area, Canada, with a high (19,834 g C m(-2)), medium (18,066 g C m(-2)), and low (11,060 g C m(-2)) soil organic C (SOC) stock. Soil organic C and total N stocks (g m(-2)) and concentrations (g kg(-1)) were significantly different (p < 0.05) among soil horizons within each of the three sites. Stable isotope analysis showed a significant enrichment in delta(13)C and delta(15)N with depth and an enrichment in delta(13)C and delta(15)N with decreasing SOC and N concentration. The mean CO(2) and CH(4) production rates were greatest in soil horizons with the highest SOC stock and were significantly higher at 21 degrees C and in flooded treatments. The delta(13)C of the evolved CO(2) (delta(13)C-CO(2)) became significantly enriched with time during decomposition, and the greatest degree of fractionation occurred in the organic Litter, Fungal, and Humic forest soil horizons and in soil with a high SOC stock compared with the mineral horizon and soil with a lower SOC stock. The delta(13)C-CO(2) was significantly depleted in flooded treatments compared with non-flooded treatments.  相似文献   

13.
The understanding of the availability of a metal in soil necessitates a minimum knowledge about its speciation in the soil solution. Here, we evaluated an alternative to the use of ion exchangers for estimating the free ionic fraction of cadmium (FCd) in solution. It is based on the exchange selectivity coefficient (VK) rather than the distribution coefficient (DK) to estimate FCd. Because VK for the Cd-Ca exchange for the used Amberlite resin was independent of the solution Ca concentration (0.5-7.5 mM) and pH (range: 4.5-6), the experiment on a solution mimicking the analyzed solution to estimate VK was not necessary. The influence of variable Ca and Mg concentrations in solution on FCd was assessed in synthetic solutions containing either citrate or malate. The best way to estimate FCd seemed to treat the exchange data as if Ca was solely present. However, neither the proposed approach nor those applying DK prevent the overestimation of FCd when Ca is partly complexed in the analyzed solution. A method intending to estimate two replicates of FCd for a given, unique solution was also studied on solutions issued from sorption-desorption experiments performed on a humic podzol. It consists of two successive supplies of a known resin mass to a unique sample. Both estimates were close and not significantly different.  相似文献   

14.
To evaluate the effects of dissolved organic carbon on sorption and mobility of the insecticide imidacloprid [1-(6-chloro-3-pyridinyl) methyl-N-nitro-2-imidazolidinimine] in soils, adsorption and column experiments were performed by using a typical calcareous soil from southeastern Spain and two different types of dissolved organic carbon, that is, dissolved organic carbon extracts from a commercial peat (DOC-PE) and high-purity tannic acid (DOC-TA). The experiments were carried out from a 0.01 M CaCl2 aqueous medium at 25 degrees C. The results obtained from the sorption experiments show that the presence of both DOC-PE and DOC-TA, over a concentration range of 15 to 100 mg L(-1), produces in all cases a decreasing amount of imidacloprid adsorbed in the soil studied. From the column experiments the retardation coefficients (RC) were calculated for imidacloprid by using either 0.01 M CaCl2 aqueous solution (RC = 2.10), 0.01 M CaCl2 DOC-PE solution (RC = 1.65), or 0.01 M CaCl2 DOC-TA solution (RC = 1.87). The results indicate that mobility of imidacloprid is increased 21.4 and 11.0% in the presence of DOC-PE and DOC-TA solutions, respectively. Dissolved organic carbon reduces imidacloprid sorption by competing with the pesticide molecules for sorption sites on the soil surface, allowing enhanced leaching of imidacloprid and potentially increasing ground water contamination.  相似文献   

15.
In this research, the performance of Polyaluminium Chloride (PAC) and Polyaluminium Chloride sludge (PACS) as coagulants for acid red 119 (AR119) dye removal from aqueous solutions were compared. The sample of PACS was collected from "Baba Sheikh Ali" water treatment plant (Isfahan, Iran) where PAC is used as a coagulant in the coagulation/flocculation process. A response surface methodology was applied to evaluate the simple and combined effects of the operating variables including initial pH, coagulant dosage and initial dye concentration and to optimize the operating conditions of the treatment process. Results reveal that the optimal conditions for dye removal were initial pH 3.42, coagulant dosage of 4.55 g dried PACS/L and initial dye concentration of 140 mg/L for PACS, while the optimal initial pH, coagulant dosage and initial dye concentration for PAC were 3.8, 57 mg/L and 140 mg/L, respectively. Under these optimal values of process parameters, the dye removal efficiency of 94.1% and 95.25% was observed for PACS and PAC, respectively. Although lower amount of PAC in comparison with PACS was needed for specific dye removal, the reuse of PACS as a low-cost material can offer some advantages such as high efficiency for AR119 dye removal and economic savings on overall water and wastewater treatment plant operation costs.  相似文献   

16.
Calcium sulfite hemihydrate (CaSO(3).0.5H2O), a common byproduct of coal-fired utilities, is fairly insoluble and can decompose to release toxic SO2 under highly acidic soil conditions; however, it can also oxidize to form gypsum. The objective of this study was to examine the effects of application rate and soil pH on the oxidation of calcium sulfite under laboratory conditions. Oxidation rates measured by release of SO4-S to solution decreased with increasing application rate. Leachate SO4-S from soils amended with 1.0 to 3.0 g kg-1 CaSO3 increased over a 21 to 28 d period before reaching a plateau. At 4 g kg-1, maximum SO4-S release was delayed until Week 7. Oxidation and release of SO4-S from soil amended with 3.0 g kg-1 calcium sulfite increased markedly with decreasing soil pH. After only 3 d incubation, the concentrations of SO4-S in aqueous leachates were 77, 122, 170, 220, and 229 mg L-1 for initial soil pH values of 7.8, 6.5, 5.5, 5.1, and 4.0, respectively. At an initial soil pH value of 4.0, oxidation/dissolution did not increase much after 3 d. At higher pH values, oxidation was maximized after 21 d. These results suggest that autumn surface applications of calcium sulfite in no-till systems should permit ample time for oxidation/dissolution reactions to occur without introducing biocidal effects related to oxygen scavenging. Soil and annual crops can thus benefit from additions of soluble Ca and SO4 if calcium sulfite is applied in advance of spring planting.  相似文献   

17.
The activated sludge process can remove significant amounts of phosphorus from sewage, but the removal efficiency is usually significantly reduced by the release of phosphate back to solution during subsequent treatment steps. This research presents a study of soluble phosphate release from activated sludge with emphasis on defining the factors that affect such release and the actual release mechanisms. Laboratory units were used for experimental purposes. The experiments were designed to study the relationship between soluble phosphate release and various environmental factors such as redox potential (ORP), dissolved oxygen (DO), pH, solids concentration, solids destruction, and sulfate salt addition. The effect of substrate utilization on phosphate uptake and the relationship between uptake characteristics and subsequent phosphate release were also studied. The results show that some phosphate storage occurs during aerobic substrate utilization. Following substrate utilization, activated sludge phosphate release is directly related to the amount of biological stress the organisms are subjected to, and the mechanism of release is primarily cell lysis. The phosphate released per unit sludge under anoxic conditions is relatively constant. Under normal environmental conditions, neither ORP or pH change have a significant affect on phosphate release.  相似文献   

18.
For immobilization technologies to be successful, the use of readily available and cost advantageous amendment is important when the remediation targets vast amounts of contaminated soils. The objectives of this study were to investigate whether the byproduct-synthesized hydroxyapatite can be used as an immobilizing amendment for dissolved Pb from a shooting range soil, and to model the kinetic data collected from dissolution experiments. A soil–solution kinetic experiment was conducted under fixed pH conditions as a function of time. A Pb-contaminated soil was reacted with various hydroxyapatite amendments to determine the dissolution rate and mineral products of soil Pb. Three types of amendments used were pure hydroxyapatite (HA), and poorly crystalline hydroxyapatites synthesized from gypsum waste (CHA), and synthesized from incinerated poultry litter (PHA). The dissolved Pb concentration decreased with the addition of amendments at pH 3–7. Both CHA and PHA were more effective than HA for attenuating Pb dissolution at pH 6 and above. According to the thermodynamic calculation at pH 6, the dissolved Pb concentration for CHA and PHA treatments was predicted to be 66% and 50% lower than that of HA treatment, respectively. A better Pb immobilization effect demonstrated by CHA and PHA resulted in their greater solubility at higher pH, which may promote the formation of chloropyromorphite precipitates. Dissolution kinetics of soil Pb was adequately explained by pseudo-first order and pseudo-second order equations in acid pH ranges. According to the ion exchange model, an adequate agreement between the experimental data and regression curves was shown in the initial 40 min of the reaction process, but the accuracy of model predictability decreased thereafter. According to kinetic models and dissolution phenomena, CHA and PHA amendments had better Pb sorption capacity with rapid kinetics than pure hydroxyapatite at weak acid to neutral pH.  相似文献   

19.
Few published studies present data on relationships between fish mercury and surface or pore water sulfate concentrations, particularly on an ecosystem-wide basis. Resource managers can use these relationships to identify the sulfate conditions that contain fish with health-concerning total mercury (THg) levels and to evaluate the role of sulfate in methyl-mercury (MeHg) production. In this study, we derived relationships between THg in three fish trophic levels (mosquitofish, sunfish, and age-1 largemouth bass) and surface water sulfate from 1998 to 2009 for multiple stations across the Everglades Protection Area (EPA). Results show the relationship between sulfate and fish THg in each fish type is nonlinear and largely skewed, similar to the relationship between MeHg production and sulfate concentration in peatland sediment pore water identified by other researchers. Peak fish THg levels occurred in ~1 to 12 mg/L sulfate conditions. There was significant variability in the fish THg data, and there were several instances of high-fish THg levels in high-sulfate conditions (>30 mg/L). Health-concerning fish THg levels were present in all surface water sulfate conditions; however, most of these levels occurred in 1–20 mg/L sulfate. The data in this study, including recent studies, show consistent and identifiable areas of high- and low-fish THg across the spectrum of surface water sulfate concentration, therefore, applying an ecosystem-wide sulfur strategy may be an effective management approach as it would significantly reduce MeHg risk in the EPA.  相似文献   

20.
The physical and chemical parameters controlling the movement of atrazine (6-chloro-N2-ethyl-N4-isopropyl-l,3,5-triazine-2,4-diamine; 98.8%) and prometryn [N,N'-bis(1-methylethyl)-6-(methylthio)-l,3,5triazine-2,4-diamine; 99.5%] were investigated in columns infiltrated with treated effluent under unsaturated transient conditions and subjected to drying events at 22 or 60 degrees C followed by rewetting. Three soils varying in soil pH and texture and three solutions were used. The infiltrating solutions consisted of either a CaCl2 matrix (CC), a swine waste-derived lagoon effluent (SW), or a simulated buffer solution (SB) representative of the element composition and pH of the SW but with no dissolved organic matter. Several parameters were monitored including leachate triazine concentrations, pH, dissolved organic carbon (DOC), inorganic carbon, and flow rates. Compared with CC, application of SW and SB increased column leachate pH, enhanced dissolution of organic carbon and particle dispersion, and decreased average flow rates, which allowed for increased desorption time. The coupled effect of these processes enhanced movement of triazines in some cases, with SW generally having the greatest effect. The individual effect of increased pH was more pronounced for prometryn (pKa=4.05) versus atrazine (pKa=1.66), and most dramatic for the soil with the lowest initial pH. High-temperature drying, which simulated intensive evaporation, further enhanced the dissolution of soil organic matter and the reduction in leachate flow rates with SW and SB applications; however, the net effect under the experimental conditions employed varied with soil type. Relative to low-temperature drying, high-temperature drying in the silty clay loam-packed columns reduced pesticide migration.  相似文献   

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