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1.
Monitored natural attenuation (MNA) has recently emerged as a viable groundwater remediation technology in the United States. Area 6 at Dover Air Force Base (Dover, DE) was chosen as a test site to examine the potential for MNA of tetrachloroethene (PCE) and trichloroethene (TCE) in groundwater and aquifer sediments. A "lines of evidence" approach was used to document the occurrence of natural attenuation. Chlorinated hydrocarbon and biogeochemical data were used to develop a site-specific conceptual model where both anaerobic and aerobic biological processes are responsible for the destruction of PCE, TCE, and daughter metabolites. An examination of groundwater biogeochemical data showed a region of depleted dissolved oxygen with elevated dissolved methane and hydrogen concentrations. Reductive dechlorination likely dominated in the anaerobic portion of the aquifer where PCE and TCE levels were observed to decrease with a simultaneous increase in cis-1,2-dichloroethene (cis-DCE), vinyl chloride (VC), ethene, and dissolved chloride. Near the anaerobic/ aerobic interface, concentrations of cis-DCE and VC decreased to below detection limits, presumably due to aerobic biotransformation processes. Therefore, the contaminant and daughter product plumes present at the site appear to have been naturally atteuated by a combination of active anaerobic and aerobic biotransformation processes.  相似文献   

2.
A polyphasic approach based on cultivation and direct recovery of 16S rRNA gene sequences was utilized for microbial characterization of an aquifer contaminated with chlorinated ethenes. This work was conducted in order to support the evaluation of natural attenuation of chlorinated ethenes in groundwater at Area 6 at Dover Air Force Base (Dover, DE). Results from these studies demonstrated the aquifer contained relatively low biomass (e.g. direct microscopic counts of < 10(7) bacteria/g of sediment) comprised of a physiologically diverse group of microorganisms including iron reducers, acetogens, sulfate reducers, denitrifiers, aerobic and anaerobic heterotrophs. Laboratory microcosms prepared with authentic sediment and groundwater provided direct microbiological evidence that the mineralization of vinyl chloride and cis-dichloroethene as well as each step in the complete reductive dechlorination of tetracloroethene to ethene can occur in the Area 6 aquifer. Enrichment cultures capable of the oxidative degradation of cis-1,2-dichloroethene (cis-DCE) and vinyl chloride (VC) were obtained from groundwater across the aquifer demonstrating the possible importance of direct, non-cometabolic oxidation of cis-DCE and VC in natural attenuation. Culture-independent analyses based upon recovery of 16S rRNA gene sequences revealed the presence of anaerobic organisms distributed primarily between two major bacterial divisions: the delta subdivision of the Proteobacteria and low-G + C gram positive. Recovery of sequences affiliated with phylogenetic groups containing known anaerobic-halorespiring organisms such as Desulfitobacterium, Dehalobacter, and certain groups of iron reducers provided qualitative support for a role of reductive dechlorination processes in the aquifer. This molecular data is suggestive of a functional linkage between the microbiology of the site and the apparent natural attenuation process. The presence and distribution of microorganisms were found to be consistent with a microbially driven attenuation of chlorinated ethenes within the aquifer and in accord with a conceptual model of aquifer geochemistry which suggest that both reductive and oxidative mechanisms are involved in heterogeneous, spatially distributed processes across the aquifer.  相似文献   

3.
4.
A multi-dimensional and multi-species reactive transport model was developed to aid in the analysis of natural attenuation design at chlorinated solvent sites. The model can simulate several simultaneously occurring attenuation processes including aerobic and anaerobic biological degradation processes. The developed model was applied to analyze field-scale transport and biodegradation processes occurring at the Area-6 site in Dover Air Force Base, Delaware. The model was calibrated to field data collected at this site. The calibrated model reproduced the general groundwater flow patterns, and also, it successfully recreated the observed distribution of tetrachloroethene (PCE), trichloroethene (TCE), dichloroethylene (DCE), vinyl chloride (VC) and chloride plumes. Field-scale decay rates of these contaminant plumes were also estimated. The decay rates are within the range of values that were previously estimated based on lab-scale microcosm and field-scale transect analyses. Model simulation results indicated that the anaerobic degradation rate of TCE, source loading rate, and groundwater transport rate are the important model parameters. Sensitivity analysis of the model indicated that the shape and extent of the predicted TCE plume is most sensitive to transmissivity values. The total mass of the predicted TCE plume is most sensitive to TCE anaerobic degradation rates. The numerical model developed in this study is a useful engineering tool for integrating field-scale natural attenuation data within a rational modeling framework. The model results can be used for quantifying the relative importance of various simultaneously occurring natural attenuation processes.  相似文献   

5.
Heim S  Ricking M  Schwarzbauer J  Littke R 《Chemosphere》2005,61(10):1427-1438
To study the recent contamination history of DDT (1,1,1-trichloro-2,2-bis(chlorophenyl)ethane) and its metabolites, as well as methoxychlor (1,1,1-trichloro-2,2-bis(p-methoxyphenyl)ethane), chlorfenson (4-chlorophenyl-p-chlorobenzenesulfonate), and further halogenated aromatics, a sediment core was collected from the Teltow Canal in Berlin (Germany). The sampling site is located nearby a former industrial point source, where recently analyses on pre-samples have indicated high concentrations of halogenated organic compounds. The deposition time of the investigated sediments was determined by gamma-spectrometrical dating. Pollution trends of selected contaminants were attributed to a time period between 5 and 10 years. Concentration profiles reflect not only the recent pollution history of these compounds, but also the time-depending effects of the ban, restriction and termination of DDT-production in the German Democratic Republic (GDR). DDT and other chlorinated aromatic compounds were produced onsite until the late 1980s. Maximum values of 133 mg kg(-1) (dry weight) for p,p'-DDD (1,1-dichloro-2,2-bis(chlorophenyl)ethane) and approximately 100 mg kg(-1) (dry weight) for p,p'-DDMS (1-chloro-2,2-bis(chlorophenyl)ethane), main metabolites of the anaerobic degradation of DDT, were determined. The occurrence of all selected contaminants, most of which have been banned more than 10 years ago, demonstrate recent contamination pathways, and the necessity of a continuous long-term monitoring of the affected environment.  相似文献   

6.
The in situ degradation of chlorinated ethenes was assessed in an anaerobic aquifer using stable isotope fractionation approaches, microcosm studies and taxon specific detection of specific dehalogenating groups of bacteria. The aquifer in the Bitterfeld/Wolfen region in Germany contained all chlorinated ethenes, benzene and toluene as contaminants. The concentrations and isotope composition of the chlorinated ethenes indicated biodegradation of the contaminants. Microcosm studies confirmed the presence of in situ microbial communities capable of the complete dechlorination of tetrachloroethene. Taxon specific investigation of the microbial communities indicated the presence of various potential dechlorinating organisms including Dehalococcoides, Desulfuromonas, Desulfitobacterium and Dehalobacter. The integrated approach, using metabolite spectra, molecular marker analysis and isotope studies, provided several lines of evidence for natural attenuation of the chlorinated ethenes.  相似文献   

7.
A two-dimensional analytical model is employed for estimating the first-order degradation rate constant of hydrophobic organic compounds (HOCs) in contaminated groundwater under steady-state conditions. The model may utilize all aqueous concentration data collected downgradient of a source area, but does not require that any data be collected along the plume centerline. Using a least squares fit of the model to aqueous concentrations measured in monitoring wells, degradation rate constants were estimated at a former manufactured gas plant (FMGP) site in the Midwest U.S. The estimated degradation rate constants are 0.0014, 0.0034, 0.0031, 0.0019, and 0.0053 day(-1) for acenaphthene, naphthalene, benzene, ethylbenzene, and toluene, respectively. These estimated rate constants were as low as one-half those estimated with the one-dimensional (centerline) approach of Buscheck and Alcantar [Buscheck, T.E., Alcantar, C.M., 1995. Regression techniques and analytical solutions to demonstrate intrinsic bioremediation. In: Hinchee, R.E., Wilson, J.T., Downey, D.C. (Eds.), Intrinsic Bioremediation, Battelle Press, Columbus, OH, pp. 109-116] which does not account for transverse dispersivity. Varying the transverse and longitudinal dispersivity values over one order of magnitude for toluene data obtained from the FMGP site resulted in nearly a threefold variation in the estimated degradation rate constant-highlighting the importance of reliable estimates of the dispersion coefficients for obtaining reasonable estimates of the degradation rate constants. These results have significant implications for decision making and site management where overestimation of a degradation rate may result in remediation times and bioconversion factors that exceed expectations. For a complex source area or non-steady-state plume, a superposition of analytical models that incorporate longitudinal and transverse dispersion and time may be used at sites where the centerline method would not be applicable.  相似文献   

8.
Between September 5 and October 5,1989 a field demonstration of the NovaTerra, Inc. Detoxifier [formerly called Toxic Treatment (USA)] was performed by the U.S. EPA under the Superfund Innovative Technology Evaluation (SITE) program. The NovaTerra Detoxifier process injects steam and hot air directly into the ground to vaporize and strip volatile and semivolatile organics. Two augers loosen and homogenize the soil during the stripping process. The steam, hot air and organics are carried to the soil surface and collected for treatment.

The field demonstration was performed at the GATX Annex Terminal located at the Port of Los Angeles, San Pedro, California. Approximately 17 percent of the 5.2 acre site is contaminated with chlorinated solvents, plasticizers, coatings, adhesives and paint additives, and other miscellaneous chemicals from aboveground storage tanks and transfer operations to railroad cars.

The objectives of this SITE Demonstration were to determine the in situ soil concentrations before and after treatment, quantify process stream emissions (fugitive and sidestreams), determine process operating conditions, and determine if vertical migration of contaminants is occurring. Results from the SITE demonstration showed that a substantial amount of the VOCs were removed, about half the SVOCs were removed, there was very little fugitive air emissions from the operation, and what little downward migration occured (if any) was inconsequential.  相似文献   

9.
Sivey JD  Lee CM 《Chemosphere》2007,66(10):1821-1828
To assess the ca. 20-year polychlorinated biphenyl (PCB) contamination trends in Lake Hartwell, SC, sediment cores from the Twelve Mile Creek arm were collected in July 2004 at two sites (G30 and G33) first sampled in the mid-1980s. Congener-specific PCB data as a function of depth from the sediment-water interface for the 2004 sediment samples were compared to data obtained from 1987 and 1998 samples taken from the same locations. Despite modest decreases in total PCB levels near the G30 sediment-water interface, historical increases in average degrees of chlorination may elevate the overall toxic risk at this site. Unlike G30, the more rapid recovery in the near-surface sediment of G33 suggests that the effectiveness of the U.S. EPA natural attenuation record of decision is site-specific and is unlikely to result in uniform surface sediment recovery throughout the most contaminated regions of Lake Hartwell.  相似文献   

10.
For many national parks and wilderness areas with special air quality protections (Class I areas) in the western United States (U.S.), wildfire smoke and dust events can have a large impact on visibility. The U.S. Environmental Protection Agency’s (EPA) 1999 Regional Haze Rule used the 20% haziest days to track visibility changes over time even if they are dominated by smoke or dust. Visibility on the 20% haziest days has remained constant or degraded over the last 16 yr at some Class I areas despite widespread emission reductions from anthropogenic sources. To better track visibility changes specifically associated with anthropogenic pollution sources rather than natural sources, the EPA has revised the Regional Haze Rule to track visibility on the 20% most anthropogenically impaired (hereafter, most impaired) days rather than the haziest days. To support the implementation of this revised requirement, the EPA has proposed (but not finalized) a recommended metric for characterizing the anthropogenic and natural portions of the daily extinction budget at each site. This metric selects the 20% most impaired days based on these portions using a “delta deciview” approach to quantify the deciview scale impact of anthropogenic light extinction. Using this metric, sulfate and nitrate make up the majority of the anthropogenic extinction in 2015 on these days, with natural extinction largely made up of organic carbon mass in the eastern U.S. and a combination of organic carbon mass, dust components, and sea salt in the western U.S. For sites in the western U.S., the seasonality of days selected as the 20% most impaired is different than the seasonality of the 20% haziest days, with many more winter and spring days selected. Applying this new metric to the 2000–2015 period across sites representing Class I areas results in substantial changes in the calculated visibility trend for the northern Rockies and southwest U.S., but little change for the eastern U.S.

Implications: Changing the approach for tracking visibility in the Regional Haze Rule allows the EPA, states, and the public to track visibility on days when reductions in anthropogenic emissions have the greatest potential to improve the view. The calculations involved with the recommended metric can be incorporated into the routine IMPROVE (Interagency Monitoring of Protected Visual Environments) data processing, enabling rapid analysis of current and future visibility trends. Natural visibility conditions are important in the calculations for the recommended metric, necessitating the need for additional analysis and potential refinement of their values.  相似文献   


11.
This paper describes one of the first well-documented field examples of natural attenuation of trichloroethylene (TCE) in groundwater in a fractured shale bedrock. The study was carried out adjacent to a former waste burial site in Waste Area Grouping 5 (WAG5) on the Oak Ridge Reservation, Oak Ridge, TN. A contaminant plume containing TCE and its daughter products were detected downgradient from the buried waste pits, with most of the contamination occurring in the upper 6 m of the bedrock. The monitoring well array consists of a 35-m-long transect of multilevel sampling wells, situated along a line between the waste pits and a seep which discharges into a small stream. Concentrations of volatile organic carbons (VOCs) were highest in the waste trenches and decreased with distance downgradient towards the seep. Sampling wells indicated the presence of overlapping plumes of TCE, cis-dichloroethylene (cDCE), vinyl chloride (VC), ethylene, ethane, and methane, with the daughter products extending further downgradient than the parent (TCE). This type of distribution suggests anaerobic biodegradation. Measurements of redox potential at the site indicated that iron-reduction, sulfate reduction, and potentially methanogensis were occurring and are conducive to dechlorination of TCE. Bacteria enrichment of groundwater samples revealed the presence of methanotrophs, methanogens, iron-reducing bacteria and sulfate-reducing bacteria, all of which have previously been implicated in anaerobic biodegradation of TCE. 16S rDNA sequence from DNA extracted from two wells were similar to sequences of organisms previously implicated in the anaerobic biodegradation of chlorinated solvents. The combined data strongly suggest that anaerobic biodegradation of the highly chlorinated compounds is occurring. Aerobic biodegradation may also be occurring in oxygenated zones, including near a seep where groundwater exits the site, or in the upper bedrock during seasonal fluctuations in water table elevation and oxygen levels.  相似文献   

12.
在北京地区某加油站开展的前期石油类污染物自然衰减现场试验的基础上,进一步开展了验证试验,结果表明本次试验得到的挥发性有机物(VOCs)变化趋势及O2、CO2含量沿土壤深度分布和前期试验结果呈现相同的规律,说明基于自然衰减法设计实施的加油站现场试验检测分析结果可靠,试验方法具有合理性、可操作性及可重复性.进一步的理论分析对前期试验结果进行了验证,得出以下结论:(1)通过氧平衡和碳平衡计算对加油站土壤内的自然衰减方式进行评价,验证了该加油站地下土壤中实际发生的微生物降解既有需氧降解也有厌氧降解;(2)利用有机物的一级衰减模型对该污染现场土壤中石油类污染物的降解速率和半衰期进行计算表明,2次试验计算得到的石油类污染物的半衰期基本一致,该污染现场石油类污染物的半衰期为50 d左右;(3)在此基础上,对该加油站包气带土壤的自然衰减能力和环境质量进行评价,2次试验结果均表明该污染现场在自然衰减的作用下已经不存在环境风险.  相似文献   

13.
Cosolvent effect on the catalytic reductive dechlorination of PCE   总被引:1,自引:0,他引:1  
Dror I  Schlautman MA 《Chemosphere》2004,57(10):1505-1514
Reductive dechlorination of chlorinated organic contaminants is an effective approach to treat this widespread group of environmentally hazardous substances. Metalloporphyrins can be used to catalyze reduction reactions by shuttling electrons from a reducing agent (electron donor) to chlorinated organic contaminants, thus rendering them to non-chlorinated acetylene, ethylene or ethane as major products. Iron, nickel and vanadium oxide tetraphenyl porphyrins (TPPs) were used as models of non-soluble metalloporphyrins that are common in subsurface environments, and hence may inflect on the ability to use natural ones. The effect of cosolvents on metalloporphyrins is demonstrated to switch the reduction of tetrachlorethylene (PCE) from no reaction to complete PCE transformation within 24 h and the production of final non-chlorinated compounds. Variations in product distributions for the different metalloporphyrins indicate that changes in the core metal can influence reaction rates and effective pathways. Furthermore, different cosolvents can generate varied product distributions, again suggesting that different pathways and/or rates are operative in the reduction reactions. Comparison of different cosolvent effects on PCE reduction using vitamin B12--a soluble natural metalloporphyrinogen--as the catalyst shows less pronounced differences between reactions in various cosolvent solutions versus only aqueous solution.  相似文献   

14.
At the field scale, the biodegradation rate is usually estimated from analytical solutions to single species transport with first-order reactions, using measured data as input. Because many contaminants, e.g., chlorinated solvents, are degraded in a sequential pattern, with degradation products further reacting to produce new species, it is of great interest to quantify the transformation rate of every reaction. The conventional inverse solutions for identifying the transformation rates are limited to single species problems. In the present study, we propose a successive optimization approach to identify the biodegradation rate for each species by using a previously developed analytical solution to multi-species first-order reactive transport using data obtained at the field scale. By specifying a link between analytical solutions to sequentially reactive transport problems and optimization methods and assuming constant transport parameters (velocity, dispersivities, and retardation factors), the first-order transformation rates are optimized successively from parent species to its daughter species.  相似文献   

15.
Groundwater contamination due to releases of petroleum products is a major environmental concern in many urban districts and industrial zones. Over the past years, a few studies were undertaken to address in situ bioremediation processes coupled with contaminant transport in two- or three-dimensional domains. However, they were concentrated on natural attenuation processes for petroleum contaminants or enhanced in situ bioremediation processes in laboratory columns. In this study, an integrated numerical and physical modeling system is developed for simulating an enhanced in situ biodegradation (EISB) process coupled with three-dimensional multiphase multicomponent flow and transport simulation in a multi-dimensional pilot-scale physical model. The designed pilot-scale physical model is effective in tackling natural attenuation and EISB processes for site remediation. The simulation results demonstrate that the developed system is effective in modeling the EISB process, and can thus be used for investigating the effects of various uncertainties.  相似文献   

16.
The hexachlorocyclohexane-isomers (HCH), hexachlorobenzene (HCB), the polychlorinated biphenyls (PCB), 1,1,1-trichloro-2,2-bis(p-chlorophenyl)ethane (4,4′-DDT) and 1,1-dichloro-2,2-bis(p-chlorophenyl)ethene (4,4′-DDE) have been measured in urban and rural air around the city of Ulm (F. R. G., 48.4° N, 10.0° E). The sampling stations are typical for continental air in the westerlies of the northern hemisphere including local and regional influences. The analytical method consists of adsorptive sampling of large volumes (1000 m3) of air on silica gel, solvent desorption with CH2Cl2, preseparation of the collected chlorinated C6/C14 hydrocarbons by liquid adsorption chromatography on silica gel, and high resolution capillary gas chromatography with electron capture-(HRGC/ECD) or mass-selective detection (HRGC/MSD). The concentrations found in the lower troposphere under different meteorological conditions reflect regional input and long range transport. The levels found range from 1 pg/m3 for 4,4′-DDT to 10 ng/m3 for gamma HCH.  相似文献   

17.
Soil samples from five contaminated sawmill sites in Sweden were characterized with respect to chlorophenols (CP), chlorinated phenoxy phenols (PCPP, hydroxylated chlorinated diphenyl ethers), chlorinated diphenyl ethers (PCDE), chlorinated dibenzofurans (PCDF) and chlorinated dibenzo-p-dioxins (PCDD). The composition of chlorinated compounds in the soil samples was compared to the composition of two preservatives commonly used in the Scandinavian wood impregnation industry: the 2,3,4,6-tetrachlorophenol preservative called Ky-5 and the pentachlorophenol preservative Dowicide G. The levels of CPs in the soil samples ranged from 0.1 to 4500 mgkg-1 d.w., PCPPs from <0.15 to 940 mgkg-1 d.w., PCDEs from <38 to 6800 microgkg-1 d.w., PCDFs from 7.4 to 18000 microgkg-1 d.w. and PCDDs from 9.9 to 35000 microgkg-1 d.w. The resulting WHO-TEQ of PCDD/Fs in the soil samples ranged from 0.14 to 3000 microgkg-1 d.w. Despite a wide range of concentrations the congener compositions were similar within tetrachlorophenate and pentachlorophenate contaminated soils respectively. The contamination at each sawmill site may be linked to the use of either a tetrachlorphenol preservative, e.g. Ky-5, or a pentachlorophenol preservative, e.g. Dowicide G. Best-fit calculations were used to compare the chlorinated phenol contents of the preservatives to those of the soil samples. This revealed a positive correlation between the hydrophobicity (logKow) of contaminants and the ratio of their levels in soil to preservatives. The relative abundance of the chlorinated compounds varied greatly between the five sites studied, suggesting that their transport parameters differ substantially.  相似文献   

18.
Abstract

In an earlier paper the ozone-forming potential of n-propyl bromide (NPB) was studied with a new methodology designed to address issues associated with a marginal smog-forming compound. However, the U.S. Environmental Protection Agency (EPA) subsequently revised its policy and now recommends using the Maximum Incremental Reactivity (MIR) scale to rank the ozone-forming potential of all volatile organic compounds (VOCs), including those of marginal ozone productivity. Nevertheless, EPA contemplated exceptions to the box-model-derived MIR scale by allowing use of photochemical grid-model simulations for case specific reactivity assessments. The California Air Resources Board (CARB) also uses the MIR scale and CARB has a Reactivity Scientific Advisory Committee that can consider exceptions to the MIR scale. In this study, grid-model simulations that were recommended by EPA are used to evaluate the incremental ozone impacts of NPB using an update to the chemical mechanism developed in an earlier paper. New methods of analysis of the grid-model output are further developed here to quantify the relative reactivities between NPB and ethane over a wide range of conditions. The new grid-model-based analyses show that NPB is significantly different and generally less in ozone-forming potential (i.e., reactivity) than predicted by the box-model-based MIR scale relative to ethane, EPA’s “bright-line” test for non-VOC status. Although NPB has low reactivity compared to typical VOCs on any scale, the new grid-model analyses developed here show that NPB is far less reactive (and even has negative reactivity) compared to the reactivity predicted by the MIR scale.  相似文献   

19.
Subsurface contamination by trichloroethene (TCE) was detected at a Michigan National Priorities List (NPL) site in 1982. The TCE plume resulted from the disposal of spent solvent and other chemicals at an industrial facility located in the eastern shore of Lake Michigan. TCE degradation products of three dichloroethene (DCE) isomers, vinyl chloride (VC) and ethene were present. The plume was depleted of oxygen and methanogenic at certain depths. Transects of the plume were sampled by slotted auger borings the year after the TCE plume was first discovered. Water samples were also taken from lake sediments to a depth of 12 m about 100 m offshore. Later samples were taken along the shoreline of the lake with a hand-driven probe. Later in 1998 water was taken from sediments about 3-m from the shoreline. The average concentration of each chemical and net apparent base coefficient between appropriate pairs of transects between the lower site and lakeshore were calculated. Loss rates were then calculated from an analytical solution of the two-dimensional advective-dispersive-reactive transport equation. Net apparent rate coefficients and a set of coupled reaction rate equations were used to extract the apparent loss coefficients. This study showed the field evidence for natural attenuation of TCE.  相似文献   

20.
危险废物事故排放的河流水环境健康风险评价   总被引:3,自引:0,他引:3  
分析了基于水体中污染物迁移转化方程的水质预测模型,并借鉴美国环保局推荐使用的健康风险评价模型,建立了一种危险废物事故排放时水环境对人体健康风险的评价方法。以电镀污泥为例验证了该方法的有效性。结果显示:该方法需要参数少且计算简单;电镀污泥中目标污染物(Cr、Cu、Ni、Zn)所引起的河流水环境非致癌风险(1.67)超过了美国标准中的可接受风险水平1.00,不可接受;致癌风险(0.88E-11)则小于美国标准中的可接受风险水平1.00E-06,风险不明显。  相似文献   

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