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Contamination of groundwater with chlorinated ethenes is common and represents a threat to drinking water sources. Standard anaerobic bioremediation methods for the highly chlorinated ethenes PCE and TCE are not always effective in promoting complete degradation. In these cases, the target contaminants are degraded to the daughter products DCE and/or vinyl chloride. This creates an additional health risk, as vinyl chloride is even more toxic and carcinogenic than its precursors. New treatment modalities are needed to deal with this widespread environmental problem. We describe successful bioremediation of a large, migrating, dilute vinyl chloride plume in Massachusetts with an aerobic biostimulation treatment approach utilizing both oxygen and ethene. Initial microcosm studies showed that adding ethene under aerobic conditions stimulated the rapid degradation of VC in site groundwater. Deployment of a full‐scale treatment system resulted in plume migration cutoff and nearly complete elimination of above‐standard VC concentrations.  相似文献   

3.
The ability of bioremediation to treat a source area containing trichloroethene (TCE) present as dense nonaqueous phase liquid (DNAPL) was assessed through a laboratory study and a pilot test at Launch Complex 34, Cape Canaveral Air Force Center. The results of microcosm testing indicate that the indigenous microbial community was capable of dechlorinating TCE to ethene if amended with electron donor; however, bioaugmentation with a dechlorinating culture (KB-1; SiREM, Guelph, Ontario, Canada) significantly increased the rate of ethene formation. In microcosms, the activity of the dechlorinating organisms in KB-1 was not inhibited at initial TCE concentrations as high as 2 mM. The initially high TCE concentration in ground water (1.2 mM or 155 mg/L) did not inhibit reductive dechlorination, and at the end of the study, the average concentration of ethene (2.4 mM or 67 mg/L) was in stoichiometric excess of this initial TCE concentration. The production of ethene in stoichiometric excess in comparison to the initial TCE concentration indicates that the bioremediation treatment enhanced the removal of TCE mass (either sorbed to soil or present as DNAPL). Detailed soil sampling indicated that the bioremediation treatment removed greater than 98.5% of the initial TCE mass. Confirmatory ground water samples collected 22 months after the bioremediation treatment indicated that chloroethene concentrations had continued to decline in the absence of further electron donor addition. The results of this study confirm that dechlorination to ethene can proceed at the high TCE concentrations often encountered in source areas and that bioremediation was capable of removing significant TCE mass from the test plot, suggesting that enhanced bioremediation is a potentially viable remediation technology for TCE source areas. Dehalococcoides abundance increased by 2 orders of magnitude following biostimulation and bioaugmentation.  相似文献   

4.
Four samples of two commercially available iron brands used as substrate for iron permeable reactive barriers (PRBs) were tested for suitability for remediation of perchloroethylene (PCE), trichloroethylene (TCE), cis-dichloroethylene (cDCE) and vinyl chloride (VC). Kinetic studies indicate that rates of reaction are enhanced for cDCE and VC on Connelly iron (2.8 x 10(-4) to 6.9 x 10(-4) L/m2/hr and 2.0 x 10(-4) to 9.0 x 10(-4) L/m2/hr, for cDCE and VC, respectively) vs. Peerless iron (3.1 x 10(-5) to 4.6 x 10(-5) L/m2/hr and 2.4 x 10(-5) to 4.1 x 10(-5) L/m2/hr, for cDCE and VC, respectively). Carbon isotopic analyses of the residual chlorinated ethylene (CE) during degradation indicate significant fractionation occurs during reductive dechlorination, with, for example, up to 70% enrichment in carbon isotopic values observed when VC is more than 99% degraded. Comparison of fractionation factors (epsilon) indicates significant differences in carbon isotopic fractionation for different iron types and for different CEs. For the lower CEs (cDCE and VC) in particular, both slower reaction rates and larger fractionation are observed for degradation on Peerless vs. Connelly iron. This is the first study to establish a correlation between the rate of abiotic degradation on Fe(0) and the extent of isotopic fractionation, and the first to confirm consistent differences in these two parameters as a function of iron type. The possibility that these differences in kinetics and carbon isotopic fractionation for cDCE and VC are related to differences in branching ratios between competing hydrogenolysis and beta-elimination reactions during reductive dechlorination on the iron surfaces is discussed.  相似文献   

5.
High‐resolution soil and groundwater monitoring was performed to assess the long‐term impacts of bioremediation using bioaugmentation with a dechlorinating microbial consortium (and sodium lactate as the electron donor) in a well‐characterized trichloroethene (TCE) dense nonaqueous phase liquid (DNAPL) source area. Monitoring was performed up to 3.7 years following active bioremediation using a high‐density monitoring network that included several discrete interval multi‐level sampling wells. Results showed that despite the absence of lactate, lactate fermentation transformation products, or hydrogen, biogeochemical conditions remained favorable for the reductive dechlorination of chlorinated ethenes. In locations where soil data showed that TCE DNAPL sources persisted, local contaminant rebound was observed in groundwater, whereas no rebound or continuous decreases in chlorinated ethenes were observed in locations where DNAPL sources were treated. While ethene levels measured 3.7 years after active treatment suggested relatively low (2 to 30%) dechlorination of the parent TCE and daughter products, carbon stable isotope analysis showed that the extent of complete dechlorination was much greater than indicated by ethene generation and that the estimated first‐order rate constant describing the complete dechlorination of TCE at 3.7 years following active bioremediation was approximately 3.6 y–1. Overall, results of this study suggest that biological processes may persist to treat TCE for years after cessation of active bioremediation, thereby serving as an important component of remedial treatment design and long‐term attenuation.  相似文献   

6.
Chlorinated ethenes such as tetrachloroethene and trichloroethene have been widely used as dry-cleaning and degreasing solvents. Under anaerobic conditions, microorganisms reduce these parent compounds to less-chlorinated daughter products such as cis-1,2-dichloroethene (cDCE), and often further to ethene. This process can be stalled at cDCE, due to insufficient supply of reductants and/or inadequate microbial-community composition. Recently, a novel bacterium, Polaromonas sp. JS666, was isolated that is able to aerobically oxidize cDCE as sole carbon and energy source. As such, it is a promising candidate for use as a subsurface, bioaugmentation agent at sites where anaerobic bioremediation is inappropriate or has stalled and cDCE has migrated to, and accumulated within, aerobic zones, or where it is practical to impose aerobic conditions. Subsurface sediments or groundwater from six such cDCE-contaminated sites were used to construct microcosms. In every sediment or groundwater inoculated with JS666, the organism was able to degrade cDCE, provided that the pH remained circum-neutral. Even when JS666 was challenged with an alternate carbon source, or in the presence of competitive/predatory microorganisms, there was a measure of success. Collectively, these microcosm studies suggest that JS666 is a viable candidate for the bioaugmentation of aerobic, cDCE-contaminated sites. A minimum inoculation level in excess of 105 cells per mL is recommended for field applications. At this level of inoculation, 100 L of inoculum culture grown to an OD600 of 1.0 should be able to treat a 10-m × 30-m × 80-m (24,000-m3) plot.  相似文献   

7.
Spatial and temporal variations in a trichloroethylene (TCE) plume at an industrial complex in Wonju, Korea, were examined based on hydrogeological data and seven rounds of groundwater quality data collected over a year. The site has considerable vertical heterogeneities; the top layer of soil is covered by impermeable paving material at several locations, followed by a series of reclaimed or residual soil layers, and with weathered rocks to the crystalline biotite granite at the bottom. Areal heterogeneity in the surface conditions plays an important role in controlling groundwater recharge. The heterogeneity structure is influenced by complex surface conditions paved with asphalt and concrete. Owing to the presence of limited recharge area and concentrated summer precipitation events, the effects of seasonal variations on groundwater hydraulics tend to diminish with distance from the recharge area. This result was established by analysing the influence of the contrasting surface recharge conditions between the near‐source zone and the far zone, and the seasonally concentrated precipitation on the transport patterns of a TCE plume. In addition, variations in the plume's downstream contaminant flux levels were also analysed along a transect line near the source zone. The results show that the general tendency of the TCE plume contaminant concentration and mass discharges were reproducible if we account for seasonal recharge variations and the associated changes in the groundwater level. During recharge events, the TCE concentration variations appear to be influenced by leaching of the residual dense non‐aqueous‐phase liquid (DNAPL) TCE trapped in the unsaturated zone. This result shows that seasonal variations in contaminant plume near the source zone is inevitable at this site, and that these variations indicate the presence of residual DNAPL at or above the water table, at least in some isolated locations. Copyright © 2011 John Wiley & Sons, Ltd.  相似文献   

8.
Effective long‐term operation of soil vapor extraction (SVE) systems for cleanup of vadose‐zone sources requires consideration of the likelihood that remediation activities over time will alter the subsurface distribution and configuration of contaminants. A method is demonstrated for locating and characterizing the distribution and nature of persistent volatile organic contaminant (VOC) sources in the vadose zone. The method consists of three components: analysis of existing site and SVE‐operations data, vapor‐phase cyclic contaminant mass‐discharge testing, and short‐term vapor‐phase contaminant mass‐discharge tests conducted in series at multiple locations. Results obtained from the method were used to characterize overall source zone mass‐transfer limitations, source‐strength reductions, potential changes in source‐zone architecture, and the spatial variability and extent of the persistent source(s) for the Department of Energy's Hanford site. The results confirmed a heterogeneous distribution of contaminant mass discharge throughout the vadose zone. Analyses of the mass‐discharge profiles indicate that the remaining contaminant source is coincident with a lower‐permeability unit at the site. Such measurements of source strength and size as obtained herein are needed to determine the impacts of vadose‐zone sources on groundwater contamination and vapor intrusion, and can support evaluation and optimization of the performance of SVE operations.  相似文献   

9.
The generation of vapor‐phase contaminant plumes within the vadose zone is of interest for contaminated site management. Therefore, it is important to understand vapor sources such as non‐aqueous‐phase liquids (NAPLs) and processes that govern their volatilization. The distribution of NAPL, gas, and water phases within a source zone is expected to influence the rate of volatilization. However, the effect of this distribution morphology on volatilization has not been thoroughly quantified. Because field quantification of NAPL volatilization is often infeasible, a controlled laboratory experiment was conducted in a two‐dimensional tank (28 cm × 15.5 cm × 2.5 cm) with water‐wet sandy media and an emplaced trichloroethylene (TCE) source. The source was emplaced in two configurations to represent morphologies encountered in field settings: (1) NAPL pools directly exposed to the air phase and (2) NAPLs trapped in water‐saturated zones that were occluded from the air phase. Airflow was passed through the tank and effluent concentrations of TCE were quantified. Models were used to analyze results, which indicated that mass transfer from directly exposed NAPL was fast and controlled by advective‐dispersive‐diffusive transport in the gas phase. However, sources occluded by pore water showed strong rate limitations and slower effective mass transfer. This difference is explained by diffusional resistance within the aqueous phase. Results demonstrate that vapor generation rates from a NAPL source will be influenced by the soil water content distribution within the source. The implications of the NAPL morphology on volatilization in the context of a dynamic water table or climate are discussed.  相似文献   

10.
Field characterization of a trichloroethene (TCE) source area in fractured mudstones produced a detailed understanding of the geology, contaminant distribution in fractures and the rock matrix, and hydraulic and transport properties. Groundwater flow and chemical transport modeling that synthesized the field characterization information proved critical for designing bioremediation of the source area. The planned bioremediation involved injecting emulsified vegetable oil and bacteria to enhance the naturally occurring biodegradation of TCE. The flow and transport modeling showed that injection will spread amendments widely over a zone of lower‐permeability fractures, with long residence times expected because of small velocities after injection and sorption of emulsified vegetable oil onto solids. Amendments transported out of this zone will be diluted by groundwater flux from other areas, limiting bioremediation effectiveness downgradient. At nearby pumping wells, further dilution is expected to make bioremediation effects undetectable in the pumped water. The results emphasize that in fracture‐dominated flow regimes, the extent of injected amendments cannot be conceptualized using simple homogeneous models of groundwater flow commonly adopted to design injections in unconsolidated porous media (e.g., radial diverging or dipole flow regimes). Instead, it is important to synthesize site characterization information using a groundwater flow model that includes discrete features representing high‐ and low‐permeability fractures. This type of model accounts for the highly heterogeneous hydraulic conductivity and groundwater fluxes in fractured‐rock aquifers, and facilitates designing injection strategies that target specific volumes of the aquifer and maximize the distribution of amendments over these volumes.  相似文献   

11.
The objective of this study was to characterize the behavior of a groundwater contaminant (trichloroethene, TCE) plume after implementation of a source‐containment operation at a site in Arizona. The plume resides in a quasi‐three‐layer system comprising a sand/gravel unit bounded on the top and bottom by relatively thick silty clayey layers. The system was monitored for 60 months beginning at start‐up in 2007 to measure the change in contaminant concentrations within the plume, the change in plume area, the mass of the contaminant removed, and the integrated contaminant mass discharge (CMD). The concentrations of TCE in groundwater pumped from the plume extraction wells have declined significantly over the course of operation, as have concentrations for groundwater sampled from 40 monitoring wells located within the plume. The total CMD associated with operation of the plume extraction wells peaked at 0.23 kg/d, decreased significantly within 1 year, and thereafter began an asymptotic decline to a current value of approximately 0.03 kg/d. Despite an 87% reduction in contaminant mass and a comparable 87% reduction in CMD for the plume, the spatial area encompassed by the plume has decreased by only approximately 50%. This is much less than would be anticipated based on ideal flushing and mass‐removal behavior. Simulations produced with a simplified three‐dimensional (3D) numerical model matched reasonably well to the measured data. The results of the study suggest that permeability heterogeneity, back diffusion, hydraulic factors associated with the specific well field system, and residual discharge from the source zone are all contributing to the observed persistence of the plume, as well as the asymptotic behavior currently observed for mass removal and for the reduction in CMD.  相似文献   

12.
The spatial distribution of residual light non-aqueous phase liquid (LNAPL) is an important factor in reactive solute transport modeling studies. There is great uncertainty associated with both the areal limits of LNAPL source zones and smaller scale variability within the areal limits. A statistical approach is proposed to construct a probabilistic model for the spatial distribution of residual NAPL and it is applied to a site characterized by ultra-violet-induced-cone-penetration testing (CPT–UVIF). The uncertainty in areal limits is explicitly addressed by a novel distance function (DF) approach. In modeling the small-scale variability within the areal limits, the CPT–UVIF data are used as primary source of information, while soil texture and distance to water table are treated as secondary data. Two widely used geostatistical techniques are applied for the data integration, namely sequential indicator simulation with locally varying means (SIS–LVM) and Bayesian updating (BU). A close match between the calibrated uncertainty band (UB) and the target probabilities shows the performance of the proposed DF technique in characterization of uncertainty in the areal limits. A cross-validation study also shows that the integration of the secondary data sources substantially improves the prediction of contaminated and uncontaminated locations and that the SIS–LVM algorithm gives a more accurate prediction of residual NAPL contamination. The proposed DF approach is useful in modeling the areal limits of the non-stationary continuous or categorical random variables, and in providing a prior probability map for source zone sizes to be used in Monte Carlo simulations of contaminant transport or Monte Carlo type inverse modeling studies.  相似文献   

13.
This work focuses on the site‐specific assessment of source zone natural attenuation (SZNA) at chlorinated aliphatic hydrocarbon (CAH)‐impacted sites. The approach is similar in some ways, but different in other ways from recently proposed SZNA assessment paradigms for petroleum‐impacted sites. The similarities lie in the organization of the approach around determining: (1) whether or not SZNA is occurring, (2) the current SZNA rate, and (3) what is the future projection for SZNA rate changes and the final state of the source zone. Differences lie in how those rates are determined, especially with respect to the quantities measured and data reduction. Petroleum‐impacted site SZNA approaches emphasize quantifying fluxes of electron acceptors, while the proposed CAH assessment approach emphasizes quantifying parent and daughter compound fluxes. A paradigm for assessing SZNA at CAH sites is presented and its use is illustrated, for example former dry cleaner site, where the SZNA rate was approximately 3.5 kg/year as tetrachloroethylene (PCE) with about 80% of the mass loss attributed to groundwater flow and 20% attributed to vapor transport.  相似文献   

14.
Simulation of biodegradation of chlorinated solvents in dense non-aqueous phase liquid (DNAPL) source zones requires a model that accounts for the complexity of processes involved and that is consistent with available laboratory studies. This paper describes such a comprehensive modeling framework that includes microbially mediated degradation processes, microbial population growth and decay, geochemical reactions, as well as interphase mass transfer processes such as DNAPL dissolution, gas formation and mineral precipitation/dissolution. All these processes can be in equilibrium or kinetically controlled. A batch modeling example was presented where the degradation of trichloroethene (TCE) and its byproducts and concomitant reactions (e.g., electron donor fermentation, sulfate reduction, pH buffering by calcite dissolution) were simulated. Local and global sensitivity analysis techniques were applied to delineate the dominant model parameters and processes. Sensitivity analysis indicated that accurate values for parameters related to dichloroethene (DCE) and vinyl chloride (VC) degradation (i.e., DCE and VC maximum utilization rates, yield due to DCE utilization, decay rate for DCE/VC dechlorinators) are important for prediction of the overall dechlorination time. These parameters influence the maximum growth rate of the DCE and VC dechlorinating microorganisms and, thus, the time required for a small initial population to reach a sufficient concentration to significantly affect the overall rate of dechlorination. Self-inhibition of chlorinated ethenes at high concentrations and natural buffering provided by the sediment were also shown to significantly influence the dechlorination time. Furthermore, the analysis indicated that the rates of the competing, nonchlorinated electron-accepting processes relative to the dechlorination kinetics also affect the overall dechlorination time. Results demonstrated that the model developed is a flexible research tool that is able to provide valuable insight into the fundamental processes and their complex interactions during bioremediation of chlorinated ethenes in DNAPL source zones.  相似文献   

15.
 There exist many sites with contaminated groundwater because of inappropriate handling or disposal of hazardous materials or wastes. Health risk assessment is an important tool to evaluate the potential environmental and health impacts of these contaminated sites. It is also becoming an important basis for determining whether risk reduction is needed and what actions should be initiated. However, in research related to groundwater risk assessment and management, consideration of multimedia risk assessment and the separation of the uncertainty due to lack of knowledge and the variability due to natural heterogeneity are rare. This study presents a multimedia risk assessment framework with the integration of multimedia transfer and multi-pathway exposure of groundwater contaminants, and investigates whether multimedia risk assessment and the separation of uncertainty and variability can provide a better basis for risk management decisions. The results of the case study show that a decision based on multimedia risk assessment may differ from one based on risk resulting from groundwater only. In particular, the transfer from groundwater to air imposes a health threat to some degree. By using a methodology that combines Monte Carlo simulation, a rank correlation coefficient, and an explicit decision criterion to identify information important to the decision, the results obtained when uncertainty and variability are separate differ from the ones without such separation. In particular, when higher percentiles of uncertainty and variability distributions are considered, the method separating uncertainty and variability identifies TCE concentration as the single most important input parameter, while the method that does not distinguish the two identifies four input parameters as the important information that would influence a decision on risk reduction.  相似文献   

16.
Natural source zone depletion (NSZD) refers to processes within chemically impacted vadose and saturated zones that reduce the mass of contaminants remaining in a defined source control volume. Studies of large petroleum hydrocarbon release sites have shown that the depletion rate by vapor phase migration of degradation products from the source control volume through the vadose zone (V‐NSZD) is often considerably higher than the rate of depletion from the source control volume by groundwater flow carrying dissolved petroleum hydrocarbons arising from dissolution, desorption, or back diffusion, and degradation products arising from biodegradation (GW‐NSZD). In this study, we quantified vadose zone and GW‐NSZD at a small unpaved fuel release site in California typical of those in settings with predominantly low permeability media. We estimated vadose zone using a dense network of efflux monitoring locations at four sampling events over 2 years, and GW‐NSZD using groundwater monitoring data downgradient of the source control volume in three depth intervals spanning up to 9 years. On average, vadose zone was 17 times greater than GW‐NSZD during the time interval of comparison, and vadose zone was in the range of rates quantified at other sites with petroleum hydrocarbon releases. Estimating vadose zone and GW‐NSZD rates is challenging but the vadose zone rate is the best indicator of overall source mass depletion, whereas GW‐NSZD rates may be useful as baselines to quantify progress of natural or engineered remediation in portions of the saturated zone in which there are impediments to loss of methane and other gases to the vadose zone.  相似文献   

17.
Adaptive site management and aggressive bioremediation in the source zone of a complex chlorinated dense nonaqueous phase liquid (DNAPL) site reduced total chlorinated hydrocarbon mass discharge by nearly 80%. Successful anaerobic bioremediation of chlorinated hydrocarbons can be impaired by inadequate concentrations of electron donors, competing electron acceptors, specific inhibitors such as chloroform, and potentially by high contaminant concentrations associated with residual DNAPL. At the study site, the fractured bedrock aquifer was impacted by a mixture of chlorinated solvents and associated daughter products. Concentrations of 1,1,2,2‐tetrachloroethane (1,1,2,2‐TeCA), 1,1,2‐trichloroethane (1,1,2‐TCA), and 1,2‐dichloroethane (1,2‐DCA) were on the order of 100 to 1000 mg/L. Chloroform was present as a co‐contaminant and background sulfate concentrations were approximately 400 mg/L. Following propylene glycol injections, concentrations of organohalide‐respiring bacteria including Dehalococcoides and Dehalogenimonas spp. increased by two to three orders of magnitude across most of the source area. Statistical analysis indicated that reaching volatile fatty acid concentrations greater than 1000 mg/L and depleting sulfate to concentrations less than 50 mg/L were required to achieve a Dehalococcoides concentration greater than the 104 cells/mL recommended for generally effective reductive dechlorination. In a limited area, chloroform concentrations greater than 5 mg/L inhibited growth of Dehalococcoides populations despite the availability of electron donor and otherwise appropriate geochemical conditions. After implementing a groundwater recirculation system targeting the inhibited area, chloroform concentrations decreased permitting significant increases in concentrations of Dehalococcoides and vinyl chloride reductase gene copies.  相似文献   

18.
Groundwater contamination risk assessment for health-threatening compounds should benefit from a stochastic environmental risk assessment which considers the effects of biological, chemical, human behavioral, and physiological processes that involve elements of biotic and abiotic aquifer uncertainty, and human population variability. This paper couples a complex model of chemical degradation and transformation with movement in an aquifer undergoing bioremediation to generate a health risk analysis for different population cohorts in the community. A two-stage Monte Carlo simulation has separate stages for population variability and aquifer uncertainty yielding a computationally efficient and conceptually attractive algorithm. A hypothetical example illustrates how risk variance analysis can be conducted to determine the distribution of risk, and the relative impact of uncertainty and variability in different sets of parameters upon the variation of risk values for adults, adolescents, and children. The groundwater example considers a community water supply contaminated with chlorinated ethenes. Biodegradation pathways are enhanced by addition of butyrate. The results showed that the contribution of uncertainty to the risk variance is comparable to that of variability. Among the uncertain parameters considered, transmissivity accounted for the major part of the output variance. Children were the most susceptible and vulnerable population cohort.  相似文献   

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Selection of monitored natural attenuation as a ground water remedy requires that sound scientific documentation clearly illustrating the effectiveness of this remedial alternative be presented to regulatory agencies and concerned citizens. An innovative radial diagram approach is applied to illustrate natural attenuation trends for total benzene, toluene, ethylbenzene, and xylenes (BTEX) and chlorinated ethenes at a former fire training area at Pittsburgh Air Force Base, New York. A BTEX-CAH (chlorinated aliphatic hydrocarbons) radial diagram map shows that concentrations of site contaminants are generally decreasing along the primary flowpath downgradient from the source area. This radial diagram map also suggests that there is a spatial correlation between decreasing CAH parent compound concentrations and increasing or stable daughter product concentrations. This provides secondary evidence of intrinsic biodegradation of TCE downgradient from the source area. A SEQUENCE-Redox™ map suggests that there is a spatial correlation between trends in electron acceptor and metabolic byproduct concentrations, and the decline in total BTEX concentrations downgradient from the source area. This correlation provides secondary evidence for the intrinsic biodegradation of total BTEX in the aquifer. This study demonstrates that radial diagram visual aids can provide a clear and efficient approach for documenting natural attenuation lines of evidence, as an alternative or a complement to using multiple contour maps, tabulated data, or log-linear plots.  相似文献   

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