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1.
Natural source zone depletion (NSZD) is increasingly being integrated into management strategies for petroleum release sites. Measurements of NSZD rates can be used to evaluate naturally occurring hydrocarbon (HC) mass losses, and provide a baseline for evaluating engineered recovery systems. Here, nominal saturated and unsaturated zone HC losses were quantified by groundwater sampling and ground surface CO2 effluxes approximately monthly over a 1-year period. In addition, subsurface gas profiles and temperature, precipitation, and groundwater elevation were evaluated to elucidate dominant environmental factors controlling NSZD rates. Results showed that NSZD rates estimated by surface CO2 effluxes were, on average, more than a factor of 3 greater than those estimated by uptake of electron acceptors (primarily sulfate) in extracted groundwater. This may indicate that vadose zone mass loss mechanisms (e.g., volatilization and subsequent biodegradation) were dominant in this system, but possible transfer of gases from the saturated zone to the vadose zone confounds this interpretation. Results for this semiarid site revealed that increasing NSZD rates tended to occur with increasing ambient monthly precipitation and temperature when accounting for time lags associated with subsurface transport. However, groundwater elevation was not found to be significantly related to NSZD rates. This result is counter to an expectation that increased smear zone exposure increases HC mass losses, and suggests that the pump-and-treat system did not greatly influence total NSZD rates directly through smear zone flushing or indirectly by lowering the regional water table.  相似文献   

2.
We compare two methods for estimating the natural source zone depletion (NSZD) rate at fuel release sites that occurs by groundwater flow through the source zone due to dissolution and transport of biodegradation products. Dissolution is addressed identically in both methods. The “mass budget method”, previously proposed and applied by others, estimates the petroleum hydrocarbon biodegradation rate based on dissolved electron acceptor delivery and dissolved biodegradation product removal by groundwater flow. The mass budget method relies on assumed stoichiometry for the degradation reactions and differences in concentrations of dissolved species (oxygen, nitrate, sulfate, reduced iron, reduced manganese, nonvolatile dissolved organic carbon, methane) at monitoring locations upgradient and downgradient of the source zone. We illustrate a refinement to account for degradation reactions associated with loss of reduced iron from solution. The “carbon budget method,” a simplification of approaches applied by others, addresses carbon‐containing species in solution or lost from solution (precipitated) and does not require assumptions about stoichiometry or information about electron acceptors. We apply both methods to a fuel release site with unusually detailed monitoring data and discuss applicability to more typical and less thoroughly monitored sites. The methods, as would typically be applied, yield similar results but have different constraints and uncertainties. Overall, we conclude that the carbon budget method has greater practical utility as it is simpler, requires fewer assumptions, accounts for most iron‐reducing reactions, and does not include CO2 that escapes from the saturated to the unsaturated zone.  相似文献   

3.
Natural depletion of subsurface petroleum liquids releases energy in the form of heat. The rate of natural source zone depletion (NSZD) can be derived from subsurface temperature data. An energy balance is performed to resolve NSZD‐generated energy in terms of W/m2. Biodegradation rates are resolved by dividing the NSZD energy by the heat of reaction in joules/mol. Required temperature data are collected using data loggers, wireless connections, and automated data storage and analysis. Continuous thermal resolution of monthly NSZD rates at a field site indicates that apparent monthly NSZD rates vary through time, ranging from 10,000 to 77,000 L/ha/year. Temporal variations in observed apparent NSZD rates are attributed to processes governing the conversion of CH4 to CO2, as opposed to the actual rates of NSZD. Given a year or more of continuous NSZD rate data, it is anticipated that positive and negative biases in apparent NSZD rates will average out, and averaged apparent NSZD rates will converge to true NSZD rates. An 8.4% difference between average apparent NSZD rates over a 31‐month period using the thermal monitoring method and seven rounds of CO2 efflux measurements using CO2 traps supports the validity of both CO2 trap and thermal monitoring methods. A promising aspect of thermal monitoring methods is that continuous data provide a rigorous approach to resolving the true mean NSZD rates as compared to temporally sparse CO2 trap NSZD rate measurements. Overall, a vision is advanced of real‐time sensor‐based groundwater monitoring that can provide better data at lower costs and with greater safety, security, and sustainability.  相似文献   

4.
There are several key data gaps in our understanding of Natural Source Zone Depletion (NSZD) processes at sites impacted by light nonaqueous phase liquid (LNAPL), and quantifying NSZD rates can be challenging due to the inherent differences in measurement methods. In this study, four different NSZD measurement methods (oxygen influx measured by the Gradient Method, long-term carbon dioxide efflux measured with Carbon Traps, instantaneous carbon dioxide efflux measured with Dynamic Closed Chambers (DCC LI-COR), and the long-term heat flux from biodegradation measured by Thermal NSZD monitoring), as well as LNAPL composition and dissolved gas sampling, were applied at a site in Southern California. These techniques were used to evaluate key questions such as: (1) how do different NSZD rate measurement methods compare, and what causes variability in NSZD results?; (2) to what extent NSZD processes are occurring in LNAPL within the saturated zone?; and (3) how is NSZD related to LNAPL composition change over time? Carbon Traps and Thermal NSZD monitoring measurement methods provided the most consistent NSZD data at this geologically heterogeneous site, with two location average NSZD rates of 540 and 480 gal/acre/year, respectively. Overall, comparisons of NSZD rates between methods were challenging due to different measurement timeframes, significant temporal and spatial heterogeneity, and operational challenges with two of the NSZD methods. Finally, samples of subsurface LNAPL were collected for analysis in 2007 and 2016; results indicated that diesel-range constituents were already very degraded and anaerobic degradation of gasoline-range constituents was ongoing. A LNAPL depletion model (Douglas et al. 1996) applied to the measured LNAPL composition change appeared to greatly overestimate the amount of LNAPL depletion compared to the measured NSZD rate, but did provide an independent semiqualitative line of evidence that LNAPL was being depleted by active NSZD processes at the site.  相似文献   

5.
Groundwater monitoring wells are present at most hydrocarbon release sites that are being assessed for cleanup. If screened across the vadose zone, these wells provide an opportunity to collect vapor samples that can be used in the evaluation of vapor movement and biodegradation processes occurring at such sites. This paper presents a low purge volume method (modified after that developed by the U.S. EPA) for sampling vapor from monitoring wells that is easy to implement and can provide an assessment of the soil gas total petroleum hydrocarbon (TPH) and O2 concentrations at the base of the vadose zone. As a result, the small purge method allows for sampling of vapor from monitoring wells to support petroleum vapor intrusion (PVI) risk assessment. The small purge volume method was field tested at the Hal's service station site in Green River, Utah. This site is well‐known for numerous soil gas measurements containing high O2 and high TPH vapor concentrations in the same samples which is inconsistent with well‐accepted biodegradation models for the vapor pathway. Using the low purge volume method, monitoring wells were sampled over, upgradient, and downgradient of the light nonaqueous phase liquid (LNAPL) footprint. Results from our testing at Hal's show that vapor from monitoring wells over LNAPL contained very low O2 and high TPH concentrations. In contrast, vapor from monitoring wells not over LNAPL contained high O2 and low TPH concentrations. The results of this study show that a low purge volume method is consistent with biodegradation models especially for sampling at sites where low permeability soils exist in and around a LNAPL source zone.  相似文献   

6.
The tetrachloroethene (PCE) source zone at a site in Endicott, New York had caused a dissolved PCE plume. This plume was commingled with a petroleum hydrocarbon plume from an upgradient source of fuel oil. The plume required a system for hydraulic containment, using extraction wells located about 360 m downgradient of the source. The source area was remediated using in situ thermal desorption (ISTD). Approximately 1406 kilograms (kg) of PCE was removed in addition to 4082 kg of commingled petroleum‐related compounds. The ISTD treatment reduced the PCE mass discharge into the plume from an estimated 57 kg/year to 0.07 kg/year, essentially removing the source term. In the 5 years following the completion of the thermal treatment in early 2010, the PCE plume has collapsed, and the concentration of degradation products in the PCE‐series plume area has declined by two to three orders of magnitude. Anaerobic dechlorination is the suspected dominant mechanism, assisted by the presence of a fuel oil smear zone and a petroleum hydrocarbon plume from a separate source area upgradient of the PCE source. Based on the post‐thermal treatment groundwater monitoring data, the hydraulic containment system was reduced in 2014 and discontinued in early 2015.  相似文献   

7.
The temperature sensitivity of microbial populations is reflected in measured source attenuation rates at hydrocarbon‐impacted sites. The objective of this study was to evaluate the correlation between temperature and source attenuation rates (concentration vs. time attenuation rate over many years) of benzene and toluene by analyzing groundwater monitoring data from >2000 hydrocarbon sites. Historical monitoring records were obtained from three databases, processed to yield long‐term multiyear source attenuation rates, and then compared with representative temperatures at each site. Statistically significant and positive relationships between temperature and source attenuation rates were established for benzene and toluene, indicating that temperature does impact hydrocarbon degradation, but is one of many factors that contribute to source attenuation. There was an observed 1.1 to 1.6 times increase in attenuation rates per 10 °C increase in temperature, which is less than the rate increases predicted by the Arrhenius equation. The temperature dependence on attenuation rate is consistent with several lines of evidence that methanogenesis plays a key role in the rate of hydrocarbon source zone attenuation rather than being controlled strictly by the availability of electron acceptors. First, methanogenesis is known to be strongly influenced by temperature, with significantly higher rates up to about 35 °C. Second, the temperature‐degradation rate relationship was stronger at sites with deeper water tables (>30 ft) that are less susceptible to oxygen influx than sites with shallow water tables (<15 ft). Third, dissolved methane concentrations were higher at sites with warmer temperatures. Overall, these results provide indirect support for a conceptual model where methanogenesis is a key degradation process at hydrocarbon sites, and that attenuation of these source zones is temperature‐sensitive.  相似文献   

8.
Sulfate reducing conditions are widely observed in groundwater plumes associated with petroleum hydrocarbon releases. This leads to sulfate depletion in groundwater which can limit biodegradation of hydrocarbons (usually benzene, toluene, ethylbenzene, xylenes [BTEX] compounds) and can therefore result in extended timeframes to achieve groundwater cleanup objectives by monitored natural attenuation. Under these conditions, sulfate addition to the subsurface can potentially enhance BTEX biodegradation and facilitate enhanced natural attenuation. However, a delivery approach that enables effective contact with the hydrocarbons and is able to sustain elevated and uniform sulfate concentrations in groundwater remains a key challenge. In this case study, sulfate addition to a groundwater plume containing predominantly benzene by land application of agricultural gypsum and Epsom salt is described. Over 4 years of groundwater monitoring data from key wells subjected to pilot‐scale and site‐wide land application events are presented. These are compared to data from pilot testing employing liquid Epsom salt injections as an alternate sulfate delivery approach. Sulfate land application, sulfate retention within the vadose zone, and periodic infiltration following ongoing precipitation events resulted in elevated sulfate concentrations (>150 mg/L) in groundwater that were sustained over 12 months between application events and stimulated benzene biodegradation as indicated by declines in dissolved benzene concentration, and compound‐specific isotope analysis data for carbon in benzene. Long‐term groundwater benzene concentration reductions were achieved in spite of periodic rebounds resulting from water table fluctuations across the smear zone. Land application of gypsum is a potentially cost‐effective sulfate delivery approach at sites with open, unpaved surfaces, relatively permeable geology, and shallow hydrocarbon impacts. However, more research is needed to understand the fate and persistence of sulfate and to improve the likelihood of success and effectiveness of this delivery approach.  相似文献   

9.
At complex sites there may be many potential sources of contaminants within the vadose zone. Screening‐level analyses are useful to identify which potential source areas should be the focus of detailed investigation and analysis. A source screening module (SSM) has been developed to support preliminary evaluation of the threat posed by vadose zone waste sites on groundwater quality. This tool implements analytical solutions to simulate contaminant transport through the unsaturated and saturated zones to predict time‐varying concentrations at potential groundwater receptors. The SSM integrates several transport processes in a single simulation that is implemented within a user‐friendly, Microsoft Excel? ‐ based interface.  相似文献   

10.
Low-permeability layers of the vadose zone containing volatile organic compounds (VOCs) may persist as source zones for long time periods and may provide contamination to groundwater. At sites with low recharge rates, where vapor migration is the dominant transport process, the impact of vadose zone sources on groundwater may be difficult to assess. Typical assessment methods include one-dimensional numerical and analytical techniques. The one-dimensional approaches only consider groundwater coupling options through boundary conditions at the water table and may yield artificially high mass flux results when transport is assumed to occur by gas-phase diffusion between a source and an interface with a zero concentration boundary condition. Improvements in mass flux assessments for VOCs originating from vadose zone sources may be obtained by coupling vadose zone gas transport and dissolved contaminant transport in the saturated zone and by incorporating the inherent three-dimensional nature of gas-phase transport, including the potential of density-driven advection. This paper describes a series of three-dimensional simulations using data from the U.S. Department of Energy's Hanford site, where carbon tetrachloride is present in a low-permeability zone about 30 m above the groundwater. Results show that, for most cases, only a relatively small amount of the contaminant emanating from the source zone partitions into the groundwater and that density-driven advection is only important when relatively high source concentrations are considered.  相似文献   

11.
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12.
Soil vapor extraction (SVE) is a prevalent remediation remedy for volatile organic compound (VOC) contaminants in the vadose zone. To support selection of an appropriate condition at which SVE may be terminated for site closure or for transition to another remedy, an evaluation is needed to determine whether vadose zone VOC contamination has been diminished sufficiently to keep groundwater concentrations below threshold values. A conceptual model for this evaluation was developed for VOC fate and transport from a vadose zone source to groundwater when vapor‐phase diffusive transport is the dominant transport process. A numerical analysis showed that, for these conditions, the groundwater concentration is controlled by a limited set of parameters, including site‐specific dimensions, vadose zone properties, and source characteristics. On the basis of these findings, a procedure was then developed for estimating groundwater concentrations using results from the three‐dimensional multiphase transport simulations for a matrix of parameter value combinations and covering a range of potential site conditions. Interpolation and scaling processes are applied to estimate groundwater concentrations at compliance (monitoring) wells for specific site conditions of interest using the data from the simulation results. The interpolation and scaling methodology using these simulation results provides a far less computationally intensive alternative to site‐specific three‐dimensional multiphase site modeling, while still allowing for parameter sensitivity and uncertainty analyses. With iterative application, the approach can be used to consider the effect of a diminishing vadose zone source over time on future groundwater concentrations. This novel approach and related simulation results have been incorporated into a user‐friendly Microsoft® Excel®‐based spreadsheet tool entitled SVEET (Soil Vapor Extraction Endstate Tool), which has been made available to the public.  相似文献   

13.
Natural source zone depletion (NSZD) has emerged as a practical alternative for restoration of light non‐aqueous phase liquid (LNAPL) sites that are in the later stages of their remediation lifecycle. Due to significant research, the NSZD conceptual model has evolved dramatically in recent years, and methanogenesis is now accepted as a dominant attenuation process (e.g., Lundegard and Johnson 2006 ; Ng et al. 2015 ). Most of the methane is generated within the pore space adjacent to LNAPL (Ng et al. 2015 ) from where it migrates through the unsaturated zone (e.g., Amos and Mayer 2006 ), where it is oxidized. While great progress has been made, there are still some important gaps in our understanding of NSZD. NSZD measurements provide little insight on which constituents are actually degrading; it is unclear which rate‐limiting factors that can be manipulated to increase NSZD rates; and how longevity of the bulk LNAPL and its key constituents can be predicted. Various threads of literature were pursued to shed light on some of the questions listed above. Several processes that may influence NSZD or its measurement were identified: temperature, inhibition from acetate buildup, protozoa predation, presence of electron acceptors, inhibition from volatile hydrocarbons, alkalinity/pH, and the availability of nutrients can all affect methanogenesis rates, while factors such as moisture content and soil type can influence its measurement. The methanogenic process appears to have a sequenced utilization of the constituents or chemical classes present in the LNAPL due to varying thermodynamic feasibility, biodegradability, and effects of inhibition, but the bulk NSZD rate appears to remain quasi‐zero order. A simplified version of the reactive transport model presented by Ng et al. 2015 has the potential to be a useful tool for predicting the longevity of key LNAPL constituents or chemical fractions, and of bulk LNAPL, but more work is needed to obtain key input parameters such as chemical classes and their biodegradation rates and any potential inhibitions.  相似文献   

14.
The vadose zone is the portion of the geologic profile above a perennial aquifer. Inclusion of mandatory vadose zone monitoring techniques as an approach to aquifer protect ion was first proposed under the Resource Conservation and Recovery Act in the United States in 1978 and has since received increasing acceptance at federal and stale levels. The goals of a vadose zone characterization and monitoring effort are to establish background conditions, identify contaminant transport pathways, identify the extent and degree of existing contamination, establish the basis for monitoring network design, measure the parameters needed in a risk assessment, and provide detection of contaminant migration toward ground water resources. The benefits of vadose zone monitoring include early warning of contaminant migration, potential reduction of ground water monitoring efforts, reduction of contaminant spreading and volume, and reduced time and cost of remediation once a contaminant release occurs. Vadose zone characterization and monitoring techniques should be considered as critical hydrologic tools in the prevention of ground water resource degradation.  相似文献   

15.
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   

16.
This research continues a 7-year study of oxygen-containing organic compounds present in groundwater at gasoline and diesel fuel release sites that are quantified as diesel-range “total petroleum hydrocarbons” when measured by methods utilizing solvent extraction and gas chromatography. Two-dimensional gas chromatography with time-of-flight mass spectrometry was used to tentatively identify 1162 compounds (TICs) in 113 groundwater samples from 22 sites. Samples were collected from wells either upgradient of the release, within the source zone, or downgradient of the source but still within the plume of dissolved organics associated with release. The names and formulas of all TICs found in samples from each well type are presented and the results from upgradient and downgradient locations are compared in detail. About 60% of the most frequently detected TICs in downgradient wells were also detected in upgradient wells. A majority of these were saturated straight chain alkyl acids, commonly called fatty acids, or fatty acid esters. Of TICs frequently detected in downgradient wells but not upgradient wells, over half were branched alkyl alcohols. Hierarchical cluster analysis results suggest about 80% of the chemical composition of downgradient samples is more similar to upgradient samples than to source area samples. This similarity is due to the presence of the same types of fatty acids and esters. Principal component analysis indicates a continuum of biodegradation between the source area and downgradient samples with the latter becoming more consistent with upgradient samples. Results suggest some TICs may not be petroleum degradation intermediates but compounds synthesized by microorganisms through secondary production and carbon cycling.  相似文献   

17.
The U.S. Environmental Protection Agency (EPA) recently proposed to amend federal regulations to require vadose zone monitoring at certain hazardous waste facilities. To support this proposal, EPA evaluated previous policy on vadose zone monitoring and examined advances in vadose zone monitoring technology. Changes in EPA vadose zone monitoring policy were driven by demonstrated advances in the available monitoring technology and improvements in understanding of vadose zone processes/When used under the appropriate conditions, currently available direct and indirect monitoring methods can effectively detect contamination that may leak from hazardous waste facilities into the vadose zone. Direct techniques examined include soil-core monitoring and soil-pore liquid monitoring. Indirect techniques examined include soil-gas monitoring, neutron moderation, complex resistivity, ground-penetrating radar, and electrical resistivity. Properly designed vadose zone monitoring networks can act as a complement to saturated zone monitoring networks at numerous hazardous waste facilities. At certain facilities, particularly those in arid climates where the saturated zone is relatively deep, effective vadose zone monitoring may allow a reduction in the scope of saturated zone monitoring programs.  相似文献   

18.
Bayless ER 《Ground water》2001,39(2):169-180
The vadose zone was examined as an environmental compartment where significant quantities of atrazine and its degradation compounds may be stored and transformed. The vadose zone was targeted because regional studies in the White River Basin indicated a large discrepancy between the mass of atrazine applied to fields and the amount of the pesticide and its degradation compounds that are measured in ground and surface water. A study site was established in a rotationally cropped field in the till plain of central Indiana. Data were gathered during the 1994 growing season to characterize the site hydrogeology and the distribution of atrazine, desethylatrazine, deisopropylatrazine, didealkylatrazine and hydroxyatrazine in runoff, pore water, and ground water. The data indicated that atrazine and its degradation compounds were transported from land surface to a depth of 1.5 m within 60 days of application, but were undetected in the saturated zone at nearby monitoring wells. A numerical model was developed, based on the field data, to provide information about processes that could retain and degrade atrazine in the vadose zone. Simulations indicated that evapotranspiration is responsible for surface directed soil-moisture flow during much of the growing season. This process causes retention and degradation of atrazine in the vadose zone. Increased residence time in the vadose zone leads to nearly complete transformation of atrazine and its degradation products to unquantified degradation compounds. As a result of macropore flow, small quantities of atrazine and its degradation compounds may reach the saturated zone.  相似文献   

19.
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   

20.
The system assessment capability (SAC) is the first total-system stochastic simulator to address inventory distribution, environmental release and transport, and impacts to human health and ecological, economic, and cultural resources from hundreds of radiological and chemical waste disposal sites for the entire Hanford Site in southeast Washington State. Flow and contaminant transport modeling in the vadose zone at 720 individual sites has been integrated into the SAC stochastic software framework using the STOMP code, providing the means to define release to the regional aquifer to support the SAC groundwater transport model. Important features, events, and processes including remedial actions, time-variant natural infiltration rates, and high volume aqueous-phase discharges were addressed in the software and data. A separate data extraction program, VZGRAB, was developed to enable analysts to aggregate vadose zone release data across the hundreds of waste sites in various ways following a SAC simulation to develop an improved understanding of the system performance and uncertainty aspects.  相似文献   

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