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1.
The partitioning and bioaccumulation of polycyclic aromatic hydrocarbons (PAHs) in water, suspended particulate matter (SPM), and fish samples from the Dongjiang River (DR), Pearl River (PR), and the Pearl River Estuary (PRE) were examined. Although PAHs are much lower in PRE than in DR or PR, PAHs in some fish species are significantly higher in PRE than in DR or PR. Aqueous or particulate PAHs respectively show significant correlations with dissolved organic carbon, particulate organic matter, and chlorophyll a, suggesting that biological pumping effect regulates their distribution. The in situ partitioning coefficients (log Koc) for PAHs are one order magnitude higher than the empirical log Koc–log Kow correlation. The bioconcentration factor (BCF) is slightly higher for the marine fish than for the freshwater fish. The above phenomena indicate that BCF may vary due to the diversity of fish species, feeding habits, and metabolism of PAHs in fish.  相似文献   

2.
Micellar-enhanced ultrafiltration (MELT) and air stripping were evaluated for surfactant-contaminant separation and surfactant recovery. Two linear alkyl diphenyloxide disulfonate (DPDS) surfactants were evaluated with the contaminants naphthalene and trichloroethylene. A separation model developed from micellar partitioning principles showed a good correlation to batch MEUF studies, whereas flux analysis highlighted concentration polarization effects in relation to hydrophobe length. MEUF effectively concentrated the surfactant-contaminant system (93 to 99 percent retention); however, this did not result in surfactant-contaminant separation. Batch and continuous flow air stripping models were developed based upon air/water ratio, surfactant concentration, and Micellar partitioning; model predictions were validated by experimental data. Sensitivity analyses illustrated the decline in contaminant-surfactant separation with increasing surfactant concentration (e.g., TCE removal efficiency declines from 83 percent to 37 percent as C-16 DPDS concentration increases from 0 to 55 mM). This effect is greater for more hydrophobic contaminants (naphthalene vs. TCE) and surfactants with greater solubilization potential (C16-DPDS vs. C-12 DPDS). The resulting design equations can account for this effect and thus properly size air strippers to achieve the desired removal efficiency in the presence of surfactant micelles. Proper selection and design of surfactant-contaminant separation and surfactant recovery systems are integral to optimizing surfactant-enhanced subsurface remediation.  相似文献   

3.
Organic contaminants present as nonaqueous phase liquids (NAPLs) in the subsurface often pose a long-term risk to human health and the environment. Investigating the distribution of NAPLs in porous media remains a major challenge in risk assessment and management of contaminated sites. Conventional soil coring and monitoring wells have been widely used over past decades as the primary means of subsurface investigation to determine NAPL extent. Known limitations of conventional approaches have led us to explore an alternative or a complementary technique to provide high-quality information of NAPL source zone architecture. This work advances an imaging tool for a variety of organic NAPL contaminants in unconsolidated soils through magnetic resonance imaging (MRI) of frozen cores. Using trichloroethylene (TCE) and o-xylene as model species, we illustrate that discriminatory freezing of water, while keeping the NAPL in a liquid state, enables high-resolution qualitative delineation of NAPL distribution within porous media. This novel approach may help improve site conceptual models and consequentially lead to highly tailored, more efficient remedial measures.  相似文献   

4.
Grain size analysis and permeametry are common methods for estimating the hydraulic conductivity (K) of porous media. It is well known that these methods have limited accuracy when they are used to characterize natural sediments. However, hydrogeological research has increasingly introduced technologies dependent on engineered porous media that may be less problematic because complex geologic structures are eliminated in the lab and field-scale packings. The recently introduced Horizontal Reactive Media Treatment Wells (HRX® Wells), for in situ, passive remediation of groundwater is one such example. The HRX Well passively collects groundwater and directs it through a horizontal pipe packed with an engineered porous medium. In this project, grain size analysis was conducted for sand and sand-iron mixtures to estimate K using the 16 algorithms provided in the HydrogeoSieveXL2.3.2 software. The results were compared to K determined by permeametry and a field-scale column, 30 cm long and 25 cm in diameter, representing an HRX Well. The best comparability of K estimates from grain size analysis and permeametry were obtained using the USBR, Slichter, and Shepherd K estimation methods. These also showed good agreement between lab-scale and field-scale K estimations, with reproducibility within the range ±20%. This study shows that laboratory K estimations can be representative across various relevant scales, including the field-scale, for engineered porous media. This finding extends to filter packs, and other engineered porous media design methods by emphasizing and demonstrating one case of accuracy in lab-scale permeability estimation for field-scale implementations.  相似文献   

5.
Conflicting sorption coefficients for ortho‐phenylphenol (OPP) have been reported in the literatures, which resulted in the conflicting assessments on OPP mobility in soil. To ascertain the sorption coefficient of OPP, batch experiments were performed based on OECD guideline 106, using three types of soils. Headspace solid‐phase microextraction (HS‐SPME) and GC‐MS were applied to the determination of OPP concentration in the liquid phase. The sorption isotherms obtained for all three soils under equilibrium conditions were described well, assuming linear sorption. The organic carbon normalized distribution coefficients (Koc) ranged from 894 to 1703 L kg?1, which suggested that OPP is moderately mobile in soil. The results also showed that the Koc value of OPP can be predicted precisely from Kow, whereas it was underestimated by one order of magnitude when water solubility is used.  相似文献   

6.
The fate and transport of highly hydrophobic chemicals are affected by the partitioning between water and dissolved organic carbon. Large variation in the partition coefficient (KDOCw) is often found, due to the selection of model organic matter or potential experimental artifacts. To investigate the roles of the type of organic matter on the partitioning of highly hydrophobic compounds, the partition coefficients of eight selected polycyclic aromatic hydrocarbons (PAHs), with 3–6 aromatic rings, were determined using a passive dosing/extraction method between water and model dissolved organic matter (humic acid, fulvic acid, sodium dodecyl sulfate micelle (SDS), and 2‐hydroxypropyl‐β‐cyclodextrin). Although the KDOCw values for 3–4 ring PAHs in this study were close to those reported in the literature, experimental KDOCw values between Aldrich humic acid (AHA) and water were higher than values reported in the literature for 5–6 ring PAHs. The KDOCw values were highest for AHA, followed by SDS and Suwannee river fulvic acid (SFA). The slopes of the linear regression between log KDOCw and log Kow were 1.23 (± 0.13), 0.82 (± 0.09), and 0.59 (± 0.13) for AHA, SDS, and SFA, respectively. The differences in the KDOCw values between AHA and the other organic matter (SDS, SFA, and CD) increased with increasing hydrophobicity of the PAHs, showing that the sorption of highly hydrophobic chemicals to the humic acid fraction may be important in the presence of mixed organic matter.  相似文献   

7.
In this study, we tested a practical strategy useful for accurate chlorinated volatile organic compound (cVOC) sorption prediction. Corresponding to the feature of the superposition of adsorption due to thermally altered carbonaceous matter (TACM) with organic carbon‐water partitioning, a nonlinear Freundlich sorption isotherm covering a wide range of aqueous concentrations was defined by equilibrium sorption measurement at one or a few low concentration points with extrapolation to the empirical organic carbon‐water partition coefficient (Koc,e) near compound solubility. We applied this approach to obtain perchloroethene equilibrium sorption isotherm parameters for TACM‐containing glacial sand and gravel subsoil samples from a field site in New York. Sorption and associated Koc,c applicable to low (5–500 µg/L) and high (>100,000 µg/L) aqueous concentrations were determined in batch experiments. (The Koc,c is the organic carbon‐normalized sorption partition coefficient corresponding to aqueous concentration Cw.) The Koc,c measurements at low concentration (~5 µg/L) were 6 to 34 times greater than the Koc,e. The importance of this type of data is illustrated through presentation of its substantial impact on the site remedy. In so doing, we provide an approach that is broadly applicable to cVOC field sites with similar circumstances (low carbon content glacial sand and gravel with TACM).  相似文献   

8.
Remediation of subsurface contamination requires an understanding of the contaminant (history, source location, plume extent and concentration, etc.), and, knowledge of the spatial distribution of hydraulic conductivity (K) that governs groundwater flow and solute transport. Many methods exist for characterizing K heterogeneity, but most if not all methods require the collection of a large number of small‐scale data and its interpolation. In this study, we conduct a hydraulic tomography survey at a highly heterogeneous glaciofluvial deposit at the North Campus Research Site (NCRS) located at the University of Waterloo, Waterloo, Ontario, Canada to sequentially interpret four pumping tests using the steady‐state form of the Sequential Successive Linear Estimator (SSLE) ( Yeh and Liu 2000 ). The resulting three‐dimensional (3D) K distribution (or K‐tomogram) is compared against: ( 1 ) K distributions obtained through the inverse modeling of individual pumping tests using SSLE, and ( 2 ) effective hydraulic conductivity (Keff) estimates obtained by automatically calibrating a groundwater flow model while treating the medium to be homogeneous. Such a Keff is often used for designing remediation operations, and thus is used as the basis for comparison with the K‐tomogram. Our results clearly show that hydraulic tomography is superior to the inversions of single pumping tests or Keff estimates. This is particularly significant for contaminated sites where an accurate representation of the flow field is critical for simulating contaminant transport and injection of chemical and biological agents used for active remediation of contaminant source zones and plumes.  相似文献   

9.
The potential for trichloroethene (TCE) biodegradation in a fractured dolomite aquifer at a former chemical disposal site in Smithville, Ontario, Canada, is assessed using chemical analysis and TCE and cis‐DCE compound‐specific isotope analysis of carbon and chlorine collected over a 16‐month period. Groundwater redox conditions change from suboxic to much more reducing environments within and around the plume, indicating that oxidation of organic contaminants and degradation products is occurring at the study site. TCE and cis‐DCE were observed in 13 of 14 wells sampled. VC, ethene, and/or ethane were also observed in ten wells, indicating that partial/full dechlorination has occurred. Chlorine isotopic values (δ37Cl) range between 1.39 to 4.69‰ SMOC for TCE, and 3.57 to 13.86‰ SMOC for cis‐DCE. Carbon isotopic values range between ?28.9 and ?20.7‰ VPDB for TCE, and ?26.5 and ?11.8‰ VPDB for cis‐DCE. In most wells, isotopic values remained steady over the 15‐month study. Isotopic enrichment from TCE to cis‐DCE varied between 0 and 13‰ for carbon and 1 and 4‰ for chlorine. Calculated chlorine‐carbon isotopic enrichment ratios (?Cl/?C) were 0.18 for TCE and 0.69 for cis‐DCE. Combined, isotopic and chemical data indicate very little dechlorination is occurring near the source zone, but suggest bacterially mediated degradation is occurring closer to the edges of the plume.  相似文献   

10.
Remediation of groundwater contaminated by chlorinated hydrocarbons via in situ technologies such as direct injection of nanoscale zero valent iron (ZVI, Fe(O)) particles is increasingly common. However, assessing target compound degradation by abiotic processes is difficult because (1) the injection may displace the contaminant plume so that concentration measurements alone are often inconclusive and (2) biodegradation may also occur, making it challenging to identify and evaluate the abiotic degradation component. In this study, trichloroethylene (TCE) and 1,1,1-trichloroethane (1,1,1-TCA) were treated in a highly heterogeneous hydrogeologic setting. The purpose of this study was to evaluate the potential for compound-specific stable isotope analysis (CSIA) to monitor the effectiveness of ZVI injection by assessing TCE and 1,1,1-TCA degradation. Prior to ZVI injection, carbon isotope measurements demonstrated biodegradation of TCE by native microorganisms. This in situ biodegradation was quantified by measuring the enrichment of 13C in TCE samples downstream of the suspected source. When ZVI was injected through only two injection wells, no changes in TCE and 1,1,1-TCA isotope signatures were detected compared to preinjection values. In contrast, when ZVI was injected through 11 wells covering a greater portion of the contaminated area, 5 out of 10 monitoring wells showed further enrichment of 13C in either TCE or 1,1,1-TCA, indicating additional target compound transformation. The abiotic nature of this TCE transformation was confirmed through temporal trends in carbon isotope values of the putative transformation products cis-dichloroethylene (cis-DCE), ethene and ethane. This demonstrates the usefulness of CSIA in distinguishing abiotic vs. biotic transformation in the field.  相似文献   

11.
《Marine pollution bulletin》2012,64(5-12):578-582
Hydrophobic organic contaminants in marine water are mostly adsorbed onto (partitioned into) sediment organic matter (SOM). To study the impact of SOM diagenesis on sediment adsorption properties, artificial sediment with rich SOM content was incubated for more than 120 days. The sediment was sampled every week, and batch sediment adsorption tests were conducted with bisphenol A (BPA) and nonylphenol (NP) as the model pollutants. The results show that the amount of organic matter loaded in the sediment decreased by nearly 80% during incubation. For the incubated sediment, the BPA partition coefficient, Kd, decreased whereas the organic normalized partition coefficient, Koc, more than doubled. The experiments with NP show an even greater increase in Koc. Organic matter diagenesis shows a profound effect on the adsorption behavior of sediment, as the SOM residue has an increasing affinity and partition capacity for organic contaminants.  相似文献   

12.
Volatile organic compounds (VOCs) am be removed from contaminated ground water and subsurface media by surfaclant-enhanced remediation processes. For the process to be economically competitive it is necessary to recover and reuse the surfactant from this concentrated solution. The VOC can be removed from this concentrated solution by flash vacuum stripping, leaving the surfactant solution for reuse. In this study, the flash vacuum stripping of trichloroethylene (TCE) from an anionic surfactant solution in a co-current packed column was studied under rough vacuum conditions. The presence of surfactants lead to a reduction in the overall liquid phase volumetric mass transfer coefficient (MTC) of 40 to 95%. depending on flow rate and surfactant concentration at 50°C and 16 kPa. At liquid loading rates of less than 13 cm3/cm2min, the MTC of TCE decreases rapidly with an increase in liquid loading rate, and at liquid loading rates above that, the MTC decreases slightly with an increase in the liquid loading rate. This trend may have been due to foaming. At surfactant concentrations above the critical micelle concentration, the effect of surfactant concentration was not significant at liquid loading rates less than 13 cm3/cm2min. However, beyond that rate, the MTC of TCE decreased drastically with an increase in surfactant concentration. The MTC of TCE increased with an increase in temperature. A large pressure drop (3 to 4 kPa/m) was observed across the packed bed due to foaming.  相似文献   

13.
During thermally enhanced in situ remediation of soils and ground water, gas streams are generated with varying temperatures, moisture content, and organic compound concentrations. In this study, we evaluated the performance of tin dioxide sensors for measuring trichloroethylene (TCE) concentrations in gas streams from a thermally enhanced soil vapor extraction system. Temperature, pressure, moisture content, and vapor flow rates affected the resistivity of the sensors, and thus the signal. When fluctuations in these parameters were eliminated by condensing excess water and healing to a constant temperature prior to measurement, the sensors provided reliable in-line measurement of TCE concentrations. Gas tracers such as methane were easily monitored in-line, providing quick and inexpensive data on subsurface vapor flow velocities and direction.  相似文献   

14.
Surfactant-Induced Reductions in Soil Hydraulic Conductivity   总被引：2，自引：0，他引：2  
Surfactant solutions are being proposed for in situ flushing of organic contaminants from soils and aquifers. The feasibility of surfactant additives in remediation may depend in large part on how these chemicals affect the hydraulic conductivity of the porous media. While there is evidence in the literature of conductivity loss during surfactant flushing (Miller et al. 1975; Nash et al. 1987), there has been little research on quantifying the process for unconsolidated sediments. Surfactant-affected hydraulic conductivity reductions were measured in two soils (Teller loam and Daugherty sand). Testing was done with eight surfactants at a variety of concentrations (10-5 to 10-l mole/kg), surfactant mixtures, and added solution electrolytes. The Teller was also tested with its organic matter removed. Maximum hydraulic conductivity decreases were 47 percent for the sand and more than two orders of magnitude for the loam. Surfactant concentrations, surfactant mixtures, soil organic content, and added solution electrolytes all affected the degree of conductivity reduction. Results indicate that surfactant-affected hydraulic conductivity losses should be considered prior to in situ remediation and may preclude surfactant use in some fine grain soils.  相似文献   

15.
Saturated hydraulic conductivity (K) is one of the most important parameters determining groundwater flow and contaminant transport in both unsaturated and saturated porous media. Although several well‐established laboratory methods exist for determining K, in situ measurements of this parameter remain very complex and scale dependent. Often, the limited accessibility of subsurface sediments for sampling means an additional impediment to our ability to quantify subsurface K heterogeneity. One potential solution is the use of outcrops as analogues for subsurface sediments. This paper investigates the use of air permeameter measurements on outcrops of unconsolidated sediments to quantify K and its spatial heterogeneity on a broad range of sediment types. The Neogene aquifer in northern Belgium is used as a case study for this purpose. To characterize the variability in K, 511 small‐scale air permeability measurements were performed on outcrop sediments representative over five of the aquifer's lithostratigraphic units. From these measurements, outcrop‐scale equivalent K tensors were calculated using numerical upscaling techniques. Validation of the air permeameter‐based K values by comparison with laboratory constant head K measurements reveals a correlation of 0.93. Overall, the results indicate that hand‐held air permeameters are very efficient and accurate tools to characterize saturated K, as well as its small‐scale variability and anisotropy on a broad range of unconsolidated sediments. The studied outcrops further provided a qualitative understanding of aquifer hydrostratigraphy and quantitative estimates about K variability at the centimetre‐scale to metre‐scale. Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   

16.
Yang Y  Liu M  Wang L  Fu J  Yan C  Zhou JL 《Marine pollution bulletin》2011,62(5):1025-1031
In the present study, phenanthrene was chosen as the probe compound for determining the sorption of PAHs in sediments from Yangtze estuary and nearby coastal area, China. Sorption isotherms were fitted well by the Freundlich and dual models, respectively. Selected sediments were further sequentially separated to remove the carbonate and organic carbon (OC). Calculated OC sorption capacity values based on both H2O2 oxidization and 375 °C combustion methods were similar and comparable to the Koc values estimated by the empirical linear sorption equations. Both sorption models and sorption data using sequentially separated samples achieve the similar conclusions: (1) the partition behavior dominated by OC in sediments with foc > 0.01; (2) for sediments with 0.001 < foc < 0.01, OC dominated sorption at relatively high aqueous concentration; whereas mineral phase adsorption dominated sorption at lower concentration especially when Cw/Sw was in the range of 0.0001-0.001 in natural aqueous system.  相似文献   

17.
How to restore the residual organic carbon and residual hydrocarbon-generating potential is discussed based on the hydrocarbon degradability of source rock. The results indicate there is linear function relationship between the restoring coefficient of residual organic carbon (Kc) and the vitrinite reflectance (R o%) of various kinds of source rock, but the relationship is secondary functional between the restoring coefficient of residual hydrocarbon-generating potential (Ks) and the vitrinite reflectance (R o%). It is pointed out thatKc = (1 -Dresidual)/(1 -D primary),Ks= Kc (D primary/D residual). The restoration of residual organic carbon and hydrocarbon-generating potential of the Cambrian and Ordovician highly mature marine carbonate in the Tarim Basin and North China region shows that the lower limit value of hydrocarbon generating potential and the organic matter abundance of carbonate source rock are basically the same as that of clastic rock. The technical difficulty in hydrocarbon generating evaluation of highly mature and overmature carbonate is solved.  相似文献   

18.
We present the first demonstration of hydraulic tomography (HT) to estimate the three-dimensional (3D) hydraulic conductivity (K) distribution of a fractured aquifer at high-resolution field scale (HRFS), including the fracture network and connectivity through it. We invert drawdown data collected from packer-isolated borehole intervals during 42 pumping tests in a wellfield at the former Naval Air Warfare Center, West Trenton, New Jersey, in the Newark Basin. Five additional tests were reserved for a quality check of HT results. We used an equivalent porous medium forward model and geostatistical inversion to estimate 3D K at high resolution (K blocks <1 m3), using no strict assumptions about K variability or fracture statistics. The resulting 3D K estimate ranges from approximately 0.1 (highest-K fractures) to approximately 10−13 m/s (unfractured mudstone). Important estimated features include: (1) a highly fractured zone (HFZ) consisting of a sequence of high-K bedding-plane fractures; (2) a low-K zone that disrupts the HFZ; (3) several secondary fractures of limited extent; and (4) regions of very low-K rock matrix. The 3D K estimate explains complex drawdown behavior observed in the field. Drawdown tracing and particle tracking simulations reveal a 3D fracture network within the estimated K distribution, and connectivity routes through the network. Model fit is best in the shallower part of the wellfield, with high density of observations and tests. The capabilities of HT demonstrated for 3D fractured aquifer characterization at HRFS may support improved in situ remediation for contaminant source zones, and applications in mining, repository assessment, or geotechnical engineering.  相似文献   

19.
This study involved a baseline evaluation of fluvial carbon export and degas rates in three nested rural catchments (1 to 80 km2) in Taboão, a representative experimental catchment of the Upper Uruguay River Basin. Analyses of the carbon content in stream waters and the catchment carbon yield were based on 4‐year monthly in situ data and statistical modeling using the United States Geological Survey load estimator model. We also estimated p CO2 and degas fluxes using carbonate equilibrium and gas‐exchange formulas. Our results indicated that the water was consistently p CO2 saturated (~90% of the cases) and that the steep terrain favors high gas evasion rates. The mean calculated fluvial export was 5.4 tC·km?2·year?1 with inorganic carbon dominating (dissolved inorganic carbon:dissolved organic carbon ratio >4), and degas rates (~40 tC km?2·year?1) were nearly sevenfold higher than the downstream export. The homogeneous land use in this nested catchment system results in similar water‐quality characteristics, and therefore, export rates are expected to be closely related to the rainfall–runoff relationships at each scale. Although the sampling campaigns did not fully reproduce storm‐event conditions and related effects such as flushing or dilution of in‐stream carbon, our results indicated a potential link between dissolved inorganic carbon and slower hydrological pathways related to subsurface water storage and movement.  相似文献   

20.
The characterization of heterogeneity in hydraulic conductivity (K) is a major challenge for subsurface remediation projects. There are a number of field studies that compare the K estimates obtained using various techniques, but to our knowledge, no field‐based studies exists that compare the performance of estimated K heterogeneity fields or the associated characterization costs. In this paper, we compare the costs of characterizing the three‐dimensional K heterogeneity and its uncertainty estimates of a glaciofluvial aquifer‐aquitard sequence at a 15 m × 15 m × 18 m field site situated on the University of Waterloo campus. We compare geostatistical analysis of high resolution permeameter K data obtained from repacked core samples in five boreholes and hydraulic tomography analysis of four pumping tests consisting of up to 41 monitoring points per test. Aside from the comparison of costs, we also assess the performance of each method by predicting several pumping tests. Our analysis reveals that hydraulic tomography is somewhat more costly than the geostatistical analysis of high resolution permeameter K data due to the higher capital costs associated with the method. However, the equipment may be reused at other sites; hence these costs may be recovered over the life of the equipment. More significantly, hydraulic tomography is able to capture the most important features of the aquifer‐aquitard sequence leading to more accurate predictions of independent pumping tests. This suggests that more robust remediation systems may be designed if site characterization is performed with hydraulic tomography.  相似文献   

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