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1.
《Marine pollution bulletin》2013,77(1-2):139-145
The sorption of phenanthrene on the Yangtze Estuary sediment was studied under varying conditions of particle size, sediment organic contents, salinity, and dissolved organic matter (DOM) concentrations. Small sediment particles showed higher trapping capacity for phenanthrene due to the higher organic contents associated. The organic carbon-based partition coefficient of phenanthrene to the Yangtze Estuary sediment was obtained as 7120 L/kg, lower than the values for other soils or sediments reported in previous studies. The magnitude and direction of the salt effect were complicated by the specific DOM studied. The sediment sorption capacity was greatly increased in saline water in the absence of DOM but decreased in the presence of DOM. Given the conditions in the Yangtze Estuary, the equilibrium sorption of phenanthrene would be decreased with increasing salinity. Overall, the nature and content of both sediment-bound and dissolved organic matter dominate the sorption of hydrophobic organic contaminants in the estuary. 相似文献
2.
Modelling and experimental study of coupled exchange of p,p′‐DDE and colloids in a flume simulated stream–streambed system 
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下载免费PDF全文 Stream–subsurface exchange plays a significant role in the fate and transport of contaminants in streams. It has been modelled explicitly by considering fundamental processes such as hydraulic exchange, colloid filtration, and contaminant interactions with streambed sediments and colloids. The models have been successfully applied to simulate the transport of inorganic metals and nutrients. In this study, laboratory experiments were conducted in a recirculating flume to investigate the exchange of a hydrophobic organic contaminant, p,p′‐dichloro‐diphenyl‐dichloroethane (DDE), between a stream and a quartz sand bed. A previously developed process‐based multiphase exchange model was modified by accounting for the p,p′‐DDE kinetic adsorption to and desorption from the bed sediments/colloids and was applied to interpret the experimental results. Model input parameters were obtained by conducting independent small‐scale batch experiments. Results indicate that the immobilization of p,p′‐DDE in the quartz sand bed can occur under representative natural stream conditions. The observed p,p′‐DDE exchange was successfully simulated by the process‐based model. The model sensitivity analysis results show that the exchange of p,p′‐DDE can be sensitive to either the sediment sorption/desorption parameters or colloidal parameters depending on the experimental conditions tested. For the experimental conditions employed here, the effect of colloids on contaminant transport is expected to be minimal, and the stream–subsurface exchange of p,p′‐DDE is dominated by the interaction of p,p′‐DDE with bed sediment. The work presented here contributes to a better mechanistic understanding of the complex transport process that hydrophobic organic contaminants undergo in natural streams and to the development of reliable, predictive models for the assessment of impacted streams. Copyright © 2015 John Wiley & Sons, Ltd. 相似文献
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This article summarizes several of many field-based studies of subsurface contaminant transport conducted over the last 30 years at the Canadian Forces Base (CFB) Borden site. The field research initially consisted of extensive monitoring of a leachate plume from an abandoned landfill and its analytical and numerical modeling. Lessons learned from these initial studies led to the execution and interpretation of a variety of tracer tests involving conservative and reactive/organic solutes tests performed at various scales. The lessons learned from these tracer tests revealed a number of deficiencies in classical theories of contaminant dispersion and reaction processes as they occur in groundwater, and thus spawned a new era of process-oriented research within the hydrogeological community. The extensively monitored tracer tests were followed by controlled spills of organic contaminants to observe their subsurface movement and distribution as well as the emplacement of a variety of contaminant sources in the saturated and unsaturated zones to study the ambient transport of contaminants. The controlled spills and emplaced sources of various contaminants were then utilized for testing various active and passive remediation technologies. These studies have led to fundamental insights and lessons learned that have significantly contributed to research on contaminant transport in both the saturated and unsaturated zones. Over the years, data generated by the University of Waterloo (UW) researchers and their collaborators continues to be examined by various research groups and has led to additional new insights on subsurface transport of various chemicals. 相似文献
4.
《Acta Geochimica》2016,(3)
In order to better understand the compositional and structural complexity of dissolved organic matter(DOM) macromolecules and provide mechanistic information on the binding of hydrophobic organic contaminants(HOCs) to DOM, we fractionated large amounts of lake water into three hydrophobic DOM-fractions. The variation of the partitioning coef?cients(K_(DOC)) of pyrene at different p H levels was examined by ?orescence quenching titration. Results show that, relative to the more polar acidic DOM-fractions, the hydrophobic neutral fraction exhibits a higher sorption ability to pyrene. Generally, the sorption of pyrene to the three hydrophobic fractions is strongly pH-dependent. The K_(DOC) values of pyrene generally increase with decreasing p H levels, which is especially obvious in the sorption of pyrene to the fulvic acid fractions, suggesting that the binding is controlled by hydrophobic interactions. The mechanisms underlying the binding of pyrene to the hydrophobic fractions were also discussed. Our data are bene?cial to further understanding the binding of HOCs to DOM and how it has been affected,which may result in more accurate predictions of K_(DOC). 相似文献
5.
Jack C. Parker 《Ground Water Monitoring & Remediation》2003,23(1):107-120
A model is presented for estimating vapor concentrations in buildings because of volatilization from soil contaminated by non- aqueous phase liquids (NAPL) or from dissolved contaminants in ground water. The model considers source depletion, diffusive- dispersive transport of the contaminant of concern (COC) and of oxygen and oxygen-limited COC biodecay. Diffusive-advective transport through foundations and vapor losses caused by foundation cross-flow are considered. Competitive oxygen use by various species is assumed to be proportional to the product of the average dissolved-phase species concentration and a biopreference factor. Laboratory and field data indicate the biopreference factor to be proportional to the organic carbon partition coefficient for the fuel hydrocarbons studied. Predicted indoor air concentrations were sensitive to soil type and subbase permeability. Lower concentrations were predicted for buildings with shallow foundations caused by flushing of contaminants by cross-flow. NAPL source depletion had a large impact on average exposure concentration. Barometric pumping had a minor effect on indoor air emissions for the conditions studied. Risk-based soil cleanup levels were much lower when biodecay was considered because of the existence of a threshold source concentration below which no emissions occur. Computed cleanup levels at NAPL-contaminated sites were strongly dependent on total petroleum hydrocarbon (TPH) content and COC soil concentration. The model was applied to two field sites with gasoline-contaminated ground water. Confidence limits of predicted indoor air concentrations spanned approximately two orders of magnitude considering uncertainty in model parameters. Measured contaminant concentrations in indoor air were within model-predicted confidence limits. 相似文献
6.
Modeling the spread of subsurface contaminants requires coupling a groundwater flow model with a contaminant transport model. Such coupling may provide accurate estimates of future subsurface hydrologic states if essential flow and contaminant data are assimilated in the model. Assuming perfect flow, an ensemble Kalman filter (EnKF) can be used for direct data assimilation into the transport model. This is, however, a crude assumption as flow models can be subject to many sources of uncertainty. If the flow is not accurately simulated, contaminant predictions will likely be inaccurate even after successive Kalman updates of the contaminant model with the data. The problem is better handled when both flow and contaminant states are concurrently estimated using the traditional joint state augmentation approach. In this paper, we introduce a dual estimation strategy for data assimilation into a one-way coupled system by treating the flow and the contaminant models separately while intertwining a pair of distinct EnKFs, one for each model. The presented strategy only deals with the estimation of state variables but it can also be used for state and parameter estimation problems. This EnKF-based dual state-state estimation procedure presents a number of novel features: (i) it allows for simultaneous estimation of both flow and contaminant states in parallel; (ii) it provides a time consistent sequential updating scheme between the two models (first flow, then transport); (iii) it simplifies the implementation of the filtering system; and (iv) it yields more stable and accurate solutions than does the standard joint approach. We conducted synthetic numerical experiments based on various time stepping and observation strategies to evaluate the dual EnKF approach and compare its performance with the joint state augmentation approach. Experimental results show that on average, the dual strategy could reduce the estimation error of the coupled states by 15% compared with the joint approach. Furthermore, the dual estimation is proven to be very effective computationally, recovering accurate estimates at a reasonable cost. 相似文献
7.
1 INTRODUCTION Sediments are the ultimate sink for many hydrophobic contaminants and represent biologically important environmental habitats. Exposure of the sediment-associated contaminants is not only influenced by the fate and transport of sediment but also is influenced by a variety of physical, chemical, and biological processes that involve no net movement of sediments. These processes include pore water transport processes such as advection and diffusion, and sediment mixing process… 相似文献
8.
Two-dimensional modeling of contaminant transport in porous media in the presence of colloids 总被引：3，自引：0，他引：3
It has long been known that colloids can facilitate the transport of contaminants in groundwater systems by reducing the effective retardation factor. A significant effort has been devoted to study colloid-facilitated contaminant transport during the past decade. Many of the previous studies were restricted to one-dimensional analyses and comparisons with finite-column experiments. In this work, a two-dimensional numerical model is developed and used to study the different interactions between colloids, contaminants, and porous media under homogeneous conditions. The numerical formulation of the model is based on discretizing mass balance equations and reaction equations using finite differences having a third-order, total variance-diminishing scheme for the advection terms. This scheme significantly reduces numerical dispersion and leads to greater accuracy compared to the standard central-differencing scheme. The model is tested against analytical solutions under simplified conditions as well as against experimental data, and the results are favorable. The model is used to investigate the impact of the various reaction rates and parameter values on the movement of contaminant plumes in two dimensions. The model is also used to investigate the hypothesis that colloids may increase the effective retardation factor of contaminant plumes. The analysis shows that assuming kinetic mass exchange between contaminant and colloids with constant reaction rate coefficients that are not related to the concentrations may lead to inaccurate results. These inaccurate results are exemplified in the finding that under the kinetic assumption the ratio of the initial concentration of colloids to the initial concentration of contaminant does not affect the amount of facilitation or retardation that occurs in the system. It is also found that colloids can increase the effective retardation factor for the contaminant under certain combinations of reaction rates and distribution coefficients. A quantitative empirical expression to identify whether colloids retard or facilitate the contaminant movement is presented. 相似文献
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A two-dimensional multicomponent reactive transport modeling approach was used to simulate contaminant transport and the evolution of redox processes at a large-scale kerosene-contaminated site near Berlin, Germany. In contrast to previous site-scale modeling studies that focused either on one or two contaminants or on steady-state redox conditions, multiple contaminants and electron acceptors, including mineral phase Iron (III), were considered with an evolving redox zonation. Inhibition terms were used to switch between the different electron acceptor processes in the reaction scheme. The transient evolution of redox zones and contaminant plumes was simulated for two separate transects of the site, which have different geology and ground water recharge distributions and where quite different downstream contaminant and terminal electron–accepting process (TEAP) distributions are observed. The same reaction system, calibrated to measured concentrations along one of the transects, was used in both cases, achieving a reasonable match with observed concentrations. The differences between the two transects could thus to some extent be attributed to the different hydrological and hydrogeological conditions, in particular ground water recharge distributions. Long-term simulations showed that the distribution of TEAPs evolves as Fe(III) becomes depleted, with conditions becoming increasingly methanogenic, leading to changes in contaminant plume lengths. The models were applied to assess the potential effects of planned changes in land use at the site that may affect the ground water recharge distribution. The simulated redox zonation responded strongly to changes in recharge, which in turn led to changes in the contaminant plume lengths. 相似文献
11.
The effect of vertical turbulent mixing on the dynamics of persistent organic pollutants has long been overlooked and its role is still hardly understood. Here we present the first comprehensive analysis of the role of turbulent diffusion on the distribution of those contaminants and its interplay with sinking fluxes. To this end, a 1D dynamic coupled hydrodynamic-contaminant model has been developed and applied to a Mediterranean continental shelf environment. The hydrodynamic sub-model is adapted from COHERENS, the contaminant sub-model is an improvement from the BIODEP model and considers the contaminant in 3 phases: dissolved-colloidal-particulate. The simulation highlights the role of turbulence in determining the POP distribution and variability in the water column. In short, turbulent flux of contaminants strengthens the upward diffusion of sediment entrained contaminants and determines the extent to which inputs from the atmosphere mix into the water column. It acts in parallel with degradation and sinking fluxes, the combined effect yielding a surface enriched - depth depleted - benthic layer enriched region distribution, which presents similarities to reported experimental measures. 相似文献
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The desorption of contaminants from soils/sediments is one of the most important processes controlling contaminant transport and environmental risks. None of the currently adopted desorption models can accurately quantify desorption at relatively low concentrations; these models often overestimate the desorption and thus the risks of hydrophobic organic chemicals, such as benzene and chlorinated solvents. In reality, desorption is generally found to be biphasic, with two soil-phase compartments. A new dual-equilibrium desorption (DED) model has been developed to account for the biphasic desorption. This model has been tested using a wide range of laboratory and field data and has been used to explain key observations related to underground storage tank plumes. The DED model relates the amount of a chemical sorbed to the aqueous concentration, with simple parameters including octanol-water partition coefficient, solubility, and fractional organic carbon; thus, it is the only biphasic model, to date, that is based on readily available parameters. The DED model can be easily incorporated into standard risk and transport models. According to this model, many regulatory standards of soils and sediments could be increased without increasing the risks. 相似文献
14.
《Ground Water Monitoring & Remediation》2000,20(1):94-103
Reagents that enhance the aqueous solubility of non-aqueous phase organic liquid (NAPL) contaminants are under investigation for use in enhanced subsurface remediation technologies. Cyclodextrin, a glucose-based molecule, is such a reagent. In this paper, laboratory experiments and numerical model simulations are used to evaluate and understand the potential remediation performance of cyclodextrin. Physical properties of cyclodextrin solutions such as density, viscosity, and NAPL-aqueous inter-facial tension are measured. Our analysis indicates that no serious obstacles exist related to fluid properties that would prevent the use of cyclodextrin solutions for subsurface NAPL remediation. Cyclodextrin-enhanced solubilization for a large suite of typical ground water contaminants is measured in the laboratory, and the results are related to the physicochemical properties of the organic compounds. The most-hydrophobic contaminants experience a larger relative solubility enhancement than the less-hydrophobic contaminants but have lower aqueous-phase apparent solubilities. Numerical model simulations of enhanced-solubilization flushing of NAPL-contaminated soil demonstrate that the more-hydrophilic compounds exhibit the greatest mass-removal rates due to their greater apparent solubilities, and thus are initially more effectively removed from soil by enhanced-solubilization-flushing reagents. However, the relatively more hydrophobic contaminants exhibit a greater improvement in contaminant mass-removal (compared with water flushing) than that exhibited for the relatively hydrophilic contaminants. 相似文献
15.
Previous field and laboratory studies showed that organically bound nutrients can contribute largely to the export of N, P, and S from soil into aquatic systems. One possible determinant for the losses of dissolved organic nutrients leaving the soil environment could be their distribution between dissolved organic matter (DOM) fractions of different mobility in soil. To elucidate the potential influence of DOM fractions under varying flow conditions on the vertical translocation of organically bound nutrients, we determined the concentrations and fluxes of dissolved organic C (DOC) and nutrients (DON, DOP, DOS) in soil water under a Scots pine (Pinus sylvestris L.) and a European beech (Fagus sylvatica L.) forest. We sampled seepage water from the organic forest floor layer and the mineral subsoil using zero‐tension lysimeters and soil pore water using tension lysimeters and suction cups. DOM in soil water was fractionated into hydrophilic and hydrophobic compounds by XAD‐8 at pH 2. We found that the organic forest floor layers were large sources for DOC, DON, DOP, and DOS. The dissolved organic nutrients were mainly concentrated in the hydrophilic DOM fraction which proved to be more mobile in mineral soil pore water than the hydrophobic one. Consequently, the concentrations and fluxes of dissolved organic nutrients decreased less with depth than those of DOC. Concentrations as well as fluxes in subsoil pore water of DOC and dissolved organic nutrients in the studied weakly developed soils were high as compared with literature data on deeply developed forest soils. Under conditions of rapid water flow through the strongly structured mineral soil at the beech site, almost no retention of DOM took place and thus the influence of the distribution of organically bound nutrients between the DOM fractions on the export of DON, DOP, and DOS was negligible. 相似文献
16.
M. Oostrom M.J. Truex A.K. Rice C.D. Johnson K.C. Carroll D.J. Becker M.A. Simon 《Ground Water Monitoring & Remediation》2014,34(2):71-84
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
17.
Both laboratory experiments and numerical modelling were conducted to study the biodegradation and transport of benzene–toluene–xylenes (BTX) in a simulated semi‐confined aquifer. The factors incorporated into the numerical model include advection, hydrodynamic dispersion, adsorption, and biodegradation. The various physico‐chemical parameters required by the numerical model were measured experimentally. In the experimental portion of the study, BTX compounds were introduced into the aquifer sand. After the contaminants had been transported through the system, BTX concentrations were measured at 12 equally spaced wells. Subsequently, microorganisms obtained from the activated sludge of a sewage treatment plant and cultured in BTX mixtures were introduced into the aquifer through the 12 sampling wells. The distribution data for BTX adsorption by the aquifer sand form a nonlinear isotherm. The degree of adsorption by the sand varies, depending on the composition of the solute. The degradation time, measured from the time since the bacteria were added to the aquifer until a specific contaminant was no longer detectable, was 35–42 h for BTX. The dissolved oxygen, after degradation by BTX compounds and bacteria, was consumed by about 40–60% in the entire simulated aquifer; thus the aerobic conditions were maintained. This study provides insights for the biodegradation and transport of BTX in aquifers by numerical modelling and laboratory experiments. Experimental and numerical comparisons indicate that the results by Monod degradation kinetics are more accurate than those by the first‐order degradation kinetics. Copyright © 2002 John Wiley & Sons, Ltd. 相似文献
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Wei He ZeLin Bai YiLong Li XiangZhen Kong WenXiu Liu Chen Yang Bin Yang FuLiu Xu 《中国科学:地球科学(英文版)》2016,59(4):746-759
Dissolved organic matter (DOM) is a group of compounds that have complex chemical structures and multiple interactions with their surrounding materials. More than one trillion tons of DOM are stocked in the world’s aquatic ecosystems. DOM is a very important part of aquatic ecosystem productivity and plays a crucial role in global carbon cycling. DOM has rich environmental behaviors and effects such as influencing the bioavailability of contaminants, serving as an important inducer of reactive oxygen species (ROS), and protecting aquatic organisms from the harm of dangerous ultraviolet radiation. There have been many systematic studies on the composition, structure, and sources of DOM because such studies are much easier to conduct than studies on the environmental behaviors and effects of DOM. Due to many factors, the research systems of DOM’s environmental behaviors and effects are still being developed and have become a hotspot of environmental science. This review paper focuses on some critical progress, problems, and trends of DOM’s environmental behaviors and effects in aquatic ecosystems, including mutual exchange mechanisms between DOM and particulate organic matter (POM) with influencing factors, photochemical behaviors of DOM especially inducing ROS, binding interactions between DOM and anthropogenic organic contaminants (AOC), interactions between DOM and microorganisms, effects of DOM on pollutants’ bioavailability, ecotoxicity, and ecological risks. Hopefully, this paper will contribute to a more systematic understanding of the DOM environmental behaviors and effects and to promoting further relevant studies. 相似文献
20.
Dimitar Marinov Ingrid Puillat Elena Jurado Jordi Dachs 《Marine pollution bulletin》2009,58(10):1554-1561
Spatio-temporal variability of pollutants in the environment is a complex phenomenon that requires a combined approach for its analysis. Whereas data on measured levels of contaminants in various environmental compartments is essential, it is not always possible to monitor at the necessary frequency and with the adequate spatial sampling distribution to capture this variability. Therefore a modelling approach able to complement experimental data and close the gaps in the monitoring programs is useful for assessing the contaminant dynamics occurring at different time scales. In this work a 1D water column fate model has been developed and tested for Polycyclic Aromatic Hydrocarbons (PAHs). The model has been coupled with a simple ecological model that includes a bioaccumulation module. Afterwards, the model has been used to study the temporal variability of contaminant concentrations as well as the fluxes between compartments. The results evidence the complex coupling between spatio-temporal scales and its influence on environmental concentration levels. 相似文献