首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献,搜索用时 31 毫秒
1.
2.
A numerical model was developed to describe the fate and transport of hydrazinium (N2H5+) and competing Ca2+ and H+ cations applied in acidic solutions to columns of Ca2+/H+-saturated sandy soil during steady saturated flow conditions. Instantaneous ternary H+-Ca2+-N2H5+ cation exchange using the Gaines-Thomas approach was combined with second-order, irreversible, kinetic chemisorption of exchange-phase N2H5+ ions as major retention mechanisms for N2H5+. Exchange-mediated chemisorption is assumed to occur as chemical binding of N2H5+ ions located on carboxyl-group exchange sites to nearby carbonyl groups, consequently decreasing the effective soil cation exchange capacity (CEC). Comparison of simulated and observed breakthrough curves (BTCs) for concentrations of N2H5+ and Ca2+ ions in column effluent was used in model evaluation. The cation transport model with cation exchange coupled with exchange-mediated chemisorption provided a valid first approximation for N2H5+ transport.  相似文献   

3.
Process-based models are frequently used to assess the water quality impacts of turfgrass management emanating from proposed or existing golf courses. Thatch complicates the prediction of pesticide transport because surface-applied pesticides must pass through an organic-rich layer before entering the soil. This study was conducted to (i) compare the use of a linear equilibrium model (LEM) and two-site nonequilibrium (2SNE) model to predict pesticide transport through soil and thatch + soil columns, and (ii) evaluate thatch effects on pesticide transport through soil columns with a volume-averaging approach. Pesticide breakthrough curves were obtained for soil and thatch + soil columns from a 1 cm h(-1) flux applied one day after applying triclopyr (3,5,6-trichloro-2-pyridinyloxyacetic acid) and carbaryl (1-napthyl-methyl carbamate). Pesticide and bromide transport parameters indicated that nonequilibrium processes were affecting pesticide transport. Columns containing zoysiagrass (Zoysia japonica Steud.) thatch had lower triclopyr and carbaryl leaching losses than did soil-only columns, although total reductions attributable to thatch did not exceed 15% of the applied pesticide. When laboratory-based retardation factors were used, the 2SNE model explained 88 to 93% of the variability for triclopyr and 70 to 94% of the variability for carbaryl. Laboratory-based retardation factors performed well in a 2SNE model to predict the peak concentration and tailing behavior of triclopyr and carbaryl with a volume-averaging approach. These results suggest that separate representation of the thatch layer in process-based models is not a prerequisite to obtain reasonable estimates of pesticide transport under steady state flow conditions.  相似文献   

4.
Soil solution chemistry influences the sorption and transport behavior of hydrophobic organic compounds (HOCs) in soil. We used both batch and column studies to investigate the influence of ionic strengths (0.03 and 1.5 M) and flow velocities (12 and 24 cm h-1) on sorption and transport of naphthalene (NAP) in aggregated soil. Sorption parameters such as the Freundlich coefficient (Kf) and exponent (n) calculated from batch studies and column experiments were also compared. Retardation of NAP transport was greater at higher solution ionic strength, which may be attributed to greater sorption affinity due to enhanced aggregation of the sorbent. The effect of ionic strength on sorption of NAP observed in the batch study was consistent with the results from the column study. The Kf and n values obtained from the batch study for the two ionic strengths ranged from 7.8 to 13.7 and 0.68 to 0.80, respectively, whereas the Kf and n values obtained from the column study ranged from 7.9 to 9.9 and 0.73 to 0.85, respectively. The effluent breakthrough curve (BTC) of NAP at a flow rate of 24 cm h-1 showed significant chemical and physical nonequilibrium behavior, implying that a considerable amount of sorption in aggregated soil was time dependent when flow was relatively fast. The BTCs calculated with the parameters determined from batch studies compared poorly with the measured BTCs. The potential for nonequilibrium transport should be incorporated in models used for predicting the fate and transport of HOCs. Furthermore, caution is required when extrapolating the results from batch studies, especially for aggregated soils.  相似文献   

5.
Commercial production and use of fullerene (C60) nanomaterials will inevitably lead to their release into the environment, where knowledge of C60 fate and transport is limited. In this study, a series of one-dimensional column experiments was conducted to assess the transport and retention of nanoscale fullerene aggregates (nC60) in water-saturated soils. Under the experimental conditions, complete retention of nC60 was observed in columns (2.5 cm inside diameter x 11 cm length) packed with Appling or Webster soil, which contain 0.75 and 3.33% organic carbon by weight, respectively. When the volume of aqueous nC60 suspension (approximately 4.5 mg L(-1)) applied to Appling soil was increased from 5 to 65 pore volumes, the travel distance increased from 3 to 8 cm, and the retention capacity approached a limiting value of 130 microg g(-1), although nC60 was not detected in the column effluent. The addition of 20 mg C L(-1) Suwannee River humic acid to the influent suspension increased the nC60 transport in Appling soil but did not resul in breakthrough. Attempts to simulate the experimental data using clean-bed filtration theory were not satisfactory, yielding retention profiles that failed to match observed data. Subsequent incorporation of a limiting retention capacity expression into the mathematical model resulted in accurate predictions of the measured nC60 retention profiles and transport behavior. The sizable retention capacities observed in this study suggest that transport of nC60 is limited in relatively fine-textured soils containing appreciable amounts of clay minerals and organic matter, with substantial accumulation of nC60 aggregates near the point of release.  相似文献   

6.
Selenium (Se) contamination of groundwater is an environmental concern especially in areas where aquifer systems are underlain by Se-bearing geologic formations such as marine shale. This study examined the influence of nitrate (NO?) on Se species in irrigated soil and groundwater systems and presents results from field and laboratory studies that further clarify this influence. Inhibition of selenate (SeO?) reduction in the presence of NO? and the oxidation of reduced Se from shale by autotrophic denitrification were investigated. Groundwater sampling from piezometers near an alluvium-shale interface suggests that SeO? present in the groundwater was due in part to autotrophic denitrification. Laboratory shale oxidation batch studies indicate that autotrophic denitrification is a major driver in the release of SeO? and sulfate. Similar findings occurred for a shale oxidation flow-through column study, with 70 and 31% more reduced Se and S mass, respectively, removed from the shale material in the presence of NO? than in its absence. A final laboratory flow-through column test was performed with shallow soil samples to assess the inhibition of SeO? reduction in the presence of NO?, with results suggesting that a concentration of NO? of approximately 5 mg L or greater will diminish the reduction of SeO?. The inclusion of the fate and transport of NO? and dissolved oxygen is imperative when studying or simulating the fate and transport of Se species in soil and groundwater systems.  相似文献   

7.
Antibiotics reach soils via spreading of manure or sewage sludge. Knowledge on the transport behavior of antibiotics in soils is needed to assess their environmental fate. The effect of flow rate and applied mass, i.e., input concentration and pulse duration, on the transport of 14C-sulfadiazine (SDZ; 4-aminoN-pyrimidin-2-yl-benzenesulfonamide) was investigated with soil column experiments and numerical studies. Sulfadiazine was applied in pulses (6.8, 68 or 306 h) under steady-state (0.051 and 0.21 cm h(-1)) and intermittent flow conditions and at two input concentrations (0.57 and 5.7 mg L(-1)). Breakthrough curves (BTCs) of 14C were measured and for one experiment concentrations of SDZ, and its transformation products 4-(2-iminopyrimidin-1(2H)-yl)aniline (An-SDZ) and N(1)-2-(4-hydroxypyrimidinyl)benzenesulfanilamide (4-OH-SDZ) were determined. After finalizing the leaching experiments, 14C was quantified in different slices of the columns. A lower flow rate led to remarkably lower eluted masses compared with the higher flow rates. All BTCs could be described well using a three-site attachment-detachment model for which a common set of parameters was determined. However, the BTC obtained with the high input concentration was slightly better described with a two-site isotherm-based model. The prediction of the concentration profiles was good with both model concepts. The fitted sorption capacities decreased in the order SDZ > 4-OH-SDZ > An-SDZ. Overall, the experiments reveal the presence of similar mechanisms characterizing SDZ transport. The dependence of model performance on concentration implies that although the three-site attachment-detachment model is appropriate to predict the transport of SDZ in soil columns, not all relevant processes are adequately captured.  相似文献   

8.
A two-dimensional reservoir toxics model is essential to establishing effective water resources management and protection. In a reservoir, the fate of a toxic chemical is closely connected with flow regimes and circulation patterns. To better understand the kinetic processes and persistence and predict the dissipation of toxic contaminants in the reservoir during a spill or storm runoff event, a toxics submodel was developed and incorporated into an existing laterally integrated hydrodynamics and transport model. The toxics submodel describes the physical, chemical, and biological processes and predicts unsteady vertical and longitudinal distributions of a toxic chemical. The two-dimensional toxicant simulation model was applied to Shasta Reservoir in California to simulate the physico-chemical processes and fate of a volatile toxic compound, methyl isothiocyanate (MITC), during a chemical spill into the Sacramento River in 1991. The predicted MITC concentrations were compared with those observed. The effect of reservoir flow regimes on the transport and fate of the toxic substance was investigated. The results suggested that the persistence of MITC is significantly influenced by different flow regimes. Methyl isothiocyanate is more persistent in the reservoir under an interflow condition due to reduced volatilization from deep layers than under an overflow condition. In the overflow situation, the plume moved more slowly toward the dam and experienced greater dissipation. This analysis can assist in toxic spill control and reservoir management, including field sampling and closure of water intakes.  相似文献   

9.
A geo-referenced environmental fate model was developed for analyzing unsteady-state dispersion and distribution of chemicals in multimedia environmental systems. Chemical transport processes were formulated in seven environmental compartments of air, canopy, surface soil, root-zone soil, vadose-zone soil, surface water, and sediment. The model assumed that the compartments were completely mixed and chemical equilibrium was established instantaneously between the sub-compartments within each compartment. A fugacity approach was utilized to formulate the mechanisms of diffusion, advection, physical interfacial transport, and transformation reactions. The governing equations of chemical mass balances in the environmental compartments were solved simultaneously to reflect the interactions between the compartments. A geographic information system (GIS) database and geospatial analysis were integrated into the chemical transport simulation to provide spatially explicit estimations of model parameters at watershed scale. Temporal variations of the environmental properties and source emissions were also considered in the parameter estimations. The outputs of the model included time-dependent chemical concentrations in each compartment and its sub-compartments, and inter-media mass fluxes between adjacent compartments at daily time steps.  相似文献   

10.
Soil-derived dissolved organic matter (DOM) has been shown to form stable complexes with the herbicide napropamide [2-(alpha-naphthoxy-N,N-diethylpropionamide] capable of enhancing the transport of napropamide through soil columns. Two soils, one containing sewage sludge-derived organic matter (SS) and the other having only natural organic matter (NoSS) were treated with napropamide and allowed to dry to promote complex formation. Soil columns were prepared by packing a 10-cm layer of untreated, dry, sieved soil followed by an overlying 5-cm layer of napropamide-treated soil. Columns were irrigated and the effluent collected and placed in dialysis chambers. After equilibration napropamide concentrations were determined on both sides of the membrane and complex and quantified based on the amount of napropamide unable to cross the membrane. it was found that for the SS soil 7% and for the NoSS 2.4% of the applied napropamide underwent facilitated transport. In addition, most of the complex transported through the columns had a molecular weight between 500 and 1000 Daltons (Da). The solutions from the SS soil were also found to have formed at least two distinct complexes that were resolved after passing through the untreated soil layer. The results obtained were in agreement with other published results and the techniques used offer a way to separate and concentrate DOM complexes from column effluents for further characterization.  相似文献   

11.
ABSTRACT: The fate of contaminants in large water bodies is highly influenced by the transfer of flow and solutes across the water sediment interface. In this paper, an analytical model is presented where flow in both sediment bed and open channel is coupled at the interface through a boundary layer occupying the upper part of the sediment bed. The presence of this layer allows not only the capture of the inertia effects through a drag term in the generalized Darcy's equation, but also the specification of different soil parameters for the two porous zones. The flow is advective and driven by wave action along the water surface. The resulting system is solved for the pressure and flux in each sediment layer. The generated transport velocity fields are linked to a random walk simulation that is used to examine the trajectories of solute particles. Comparison of these trajectories against experimental tracer tests suggests a pattern very similar to the one attributed to the presence of surface mounds. The results clearly show the significance of the boundary layer and the drag term for soil with high permeability and the impact of both the thickness of the boundary layer and the length of the gravity wave relative to the depth of the water channel on the transport and exchange across the interface. The paper also examines the sensitivity of the mass exchange to the permeability of the two porous zones.  相似文献   

12.
Parathion is an insecticide of a group of highly toxic organophosphorus compounds. To investigate the dissipation and toxicological impact of parathion [O,O-diethyl O-(4-nitrophenyl) phosphorothioate] and its highly toxic metabolite, paraoxon, soil laboratory experiments were conducted in columns during a 19-d experiment under variably saturated conditions. Water and pesticide transport, sorption, and biodegradation of parathion were measured in three soil pools (soluble phase, weakly and strongly sorbed phases) using C-labeled pesticide. The effects of parathion and its metabolite on the mobility of soil nematodes were observed and then modeled with an effective variable, which combined pesticide concentration and time of application. Results showed that parathion was highly sorbed and slowly degraded to a mixture of metabolites. The parent compound and its metabolites remained located in the top 0.06-m soil layer. A kinetic model describing the sorption, biodegradation, and allocation into different soil pools of parathion and its metabolites was coupled with heat and water transport equations to predict the fate of parathion in soil. Simulated results were in agreement with experimental data, showing that the products remained in the upper soil layers even in the case of long-term (11-mo) simulation. The strongly sorbed fraction may be regarded as a pesticide reservoir that regularly provides pesticide to the weakly sorbed phase, and then, liquid phase, respectively. From both modeling and observations, no major toxicological damage of parathion and paraoxon to soil nematodes was found, although some effects on nematodes were possible, but at the soil surface only (0.01- and 0.02-m depth).  相似文献   

13.
A multimedia environmental fate model was developed to study the temporal dynamics and spatial distribution of a chemical pollutant at watershed scale. The theoretical considerations and implementation of the model were described in the accompanying paper (Part I). This paper presents the result of a test simulation on the transport of trichloroethylene (TCE) in the Connecticut River Basin. The simulation results were reported as time series of concentrations and inter-media transport fluxes in the compartments of atmosphere, plant, soil, surface water, and sediment. Predicted concentrations from the test simulation were compared with published field data or predictions by validated models. The temporal trends in TCE predictions were evaluated by comparing the simulation results with monthly TCE concentrations in various environmental compartments and monthly fluxes of inter-media transport processes. Results indicated that the simulation results were in reasonable agreement with reported data in the literature. The results also revealed that the mass transport of TCE from the atmosphere compartment to soil and surface water was a major route of TCE dispersion in the environment.  相似文献   

14.
Municipal sewage sludge is often used on arable soils as a source of nitrogen and phosphorus, but it also contains organic contaminants that may be leached to the ground water. Di(2-ethylhexyl)phthalate (DEHP) is a priority pollutant that is present in sewage sludge in ubiquitous amounts. Column experiments were performed on undisturbed soil cores (20-cm depth x 20-cm diameter) with three different soil types: a sand, a loamy sand, and a sandy loam soil. Dewatered sewage sludge was spiked with 14C-labeled DEHP (60 mg kg(-1)) and bromide (5 g kg(-1)). Sludge was applied to the soil columns either as five aggregates, or homogeneously mixed with the surface layer. Also, two leaching experiments were performed with repacked soil columns (loamy sand and sandy loam soil). The DEHP concentrations in the effluent did not exceed 1.0 microg L(-1), and after 200 mm of outflow less than 0.5% of the applied amount was recovered in the leachate in all soils but the sandy loam soil with homogeneous sludge application (up to 3.4% of the applied amount recovered). In the absence of macropore flow, DEHP in the leachate was primarily sorbed to mobilized dissolved organic macromolecules (DOM, 30.3 to 81.3%), while 2.4 to 23.6% was sorbed to mobilized mineral particles. When macropore flow occurred, this changed to 16.5 to 37.4% (DOM) and 36.9 to 40.6% (mineral particles), respectively. The critical combination for leaching of considerable amounts of DEHP was homogeneous sludge application and a continuous macropore structure.  相似文献   

15.
ABSTRACT: The Watershed Nutrient Transport and Transformation (NTT-Watershed) model is a physically based, energy-driven, multiple land use, distributed model that is capable of simulating water and nutrient transport in a watershed. The topographic features and subsurface properties of the watershed are refined into uniform, homogeneous square grids. The vertical discretization includes vegetation, overland flow, soil water redistribution and groundwater zones. The chemical submodel simulates the nitrogen dynamics in terrestrial and aquatic systems. Three chemical state variables are considered (NO3--, NH4+, and Org-N). The NTT-Watershed model was used to simulate the fate and transport of nitrogen in the Muddy Brook watershed in Connecticut. The model was shown to be capable of capturing the hydrologic and portions of the nitrogen dynamics in the watershed. Watershed planners could use this model in developing strategies of best management practices that could result in maximizing the reductions of nitrogen export from a watershed.  相似文献   

16.
Viruses from contaminant sources can be transported through porous media to drinking water wells. The objective of this study was to investigate inactivation and sorption of viruses during saturated and unsaturated transport in different soils. Bacteriophages phiX174 and MS-2, and Br- tracer in a phosphate-buffered saline solution were introduced into saturated and unsaturated soil columns as a step function under constant flow rate and hydraulic conditions. Results showed that significantly greater virus removal occurred in the unsaturated columns than in the saturated columns in the two soils containing high metal oxides content. However, the increase in virus retention under unsaturated conditions was not significant in two other soils having high phosphorus and calcium contents and high pH, and in another soil with high organic matter content. The results imply that the extent of water content effect on inactivation and sorption of viruses can range from significant to minimal depending on the properties of the transport medium. We found that the presence of in situ metal oxides was a significant factor responsible for virus sorption and inactivation. Therefore, soils with high metal oxides content may have the potential to be used as hydrological barriers in preventing microbial contamination in the subsurface environments. We also found that the water content effect on virus removal and inactivation strongly depended on solid properties of the testing medium.  相似文献   

17.
There is considerable concern about pollution of surface waters with P. Although most of the research has focused on inorganic P in surface runoff, it has recently become possible to easily follow the fate of soluble organic P forms in soils and waters. Two experiments were performed to compare the relative mobility and soil fixation affinity of orthophosphate monoesters, orthophosphate diesters, and soluble inorganic P. We used three P substrates, 4-methylumbelliferyl phosphate (MUP), deoxyribonucleic acid (DNA), and KH(2)PO(4) in (i) a soil column experiment and (ii) a soil P adsorption test tube experiment. Shortly after columns were prepared, approximately two pore volumes of 0.005 M CaCl(2) were passed through 25 cm length columns containing 10 cm of loamy sand amended with approximately 10 mg P as MUP, DNA, or KH(2)PO(4) above 15 cm of nonamended loamy sand. The total net quantity of 757.8 microg P 2L(-1) of orthophosphate diesters in the leachate from the DNA columns exceeded the net quantity of orthophosphate monoesters in leachate from the MUP columns (4.6 microg P 2L(-1)) and soluble inorganic P from the KH(2)PO(4) columns (34.0 microg P 2L(-1)). Adsorption of soluble organic and inorganic P in the test tube experiment yielded similar results: DNA, containing orthophosphate diesters, had a relatively low affinity for soils. In both experiments, high concentrations of other P compounds were identified in samples treated with organic P substrates, suggesting enzymatic hydrolysis by native soil phosphatase enzymes. These findings indicate that repeated application of organic forms of P could lead to significant leaching of P to ground water.  相似文献   

18.
Prediction of the Fate and Transport Processes of Atrazine in a Reservoir   总被引:1,自引:0,他引:1  
The fate and transport processes of a toxic chemical such as atrazine, an herbicide, in a reservoir are significantly influenced by hydrodynamic regimes of the reservoir. The two-dimensional (2D) laterally-integrated hydrodynamics and mass transport model, CE-QUAL-W2, was enhanced by incorporating a submodel for toxic contaminants and applied to Saylorville Reservoir, Iowa. The submodel describes the physical, chemical, and biological processes and predicts unsteady vertical and longitudinal distributions of a toxic chemical. The simulation results from the enhanced 2D reservoir model were validated by measured temperatures and atrazine concentrations in the reservoir. Although a strong thermal stratification was not identified from both observed and predicted water temperatures, the spatial variation of atrazine concentrations was largely affected by seasonal flow circulation patterns in the reservoir. In particular, the results showed the effect of flow circulation on spatial distribution of atrazine during summer months as the river flow formed an underflow within the reservoir and resulted in greater concentrations near the surface of the reservoir. Atrazine concentrations in the reservoir peaked around the end of May and early June. A good agreement between predicted and observed times and magnitudes of peak concentrations was obtained. The use of time-variable decay rates of atrazine led to more accurate prediction of atrazine concentrations, while the use of a constant half-life (60 days) over the entire period resulted in a 40% overestimation of peak concentrations. The results provide a better understanding of the fate and transport of atrazine in the reservoir and information useful in the development of reservoir operation strategies with respect to timing, amount, and depth of withdrawal.  相似文献   

19.
An unsaturated-zone transport model was used to examine the transport and fate of metolachlor applied to an agricultural site in Maryland, USA. The study site was instrumented to collect data on soil-water content, soil-water potential, ground water levels, major ions, pesticides, and nutrients from the unsaturated zone during 2002-2004. The data set was enhanced with site-specific information describing weather, soils, and agricultural practices. The Root Zone Water Quality Model was used to simulate physical, chemical, and biological processes occurring in the unsaturated zone. Model calibration to bromide tracer concentrations indicated flow occurred through the soil matrix. Simulated recharge rates were within the measured range of values. The pesticide transport model was calibrated to the intensive data collection period (2002-2004), and the calibrated model was then used to simulate the period 1984 through 2004 to examine the impact of sustained agricultural management practices on the concentrations of metolachlor and its degradates at the study site. Simulation results indicated that metolachlor degrades rapidly in the root zone but that the degradates are transported to depth in measurable quantities. Simulations indicated that degradate transport is strongly related to the duration of sustained use of metolachlor and the extent of biodegradation.  相似文献   

20.
The environmental fate of herbicides can be studied at different levels: in the lab with disturbed or undisturbed soil columns or in the field with suction cup lysimeters or soil enclosure lysimeters. A field lysimeter experiment with 10 soil enclosures was performed to evaluate the mass balance in different environmental compartments of the phenylurea herbicides diuron [3-(3,4-diclorophenyl)-1,1-dimethyl-urea] and linuron [3-(3,4-dichlorophenyl)-1-methoxy-1-methylurea]. After application on the agricultural soil, the herbicides were searched for in soil, pore water, and air samples. Soil and water samples were collected at different depths of the soil profile and analyzed to determine residual concentrations of both the parent compounds and of their main transformation products, to verify their persistence and their leaching capacity. Air volatilization was calculated using the theoretical profile shape method. The herbicides were detected only in the surface layer (0-10 cm) of soil. In this layer, diuron was reduced to 50% of its initial concentration at the end of the experiment, while linuron was still 70% present after 245 d. The main metabolites detected were DCPMU [3-(3,4-dichlorophenyl)-1-methylurea] and DCA (3,4-dichloroaniline). In soil pore water, diuron and linuron were detected at depths of 20 and 40 cm, although in very low concentrations. Therefore the leaching of these herbicides was quite low in this experiment. Moreover, volatilization losses were inconsequential. The calculated total mass balance showed a high persistence of linuron and diuron in the soil, a low mobility in soil pore water (less than 0.5% in leachate water), and a negligible volatilization effect. The application of the Pesticide Leaching Model (PELMO) showed similar low mobility of the chemicals in soil and water, but overestimated their volatilization and their degradation to the metabolite DCPMU. In conclusion, the use of soil enclosure lysimeters proved to be a good experimental design for studying mobility and transport processes of herbicides in field conditions.  相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号