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1.
Breakthrough curves, on a semi-log scale, from tests in porous media with block-input of viruses, bacteria, protozoa and colloidal particles often exhibit a typical skewness: a rather slowly rising limb and a smooth transition of a declining limb to a very long tail. One-site kinetic models fail to fit the rising and declining limbs together with the tail satisfactorily. Inclusion of an equilibrium adsorption site does not seem to improve simulation results. This was encountered in the simulation of breakthrough curves from a recent field study on the removal of bacteriophages MS2 and PRD1 by passage through dune sand. In the present study, results of laboratory experiments for the study of this issue are presented. Breakthrough curves of salt and bacteriophages MS2, PRDI, and phiX174 in 1 D column experiments have been measured. One- and two-site kinetic models have been applied to fit and predict breakthrough curves from column experiments. The two-site model fitted all breakthrough curves very satisfactorily, accounting for the skewness of the rising limb as well as for the smooth transition of the declining limb to the tail of the breakthrough curve. The one-site model does not follow the curvature of the breakthrough tail, leading to an overestimation of the inactivation rate coefficient for attached viruses. Interaction with kinetic site 1 is characterized by relatively fast attachment and slow detachment, whereas attachment to and detachment from kinetic site 2 is fast. Inactivation of viruses and interaction with kinetic site 2 provide only a minor contribution to removal. Virus removal is mainly determined by the attachment to site 1. Bacteriophage phiX174 attached more than MS2 and PRD1, which can be explained by the greater electrostatic repulsion that MS2 and PRD1 experience compared to the less negatively charged phiX174.  相似文献   

2.
In a recent field study on dune recharge, bacteriophages MS2 and PRD1 were found to be removed 3 log10 over the first 2.4 m and only 5 log10 over the next 27 m. To understand the causes of this nonlinear removal, column experiments were carried out under conditions similar to the field: same recharge water, temperature (5 +/- 3 degrees C) and pore water velocity (1.5 m day(-1)). Soil samples were taken along a streamline between the recharge canal and the first monitoring well. Bacteriophage phiX174 was included for comparison. The high initial removal in the field was found not to be due to heterogeneity of phage suspensions but to soil heterogeneity. Phage removal rates correlated strongly positively with soil organic carbon content, and relatively strongly positively with silt content and the presence of ferric oxyhydroxides. Soil organic carbon content, silt content and the presence of ferric oxyhydroxides were found to decrease exponentially with travel distance. Removal rates of phiX174 were found to be 3-10 times higher than those of MS2 and PRD1 due to the lower electrostatic repulsion that the less negatively charged phiX174 experiences. It is suggested that the high initial removal in the field is due to the presence of favorable sites for attachment formed by ferric oxyhydroxides that decrease exponentially with travel distance. Similar removal rates may be found at both laboratory and field scale. However, due to local variations at field scale detailed knowledge on soil heterogeneity may be needed to enable a reliable prediction of removal.  相似文献   

3.
We performed a sensibility analysis of model selection in modeling the reactive transport of cesium in crushed granite through model calibration and validation. Based on some solid phase analysis data and kinetic batch experimental results, we hypothesized three two-site sorption models in the LEHGC reactive transport model to fit the breakthrough curves (BTCs) from the corresponding column experiments. The analysis of breakthrough curves shows that both the empirical two-site kinetic linear sorption model and the semi-mechanistic/semi-empirical two-site kinetic surface complexation model, regardless of their complexity, can match our experimental data fairly well under given test conditions. A numerical experiment to further compare the two models shows that they behave differently when the pore velocity is not of the same order of magnitude as our test velocities. This result indicates that further investigations to help determine a better model are needed. We suggest that a multistage column experiment, which tests over the whole range of practical flow velocities, should be conducted to help alleviate inadequate hypothesized models.  相似文献   

4.
A sand column leaching system with well-controlled suction and flow rate was built to investigate the effects on bacterial transport of air-water interface effects (AWI) correlated to water content, particle size, and column length. Adsorption of Escherichia coli strain D to silica sands was measured in batch tests. The average % adsorption for coarse and fine sands was 45.9+/-7.8% and 96.9+/-3.2%, respectively. However, results from static batch adsorption experiments have limited applicability to dynamic bacterial transport in columns. The early breakthrough of E. coli relative to bromide was clear for all columns, namely c. 0.15 to 0.3 pore volume earlier. Column length had no significant effects on the E. coli peak concentration or on total recovery in leachate, indicating retention in the top layer of sands. Tailing of breakthrough curves was more prominent for all fine sand columns than their coarse sand counterparts. Bacterial recovery in leachate from coarse and saturated sand columns was significantly higher than from fine and unsaturated columns. Observed data were fitted by the convection-dispersion model, amended for one-site and two-site adsorption to particles, and for air-water interface (AWI) adsorption. Among all models, the two-site+AWI model achieved consistently high model efficiency for all experiments. Thus it is evident from experimental and modeling results that AWI adsorption plays an important role in E. coli transport in sand columns.  相似文献   

5.
The potential contamination of groundwater by herbicides is often controlled by processes in the vadose zone, through which herbicides travel before entering groundwater. In the vadose zone, both physical and chemical processes affect the fate and transport of herbicides, therefore it is important to represent these processes by mathematical models to predict contaminant movement. To simulate the movement of simazine, a herbicide commonly used in Chilean vineyards, batch and miscible displacement column experiments were performed on a disturbed sandy soil to quantify the primary parameters and processes of simazine transport. Chloride (Cl(-)) was used as a non-reactive tracer, and simazine as the reactive tracer. The Hydrus-1D model was used to estimate the parameters by inversion from the breakthrough curves of the columns and to evaluate the potential groundwater contamination in a sandy soil from the Casablanca Valley, Chile. The two-site, chemical non-equilibrium model was observed to best represent the experimental results of the miscible displacement experiments in laboratory soil columns. Predictions of transport under hypothetical field conditions using the same soil from the column experiments were made for 40 years by applying herbicide during the first 20 years, and then halting the application and considering different rates of groundwater recharge. For recharge rates smaller than 84 mm year(-1), the predicted concentration of simazine at a depth of 1 m is below the U.S. EPA's maximum contaminant levels (4 microg L(-1)). After eight years of application at a groundwater recharge rate of 180 mm year(-1) (approximately 50% of the annual rainfall), simazine was found to reach the groundwater (located at 1 m depth) at a higher concentration (more than 40 microg L(-1)) than the existing guidelines in the USA and Europe.  相似文献   

6.
Model predictions of pesticide transport in structured soils are complicated by multiple processes acting concurrently. In this study, the hydraulic, physical, and chemical nonequilibrium (HNE, PNE, and CNE, respectively) processes governing herbicide transport under variably saturated flow conditions were studied. Bromide (Br-), isoproturon (IPU, 3-(4-isoprpylphenyl)-1,1-dimethylurea) and terbuthylazine (TER, N2-tert-butyl-6-chloro-N4-ethyl-1,3,5-triazine-2,4-diamine) were applied to two soil columns. An aggregated Ap soil column and a macroporous, aggregated Ah soil column were irrigated at a rate of 1 cm h(-1) for 3 h. Two more irrigations at the same rate and duration followed in weekly intervals. Nonlinear (Freundlich) equilibrium and two-site kinetic sorption parameters were determined for IPU and TER using batch experiments. The observed water flow and Br- transport were inversely simulated using mobile-immobile (MIM), dual-permeability (DPM), and combined triple-porosity (DP-MIM) numerical models implemented in HYDRUS-1D, with improving correspondence between empirical data and model results. Using the estimated HNE and PNE parameters together with batch-test derived equilibrium sorption parameters, the preferential breakthrough of the weakly adsorbed IPU in the Ah soil could be reasonably well predicted with the DPM approach, whereas leaching of the strongly adsorbed TER was predicted less well. The transport of IPU and TER through the aggregated Ap soil could be described consistently only when HNE, PNE, and CNE were simultaneously accounted for using the DPM. Inverse parameter estimation suggested that two-site kinetic sorption in inter-aggregate flow paths was reduced as compared to within aggregates, and that large values for the first-order degradation rate were an artifact caused by irreversible sorption. Overall, our results should be helpful to enhance the understanding and modeling of multi-process pesticide transport through structured soils during variably saturated water flow.  相似文献   

7.
Large amounts of 137Cs have been accidentally released to the subsurface from the Hanford nuclear site in the state of Washington, USA. The cesium-containing liquids varied in ionic strengths, and often had high electrolyte contents, mainly in the form of NaNO3 and NaOH, reaching concentrations up to several moles per liter. In this study, we investigated the effect of ionic strengths on Cs migration through two types of porous media: silica sand and Hanford sediments. Cesium sorption and transport was studied in 1, 10, 100, and 1000 mM NaCl electrolyte solutions at pH 10. Sorption isotherms were constructed from batch equilibrium experiments and the batch-derived sorption parameters were compared with column breakthrough curves. Column transport experiments were analyzed with a two-site equilibrium-nonequilibrium model. Cesium sorption to the silica sand in batch experiments showed a linear sorption isotherm for all ionic strengths, which matched well with the results from the column experiments at 100 and 1000 mM ionic strength; however, the column experiments at 1 and 10 mM ionic strength indicated a nonlinear sorption behavior of Cs to the silica sand. Transport through silica sand occurred under one-site sorption and equilibrium conditions. Cesium sorption to Hanford sediments in both batch and column experiments was best described with a nonlinear Freundlich isotherm. The column experiments indicated that Cs transport in Hanford sediments occurred under two-site equilibrium and nonequilibrium sorption. The effect of ionic strength on Cs transport was much more pronounced in Hanford sediments than in silica sands. Effective retardation factors of Cs during transport through Hanford sediments were reduced by a factor of 10 when the ionic strength increased from 100 to 1000 mM; for silica sand, the effective retardation was reduced by a factor of 10 when ionic strength increased from 1 to 1000 mM. A two order of magnitude change in ionic strength was needed in the silica sand to observe the same change in Cs retardation as in Hanford sediments.  相似文献   

8.
Breakthrough adsorption study of migratory nickel in fine-grained soil.   总被引:1,自引:0,他引:1  
The present study was conducted to evaluate the breakthrough curve for nickel adsorption in fine-grained soil from a nearby ash pond site of a thermal power plant. Nickel was found to be the major polluting solute in the ash sluicing wastewater. The adsorption of nickel by vertical soil column batch test and horizontal migration test was carried out in the laboratory. Field investigation was conducted also, by installing test wells around the ash pond site. Experimental results showed a good adsorptive capacity of soil for nickel ions. The breakthrough curves showed a reasonable fitting with a one-dimensional mathematical model. The breakthrough curves yielded from field test results showed good agreement with a two-dimensional mathematical model.  相似文献   

9.
Lattice Boltzmann model for agrochemical transport in soils   总被引:2,自引:0,他引:2  
Agrochemical transport in soils is complicated and involves physical, chemical and biochemical reactions; its mathematical modelling remains a challenging task. This paper presents a lattice Boltzmann model to simulate the agrochemical movement. The lattice Boltzmann model is a microscopic and process-based model, simulating the transport process by tracking chemical particles. The model presented in this paper is for one-dimensional vertical leaching and assumes that the chemical particles at the microscopic level move in five directions: one stagnant, two in vertical direction and two in an internal horizontal direction bounded by two reactive walls. Reactions at the walls are assumed to take place at two different rates, one in fast rate where the chemicals in the solution and on the wall are in an instant equilibrium, and the other in slow rate where the mass exchange rate between the chemicals in the solution and on the wall is a first-order kinetic. The reactions on both walls are assumed to occur instantly when the chemical particles moving in the internal direction hit the walls. To test the model, we measured the leaching of atrazine through soil columns in the laboratory. The results simulated with the lattice Boltzmann model are compared with the measured breakthrough curves and the non-equilibrium two-site convection-dispersion model; they all show close agreement. The transport parameters needed in the models are obtained from the measurement of adsorption isotherm of atrazine, bromide leaching in the same soil columns and calibration.  相似文献   

10.
11.
A semianalytical soil-pesticide transport model is formulated based on a compartmental approach to determine spatial and temporal variations of pesticide residues across a soil profile. The compartmental model is implemented by drawing an analogy between a series of continuous-flow stirred tank reactors and a soil horizon that consists of multiple perfectly mixed compartments. The analogy is strengthened by exploiting a relation between the compartment series and the conventional convective-dispersive equation (CDE) for vertical transport in the soil. Consequently, the number of compartments in the model formulation is not free, but dictated as a function of transport parameters. The model formulation allows consideration of arbitrary boundary value specifications and also, for some cases, spatially varying initial concentration profiles. Sorption kinetics is represented via a two-site model that involves a linear sorption isotherm and a first-order irreversible sorption or a radial diffusive penetrating model. For these three cases, analysis of the compartmental model allows the resultant concentration profiles to be expressed in terms of the Poisson distribution. When a nonlinear kinetic sorption model is used to simulate the sorption processes, an analytical solution is not found and a numerical approach is required.  相似文献   

12.
Cosolvent flushing is a technique that has been proposed for the removal of hydrophobic organic contaminants in the subsurface. Cosolvents have been shown to dramatically increase the solubility of such compounds compared to the aqueous solubility; however, limited data are available on the effectiveness of cosolvents for field-contaminated media. In this work, we examine cosolvent flushing for the removal of polycyclic aromatic hydrocarbons (PAHs) in soil from a former manufactured gas plant (FMGP). Batch studies confirmed that the relationship between the soil-cosolvent partitioning coefficient (K(i)) and the volume fraction of cosolvent (f(c)) followed a standard log-linear equation. Using methanol at an fc of 0.95, column studies were conducted at varying length scales, ranging from 11.9 to 110 cm. Removal of PAH compounds was determined as a function of pore volumes (PVs) of cosolvent flushed. Despite using a high f(c), rate and chromatographic effects were observed in all the columns. PAH effluent concentrations were modeled using a common two-site sorption model. Model fits were improved by using MeOH breakthrough curves to determine fitted dispersion coefficients. Fitted mass-transfer rates were two to three orders of magnitude lower than predicted values based on published data using artificially contaminated sands.  相似文献   

13.
In this paper, we used the continuous time random walk (CTRW) framework to characterize the transport process in 1250-cm long one-dimensional homogenous and heterogeneous soil columns at the experiments conducted by Huang et al. [Huang, K., Toride, N., van Genuchten, M.Th., 1995. Experimental investigation of solute transport in large, homogeneous and heterogeneous, saturated soil columns. Trans. Porous Media. 18, 283-302]. The transport process was also simulated by using the advection-dispersion equation (ADE) and the spatial fractional advection-dispersion equation (FADE) for comparison. In the homogeneous soil column, the non-Fickian behavior is found at the distances less than 1000cm with beta values larger than 1.60, but less than 2, and Fickian form transport is obtained at distances larger than 1000cm with beta values larger than 2. In the heterogeneous soil column, we found the most anomalous behavior at distances from 200cm to 700cm with beta values ranging from 0.894 to 0.958, and non-Fickian transport process is observed at distances larger than 800cm with beta values in the range between 1 and 1.3. More significant non-Fickian behavior is found for transport in the heterogeneous soil column than that in the homogeneous soil column. The CTRW fits to the breakthrough curves (BTCs) have lower values of root mean square error (RMSE) and higher values of determination coefficient (r(2)), with respect to the fits of ADE and FADE. The CTRW model also is better captures the full evolution of BTCs, and especially their tails.  相似文献   

14.
This study focuses on the influences of a warm high-pressure meteorological system on aerosol pollutants, employing the simulations by the Models-3/CMAQ system and the observations collected during October 10–12, 2004, over the Pearl River Delta (PRD) region. The results show that the spatial distributions of air pollutants are generally circular near Guangzhou and Foshan, which are cities with high emissions rates. The primary pollutant is particulate matter (PM) over the PRD. MM5 shows reasonable performance for major meteorological variables (i.e., temperature, relative humidity, wind direction) with normalized mean biases (NMB) of 4.5–38.8% and for their time series. CMAQ can capture one peak of all air pollutant concentrations on October 11, but misses other peaks. The CMAQ model systematically underpredicts the mass concentrations of all air pollutants. Compared with chemical observations, SO2 and O3 are predicted well with a correlation coefficient of 0.70 and 0.65. PM2.5 and NO are significantly underpredicted with an NMB of 43% and 90%, respectively. The process analysis results show that the emission, dry deposition, horizontal transport, and vertical transport are four main processes affecting air pollutants. The contributions of each physical process are different for the various pollutants. The most important process for PM10 is dry deposition, and for NOx it is transport. The contributions of horizontal and vertical transport processes vary during the period, but these two processes mostly contribute to the removal of air pollutants at Guangzhou city, whose emissions are high. For this high-pressure case, the contributions of the various processes show high correlations in cities with the similar geographical attributes. According to the statistical results, cities in the PRD region are divided into four groups with different features. The contributions from local and nonlocal emission sources are discussed in different groups.
Implications: The characteristics of aerosol pollution episodes are intensively studied in this work using the high-resolution modeling system MM5/SMOKE/CMAQ, with special efforts on examining the contributions of different physical and chemical processes to air concentrations for each city over the PRD region by a process analysis method, so as to provide a scientific basis for understanding the formation mechanism of regional aerosol pollution under the high-pressure system over PRD.  相似文献   

15.
In this note, we applied the temporal moment solutions of [Das and Kluitenberg, 1996. Soil Sci. Am. J. 60, 1724] for one-dimensional advective-dispersive solute transport with linear equilibrium sorption and first-order degradation for time pulse sources to analyse soil column experimental data. Unlike most other moment solutions, these solutions consider the interplay of degradation and sorption. This permits estimation of a first-order degradation rate constant using the zeroth moment of column breakthrough data, as well as estimation of the retardation factor or sorption distribution coefficient of a degrading solute using the first moment. The method of temporal moment (MOM) formulae was applied to analyse breakthrough data from a laboratory column study of atrazine, hexazinone and rhodamine WT transport in volcanic pumice sand, as well as experimental data from the literature. Transport and degradation parameters obtained using the MOM were compared to parameters obtained by fitting breakthrough data from an advective-dispersive transport model with equilibrium sorption and first-order degradation, using the nonlinear least-square curve-fitting program CXTFIT. The results derived from using the literature data were also compared with estimates reported in the literature using different equilibrium models. The good agreement suggests that the MOM could provide an additional useful means of parameter estimation for transport involving equilibrium sorption and first-order degradation. We found that the MOM fitted breakthrough curves with tailing better than curve fitting. However, the MOM analysis requires complete breakthrough curves and relatively frequent data collection to ensure the accuracy of the moments obtained from the breakthrough data.  相似文献   

16.
Deng J  Jiang X  Zhang X  Hu W  Crawford JW 《Chemosphere》2008,71(11):2150-2157
Contaminant transport in soils is complicated and involves some physical and chemical nonequilibrium processes. In this research, the soil column displacement experiments of Cl and atrazine under different flow velocities were carried out. The data sets of Cl transport in sandy loam fitted to the convection dispersion equation (CDE) and the two-region model (TRM) indicated that the effects of physical nonequilibrium process produced by immobile water on the breakthrough curves (BTCs) of Cl and atrazine transport through the repacking soil columns were negligible. The two-site model (TSM) and the continuous time random walk (CTRW) were also used to fit atrazine transport behavior at the flow rate of 19.86 cm h−1. The CTRW convincingly captured the full evolution of atrazine BTC in the soil column, especially for the part of long tailing. However, the TSM failed to characterize the tailing of atrazine BTC in the soil column. The calculated fraction of equilibrium sorption sites, F, ranging from 0.78 to 0.80 for all flow rates suggested the contribution of nonequilibrium sorption sites to the asymmetry of atrazine BTCs. Furthermore, the data sets for the flow rates of 6.68 cm h−1 and 32.81 cm h−1 were predicted by the TSM and the CTRW. As to the flow rate of 6.68 cm h−1, the CTRW predicted the entire BTC of atrazine transport better than the TSM did. For the flow rate of 32.81 cm h−1, the CTRW characterized the late part of the tail better, while the TSM failed to predict the tailings of atrazine BTC.  相似文献   

17.
We present results from experiments on the migration of 137Cs through columns containing quartz sand. Times for 137Cs movement through these columns and the quantity of 137Cs adsorbed by the sand decreased as the ionic strength of the pore water increased from 0.002 to 0.1 m. The breakthrough curves were characterized by a slow approach towards steady-state concentrations as well as by long tails, indicating that 137Cs adsorption to the sand grains was, at least in part, controlled by rate-limited reactions. Various formulations for solute mass transfer were tested for their ability to fit the experimental breakthrough curves. Based on a statistical analysis, a nonlinear, two-site model was identified as the most appropriate for describing the suite of experimental data. Variation in the model parameter that describes the rate of 137Cs adsorption to the sand showed no consistent pattern with changes in ionic strength. In contrast, model parameters describing the sorption capacity of the sand grains and the fraction of kinetic sorption sites on the sand decreased with increasing ionic strength. The parameter describing the rate of 137Cs desorption varied directly with changes in ionic strength.  相似文献   

18.
A tracer study was conducted in a 3-ha surface flow constructed wetland to analyze transport performance of PRD1, an enteric virus model. The convection-dispersion equation (CDE), including a first-order reaction model, adequately simulated transport performance of PRD1 in the wetland under an average hydraulic loading rate of 82 mm/d. Convective velocity (v) and longitudinal dispersion coefficient (D) were estimated by modeling a conservative tracer (bromide) pulse through the wetland. Both PRD1 and bromide were simultaneously added to the entering secondary treated wastewater effluent. The mass of bromide and PRD1 recovered was 76 and 16%, respectively. The PRD1 decay rate was calculated to be 0.3/day. The findings of this study suggest that the CDE model and analytical moment equations represent a suitable option to characterize virus transport performance in surface flow constructed wetlands.  相似文献   

19.
A dual-permeability model (S_1D_DUAL) was developed to simulate the transport of land-applied pesticides in macroporous media. In this model, one flow domain was represented by the bulk matrix and the other by the preferential flow domain (PFD) where water and chemicals move at faster rates. The model assumed the validity of Darcian flow and the advective-dispersive solute transport in each of the two domains with inter-domain transfer of water and solutes due to pressure and concentration gradients. It was conceptualized that sorption and biodegradation rates vary with soil depth as well as in each of the two flow domains. In addition to equilibrium sorption, kinetic sorption was simulated in the PFD. Simulations were conducted to evaluate the combined effects of preferential flow, depth- and domain-variant sorption, and degradation on leaching of two pesticides: one with strong sorption potential (trifluralin) and the other with weak sorption potential (atrazine). Simulation results for a test case showed that water flux in the PFD was three times more than in the matrix for selected storm events. When equilibrium sorption was considered, the simulated profile of trifluralin in each domain was similar; however, the atrazine profile was deeper in the PFD than in the bulk matrix under episodic storm events. With an assumption of negligible sorption in the PFD, both the atrazine and the trifluralin profiles moved twice deeper into the PFD. The simulated concentrations of the chemicals were several orders higher in the PFD than in the matrix, even at deeper depths. The volume fraction of the macropores and the sorption and biodegradation properties of the chemicals could also affect the amount of pesticides leaving the root zone. For an intense storm event, slow sorption reaction rates in the PFD produced higher breakthrough concentrations of atrazine at the bottom of the simulated soil profile, thus posing the risk for breakthrough of chemicals from the root zone.  相似文献   

20.
Abstract

Contaminated solid wastes exist in many industrial sites, gas plants, and oil refineries. One method of decontaminating the soil is to subject it to high temperatures in a rotary calciner in an anaerobic environment. Preliminary results from a computational model are presented in this paper for the flow and heat transfer from granular solid particles under treatment in a rotary kiln calciner. A fluidization model using kinetic theory of granular flow has been employed to solve the particle flow and heat transfer problem. While a two-dimensional model is used to predict the rotation induced flow of the solid particles, a pseudo three-dimensional model for heat transfer is developed where the axial bulk temperature gradient is obtained from a one-dimensional energy balance model. The model predictions indicate interesting features of the flow and temperature fields in the bed material. Future tasks include the development of a devolatilization model to study the decontamination of waste soil in the rotary calciner.  相似文献   

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