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1.
For several decades, phosphate ores containing 226Ra as well as several trace metals have been processed in Belgium to produce calcium phosphate for use in cattle food. The waste water is discharged in two small rivers, the Laak and the Winterbeek.In this study, the levels of 226Ra and trace metals in surface water and sediments of the Winterbeek were investigated and the mobility of these compounds was assessed using DGT (Diffusive Gradient in Thin Films) and sequential extraction techniques.The concentrations of 226Ra and trace metals in water and sediment indicate a decreasing trend in inputs to the Winterbeek.The mobility of 226Ra, assessed by DGT, is related to the reductive mobilization of Fe. The sequential extraction technique shows that at some stations an important fraction of 226Ra is found to labile sediment phases.Diffusive 226Ra sediment fluxes, are however, relatively small and have only a minor contribution to the water column concentration of 226Ra.  相似文献   

2.
Soil radon was measured from late October 2000 to January 2001 at three test sites on the campus of Hokkaido University in Sapporo, Japan. Factors affecting radon concentrations were investigated with relation to meteorological data, as well as soil 226Ra content, mineral composition, water content, and pH, Eh and conductivity. Soil radon varied with time and with sampling site appreciably, in a manner unaltered by the surface geology. However, the ratio of radon isotopes (220Rn/222Rn) in the soil was constant within each sampling site, regardless of varying concentration of these nuclides during the monitoring period. Snow covering on the soil surfaces may affect the 222Rn concentration.  相似文献   

3.
This paper presents a comparative study of 222Rn emanation from the ore and backfill tailings in an underground uranium mine located at Jaduguda, India. The effects of surface area, porosity, 226Ra and moisture contents on 222Rn emanation rate were examined. The study revealed that the bulk porosity of backfill tailings is more than two orders of magnitude than that of the ore. The geometric mean radon emanation rates from the ore body and backfill tailings were found to be 10.01?×?10?3 and 1.03 Bq m?2 s?1, respectively. Significant positive linear correlations between 222Rn emanation rate and the 226Ra content of ore and tailings were observed. For normalised 226Ra content, the 222Rn emanation rate from tailings was found to be 283 times higher than the ore due to higher bulk porosity and surface area. The relative radon emanation from the tailings with moisture fraction of 0.14 was found to be 2.4 times higher than the oven-dried tailings. The study suggested that the mill tailings used as a backfill material significantly contributes to radon emanation as compared to the ore body itself and the 226Ra content and bulk porosity are the dominant factors for radon emanation into the mine atmosphere.  相似文献   

4.
This paper presents a reaction-based water quality transport model in subsurface flow systems. Transport of chemical species with a variety of chemical and physical processes is mathematically described by M partial differential equations (PDEs). Decomposition via Gauss-Jordan column reduction of the reaction network transforms M species reactive transport equations into two sets of equations: a set of thermodynamic equilibrium equations representing N(E) equilibrium reactions and a set of reactive transport equations of M-N(E) kinetic-variables involving no equilibrium reactions (a kinetic-variable is a linear combination of species). The elimination of equilibrium reactions from reactive transport equations allows robust and efficient numerical integration. The model solves the PDEs of kinetic-variables rather than individual chemical species, which reduces the number of reactive transport equations and simplifies the reaction terms in the equations. A variety of numerical methods are investigated for solving the coupled transport and reaction equations. Simulation comparisons with exact solutions were performed to verify numerical accuracy and assess the effectiveness of various numerical strategies to deal with different application circumstances. Two validation examples involving simulations of uranium transport in soil columns are presented to evaluate the ability of the model to simulate reactive transport with complex reaction networks involving both kinetic and equilibrium reactions.  相似文献   

5.
The conditions under which rate-limited sorption is important for cleanup of layered soils by vapor extraction are investigated. The investigation includes two steps: (a) the cleanup time is estimated for a number of scenario cases by means of a numerical model and (b) the numerical results are approximated using analytical solutions derived for simplified models. In this way, equations are derived, which give insight into the influence of different parameters characterizing the properties of the soil, the geometry of the formation, the mass transfer mechanisms in it, and the distribution of the contaminant mass in the different phases (gas phase, water phase and solid phase). The numerical model used is based on the advection-dispersion differential equations for Darcian isothermal airflow, local equilibrium contaminant mass transfer between gas phase and soil water and first-order kinetics for mass transfer between soil water and solid phase. The numerical results are approximated combining an analytical solution to estimate cleanup time in layered formations for local equilibrium sorption, which has been presented in a previous work (J. Contam. Hydrol., 36 (1999) 105). with an analytical solution based on the well-mixed reservoir model under consideration of rate-limited sorption. The analytical approximation of the cleanup time is in reasonable agreement with the numerical results and allows its estimation with small computational effort.  相似文献   

6.
A two-dimensional flow and transport model was developed for simulating transient water flow and nonreactive solute transport in heterogeneous, unsaturated porous media containing air and water. The model is composed of a unique combination of robust and accurate numerical algorithms for solving the Richards', Darcy flux, and advection-dispersion equations. The mixed form of Richards' equation is solved using a finite-element formulation and a modified Picard iteration scheme. Mass lumping is employed to improve solution convergence and stability behavior. The flow algorithm accounts for hysteresis in the pressure head-water content relationship. Darcy fluxes are approximated with a Galerkin and Petrov-Galerkin finite-element method developed for random heterogeneous porous media. The transport equation is solved using an Eulerian-Lagrangian method. A multi-step, fourth-order Runge-Kutta, reverse particle tracking technique and a quadratic-linear interpolation scheme are shown to be superior for determining the advective concentration. A Galerkin finite-element method is used for approximating the dispersive flux. The unsaturated flow and transport model was applied to a variety of rigorous problems and was found to produce accurate, mass-conserving solutions when compared to analytical solutions and published numerical results.  相似文献   

7.
8.
The gel barrier formation by a gelling liquid (Colloidal Silica) injection in an unsaturated porous medium is investigated by developing a mathematical model and conducting numerical simulations. Gelation process is initiated by adding electrolytes such as NaCl, and the gel phase consisting of cross-linked colloidal silica particles grows as the gelation process proceeds. The mathematical model describing the transport and gelation of Colloidal Silica (CS) is based on coupled mass balance equations for the gel mixture (the sol phase plus the gel phase), gel phase (cross-linked colloidal silica particles plus water captured between cross-linked particles), and colloidal silica particles (discrete and cross-linked) and NaCl in the sol (suspension of discrete colloidal silica particles in water) and gel phases. The solutions in terms of volumetric fraction of the gel phase yield the gel mixture viscosity via the dependency on the volumetric fraction of gel phase. This dependency is determined from a kinetic gelation model with time-normalized viscosity curves. The proposed model is verified by comparing experimentally and numerically determined hydraulic conductivities of gel-treated soil columns at different CS injection volumes. The numerical experiments indicate that an impermeable gel layer is formed within the time period twice the gel-point in a one-dimensional flow system. At the same normalized time corresponding to twice the gel-point, the CS solutions with lower NaCl concentrations result in further migration and poor performance in plugging the pore space. The viscosity computation proposed in this study is compared with another method available in the literature. It is observed that the other method estimates the viscosity at the mixing zone higher than the one proposed by the authors. The proposed model can simulate realistic injection scenarios with various combinations of operating parameters such as NaCl concentration and NaCl mixing time, and thus providing guidelines in performing this technology on site.  相似文献   

9.
Stable colloidal particles can travel long distances in subsurface environments and carry particle-reactive contaminants with them to locations further than predicted by the conventional advective-dispersive transport equation. When such carriers exist in a saturated porous medium, the system can be idealized as consisting of three phases: an aqueous phase, a carrier phase, and a stationary solid matrix phase. However, when colloids are present in an unsaturated porous medium, the system representation should include one more phase, i.e. the air phase. In the work reported, a mathematical model was developed to describe the transport and fate of the colloidal particles and a non-volatile contaminant in unsaturated porous media. The model is based on mass balance equations in a four-phase porous medium. Colloid mass transfer mechanisms among aqueous, solid matrix, and air phases, and contaminant mass transfer between aqueous and colloid phases are represented by kinetic expressions. Governing equations are non-dimensionalized and solved to investigate colloid and contaminant transport in an unsaturated porous medium. A sensitivity analysis of the transport model was utilized to assess the effects of several parameters on model behavior. The colloid transport model matches successfully with experimental data of Wan and Wilson. The presence of air-water interface retards the colloid transport significantly counterbalancing the facilitating effect of colloids. However, the retardation of contaminant transport by colloids is highly dependent on the properties of the contaminant and the colloidal surface.  相似文献   

10.
Abstract

Mass balance and fate of atrazine‐ 14C and pentachlorophenol‐ 14C (PCP‐ 14C) were studied in short‐term tests in a closed aerated laboratory soil‐plant system, using two concentrations in soil and two plant species, as well as under outdoor conditions for one vegetation period. In the laboratory, for both pesticides bioaccu‐mulation factors of radiocarbon taken up by the roots into plants were low. They were higher for lower (1 ppm) than for higher soil concentrations (6 ppm for atra‐zine, 4 ppm for pentachlorophenol) and varied with the plant species. Mineralization to 14CO2 in soil was negatively related to soil concentration only for PCP‐ 14C. Conversion rates in soil including the formation of soil‐bound residues were higher for the lower concentrations of both pesticides than for the higher ones; conversion rates in plants were species‐dependent. In 14 terms of CO2 formation and of conversion rates, PCP was less persistent in soil than was atrazine. For both pesticides, laboratory data on conversion and mineralization gave a rough prediction of their persistence in soil under long‐term outdoor conditions, whereas bio‐accumulation factors in plants under long‐term outdoor conditions could not be predicted by short‐term laboratory experiments.  相似文献   

11.
Finite-difference and finite-element methods of approximation have been extended to solve the one-dimensional nonlinear partial differential equations that describe the simultaneous transport of heat, moisture and chemical in the unsaturated zone. Especially for chemical transport, nodal spacing criteria are required to minimize numerical dispersion and oscillatory behavior in the solution vector for chemical concentration. Conservative criteria for nodal spacing for saturated flow can be used to set nodal spacing for unsaturated zone transport. When nodal spacing criteria are satisfied, for the same set of transport and boundary conditions, chemical concentration profiles calculated by the two numerical methods will be almost the same. A situation that is simulated very well with one-dimensional models, is the application of chemicals to land surfaces. To compare and contrast the characteristics of solutions given by the two numerical methods, moisture content, temperature and chemical concentration profiles for a 75-day period after application in the unsaturated zone are calculated for two representative types of organic chemicals. In the first, the chemical is very slowly degraded in the subsurface environment but strongly sorbed to soil surfaces. In the second, the chemical is rapidly degraded but weakly sorbed to soil surfaces. Because of differences in sorption coefficients and mechanisms of degradation, for the same set of hydrodynamic properties of the subsurface, the weakly sorbed chemical is more widely distributed throughout the unsaturated zone, whereas the strongly sorbed chemical stays very close to where it is put initially with little penetration into the subsurface. Satisfying nodal spacing criteria minimizes the impact of the method of approximation on the calculated solutions of the transport equations. For better model predictive performance, however, there are needs for more fundamental information on processes governing transport in the subsurface.  相似文献   

12.
The vadose zone is the intermediate medium between the atmosphere and groundwater. The modeling of the processes taking place in the vadose zone needs different approaches to those needed for groundwater transport problems because of the marked changes in environmental conditions affecting the vadose zone. A mathematical model to simulate the water flow, and the fate and transport of recalcitrant contaminants was developed, which could be applied to various bioremediation methods such as phytoremediation and natural attenuation in the vadose zone. Two-phase flow equations and heat flux models were used to develop the model. Surface energy, balance equations were used to estimate soil surface temperature, and root growth and root distribution models were incorporated to represent the special contribution of plant mots in the vegetated soils. Interactions between the roots and environmental conditions such as temperature and water content were treated by incorporating a feedback mechanism that made allowance for the effects of water and temperature stresses on root distribution and water uptake by roots. In conducting the modeling study, Johnson grass and unplanted soil were simulated to compare the effect of root water uptake on soil water content. After the numerical experiments were conducted to investigate model behavior, the proposed model was applied to estimate actual water flow and heat flow in field lysimeter experiments over a 1-year period. Root growth and distribution for Johnson grass and rye grass were simulated to compare the warm season grass to the cold season grass. A significant agreement was observed between the simulations and measured data.  相似文献   

13.
An analytical solution is presented for one-dimensional vertical transport of volatile chemicals through the vadose zone to groundwater. The solution accounts for the important transport mechanisms of the steady advection of water and gas, diffusion and dispersion in water and gas, as well as adsorption, and first-order degradation. By assuming a linear, equilibrium partitioning between water, gas and the adsorbed chemical phases, the dependent variable in the mathematical model becomes the total resident concentration. The general solution was derived for cases having a constant initial total concentration over a discrete depth interval and a zero initial total concentration elsewhere. A zero concentration gradient is assumed at the groundwater table. Examples are given to demonstrate the application of the new solution for calculating the case of a non-uniform initial source concentration, and estimating the transport of chemicals to the groundwater and the atmosphere. The solution was also used to verify a numerical code called VLEACH. We discovered an error in VLEACH, and found that the new solution agreed very well with the numerical results by corrected VLEACH. A simplified solution to predict the migration of volatile organic chemical due to the gas density effect has shown that a high source concentration may lead to significant downward advective gas-phase transport in a soil with a high air-permeability.  相似文献   

14.
This paper presents results of a numerical investigation of soil vapor extraction (SVE) systems at the laboratory scale. The SVE technique is used to remove volatile chlorinated hydrocarbons (VCHC) from the water-unsaturated soil zone. The developed numerical model solves equations of flow, transport and interfacial mass transfer regarding an isothermal n-component and three-phase system. The mathematical model is based on a simple pore network and phase distribution model and designed to be scaled by a characteristic length. All mathematical expressions are structured into VCHC specific and VCHC non-specific parameters. Furthermore, indicators are introduced that help to separate thermodynamic equilibrium from thermodynamic non-equilibrium domains and to determine the controlling physical parameters. For numerical solution, the system of partial differential equations is discretized by a finite volume method and an implicit Euler time stepping scheme. Computational effort is reduced notably through techniques that enable spatial and temporal adaptivity, through a standard multigrid method as well as through a problem-oriented sparse-matrix storage concept. Computations are carried out in two dimensions regarding the laboratory experiment of Fischer et al. [Water Resour. Res. 32 (12) 1996 3413]. By varying the characteristic length scale of the pore network and phase distribution model, it is shown that the experimental gas phase concentrations cannot be explained only by the volatility and diffusivity of the VCHC. The computational results suggest a sorption process whose significance grows with the aqueous activity of the less or non-polar organic compounds.  相似文献   

15.
A study of the (226)Ra contamination of the river sediments surrounding the Brazilian uranium mining and milling facilities was carried out. The nondetrital (226)Ra concentrations were determined performing a 0.5 N HCl leaching. Some preliminary speciations experiments using Tessier's sequential extraction procedure were also carried out. (228)Ra was used as a monitor of the natural variations. In general one could not observe increase in the non-detrital (226)Ra fraction between the pre-operational and operational data. Additionally, speciations experiments have shown the exchangeable fraction to be the main one responsible for (226)Ra content. Although the results indicate that the sediment is an important means of radium downstream transport, its availability suggests the soluble form to be the main path through the main foodchain. Attention must be paid to the release of (226)Ra bound to barium sulphate from the chemical processing effluent since increments of that fraction were observed in bottom sediments.  相似文献   

16.
A contaminant transport model was developed to simulate the fate and transport of organic compounds such as TNT (2,4,6-trinitrotoluene), using the single-root system. Onions were planted for this system with 50-ml plastic tubes. Mass in the soil, soil solution, root and leaf was monitored using 14C-TNT. Model parameters were acquired from the experiments in the single-root system and were used to simulate total TNT concentration in soil, providing the average concentrations in the rhizosphere and bulk soil as well as root and leaf compartments. Because the existing RCF (root concentration factor) and TSCF (transpiration stream concentration factor) equations based on logKow (octanol-water partition coefficient) were not correlated to TNT uptake, a new term, root uptake rate (Rur), and a new Tscf equation, based on the experimental data, were introduced in the proposed model. The results from both modeling and experimental studies showed higher concentrations of TNT in the rhizosphere than in the bulk soil, because mass transported from the surrounding soil into the rhizosphere was higher than that by root uptake.  相似文献   

17.

Background, goal, and scope

Natural radioactivity in phosphate rock (PR) is transferred to phosphate fertilizer (PF) during the manufacturing process of the PF. The continuous addition of the PF to the cultivated soil accumulates the radionuclides in the land and increases the level of radioactivity in the soil. The purpose of the present study was to investigate the enhanced level of accumulated radioactivity due to the continuous addition of the PF in the farmlands of Nuclear Institute of Agriculture and Biology (NIAB) at Faisalabad in Pakistan. The selected study area consisted of the highly fertilized farmlands and an unfertilized barren land of the NIAB.

Introduction

The understudy area is very fertile for the growth of various types of crops; therefore, four agricultural research institutes have been established at Faisalabad and NIAB is one of those. The NIAB has developed various research farmlands at different places in Pakistan. The crop yield has been increased by adding various fertilizers in the farmlands. The addition of the PF accompanied with the radionuclides enhances radioactivity in the fields. Human being is exposed directly or indirectly to this radiological hazard. A prolong exposure may become a cause of health risk.

Materials and methods

The area of study consisted of three types of lands: the land under cultivation for the last 40 and 30?years called Site 1 and Site 2, respectively, and the barren land was called Site 3. A total of 75 soil samples were collected within the crop rooting zone (up to 25?cm deep) of the soil of the NIAB farms. The samples were dried, pulverized to powder, sealed in plastic containers, and stored to achieve equilibrium between 226Ra and 222Rn. Activity concentrations of the radionuclides 238U (226Ra), 232Th, and 40K in soil samples were determined by using a high resolution gamma ray spectrometry system, consisting of an high purity germanium detector coupled through a spectroscopy amplifier with a PC based MCA installed with Geni-2000 software.

Results

The measured activity concentration levels of 40K were 662?±?15, 615?±?17, and 458?±?20?Bq?kg?1, 226Ra were 48?±?6, 43?±?5, and 26?±?4?Bq?kg?1, and that of 232Th were 39?±?5, 37?±?5, 35?±?5?Bq?kg?1, respectively, in the soil of the Sites 1, 2, and 3. Gamma dose rate 1?m above the soil surface was 55, 51, and 40?nGy?h?1 from Sites 1, 2, and 3, respectively. External dose rates in the rooms constructed of the bricks made of the soil from Sites 1, 2, and 3 were 161, 149, and 114?nGyh?1, respectively.

Discussions

Activity concentration values of 40K and 226Ra in the soil of Sites 1 and 2 were higher than that in the soil of Site 3. The relative rise of 40K was 43?% and 34?% and that of 226Ra was 85?% and 65?% respectively in these sites. Activity concentrations of 232Th in all these sites were in the background range. Gamma dose rate 1?m above soil surface of Sites 1 and 2 was 40?% and 30?% respectively higher than that from the soil of Site 3. The rise in activity of 40K and 226Ra and gamma dose from the Site 1 was greater than that from the Site 2. The least activity and dose were observed from the Site 3. Gamma dose in the dwellings made of fertilized soil bricks of Site 1 and Site 2 were respectively calculated to be 41?% and 32?% higher than that in the abodes made of unfertilized soil bricks of Site 3.

Conclusions

Activity concentrations of 226Ra and 40K were observed to be enhanced in the fertilized farmlands of the NIAB. Outdoor and indoor gamma dose as radiological hazard were found to be increasing with the continuous addition of PF in the understudy farmlands.

Recommendations

It is recommended that naturally occurring radioactive metal should be removed during the process of manufacturing of the PF from the PR.

Prospective

The rise in radioactivity in the farmlands due to the addition of the PF can be a source of direct or indirect exposure to radiation that may enhance cancer risk of the exposed individuals.  相似文献   

18.
Continuous time random walk (CTRW) formulations have been demonstrated to provide a general and effective approach that quantifies the behavior of solute transport in heterogeneous media in field, laboratory, and numerical experiments. In this paper we first apply the CTRW approach to describe the sorbing solute transport in soils under chemical (or) and physical nonequilibrium conditions by curve-fitting. Results show that the theoretical solutions are in a good agreement with the experimental measurements. In case that CTRW parameters cannot be determined directly or easily, an alternative method is then proposed for estimating such parameters independently of the breakthrough curve data to be simulated. We conduct numerical experiments with artificial data sets generated by the HYDRUS-1D model for a wide range of pore water velocities (υ) and retardation factors (R) to investigate the relationship between CTRW parameters for a sorbing solute and these two quantities (υ, R) that can be directly measured in independent experiments. A series of best-fitting regression equations are then developed from the artificial data sets, which can be easily used as an estimation or prediction model to assess the transport of sorbing solutes under steady flow conditions through soil. Several literature data sets of pesticides are used to validate these relationships. The results show reasonable performance in most cases, thus indicating that our method could provide an alternative way to effectively predict sorbing solute transport in soils. While the regression relationships presented are obtained under certain flow and sorption conditions, the methodology of our study is general and may be extended to predict solute transport in soils under different flow and sorption conditions.  相似文献   

19.
Perchlorate is a stable anion that has been introduced into the environment through activities related to its production and use as a solid rocket propellant. Perchlorate is thought to transport through soils without being adsorbed; thus, for determination of perchlorate in soil, samples are typically extracted with water prior to analysis. The completeness of extraction depends on perchlorate existing as a free ion within the soil matrix. In this study, perchlorate extraction efficiency was evaluated with five soil types under two different oxygen states. For each soil, 30% (w/w) slurries were prepared and equilibrated under either oxic or anoxic conditions prior to spiking with a stock solution of sodium perchlorate, and the slurries were then maintained for 1-week or 1-month. At the end of the exposure, slurries were centrifuged and separated into aqueous and soil phases. After phase separation, the soil was washed first with deionized water and then with 50mM NaOH, producing second and third aqueous phases, respectively. Perchlorate concentrations in the three aqueous phases were determined using ion chromatography. The results obtained from this study suggest that matrix interference and signal suppression due to high conductivity have greater effects upon observed perchlorate concentrations by ion chromatography than does perchlorate interaction with soil. Thus, a single water extraction is sufficient for quantitative determination of perchlorate in soil.  相似文献   

20.
The results of seven years lysimeter experiments to determine the uptake of 60Co, 137Cs and 226Ra into agricultural crops (endive, maize, wheat, mustard, sugarbeet, potato, Faba bean, rye grass) are described. The lysimeter consists of twelve monolithic soil profiles (four soil types and three replicates) and is located in Seibersdorf/Austria, a region with a pannonian climate (pronounced differences between hot and semi-arid summers and humid winter conditions, annual mean of precipitation: 517 mm, mean annual temperature: 9.8 degrees C). Besides soil-to-plant transfer factors (TF), fluxes were calculated taking into account biomass production and growth time. Total median values of TF's (dry matter basis) for the three radionuclides decreased from 226Ra (0.068 kg kg(-1)) to 137Cs (0.043 kg kg(-1)) and 60Co (0.018 kg kg(-1)); flux values exhibited the same ranking. The varying physical and chemical properties of the four experimental soils resulted in statistically significant differences in transfer factors or fluxes between the investigated soils for 137Cs and 226Ra, but not for 60Co. Differences in transfer between plant species and plant parts are distinct, with graminaceous species showing, on average, TF values 5.8 and 15 times lower than dicotyledonous species for 137Cs and 60Co, respectively. This pattern was not found for 226Ra. It can be concluded that 137Cs transfer is heavily influenced by soil characteristics, whilst the plant-specific factors are the main source of TF variability for 60Co. The variability of 226Ra transfer originates both from soil properties and plant species behaviour.  相似文献   

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