Influence of melt‐freeze‐cycles on the radionuclide transport in homogeneous laboratory snowpack

Radionuclides released to the environment and deposited with or onto snow can be stored over long time periods if ambient temperature stays low, particularly in glaciated areas or high alpine sites. The radionuclides will be accumulated in the snowpack during the winter unless meltwater runoff at the snow base occurs. They will be released to surface waters within short time during snowmelt in spring. In two experiments under controlled melting conditions of snow in the laboratory, radionuclide migration and runoff during melt‐freeze‐cycles were examined. The distribution of Cs‐134 and Sr‐85 tracers in homogeneous snow columns and their fractionation and potential preferential elution in the first meltwater portions were determined. Transport was associated with the percolation of meltwater at ambient temperatures above 0 °C after the snowpack became ripe. Mean migration velocities in the pack were examined for both nuclides to about 0.5 cm hr^?1 after one diurnal melt‐freeze‐cycle at ambient temperatures of ?2 to 4 °C. Meltwater fluxes were calculated with a median of 1.68 cm hr^?1. Highly contaminated portions of meltwater with concentration factors between 5 and 10 against initial bulk concentrations in the snowpack were released as ionic pulse with the first meltwater. Neither for caesium nor strontium preferential elution was observed. After recurrent simulated day‐night‐cycles (?2 to 4 °C), 80% of both radionuclides was released with the first 20% of snowmelt within 4 days. 50% of Cs‐134 and Sr‐85 were already set free after 24 hr. Snowmelt contained highest specific activities when the melt rate was lowest during the freeze‐cycles due to concentration processes in remaining liquids, enhanced by the melt‐freeze‐cycling. This implies for natural snowpack after significant radionuclide releases, that long‐time accumulation of radionuclides in the snow during frost periods, followed by an onset of steady meltwater runoff at low melt rates, will cause the most pronounced removal of the contaminants from the snow cover. This scenario represents the worst case of impact on water quality and radiation exposure in aquatic environments.     

Bentonite as a Natural Adsorbent for the Sorption of Iron from the Ground Water Exploited from Aswan Area, Egypt

Sorption of dissolved Fe²⁺ on bentonite was studied using a batch technique. The distribution coefficient, K_d , was evaluated for a bentonite-iron system as a function of contact time, pH, sorbent and sorbate concentrations, and temperature. Sorption results were interpreted in terms of Freundlich's and Langmuir's equations. Thermodynamic parameters for the sorption system were determined at three temperatures: 298°, 308°, and 318°K. The values of ΔH°(-4.0 kjmol⁻¹) and ΔG°(-2.46 Kjmol⁻¹) at 298°K (25°C) suggest that sorption of iron on bentonite is an exothermic and a spontaneous process. The ΔG° value became less negative at higher temperatures and, therefore, less iron was sorbed at higher temperatures. The desorption studies with 0.01 M CaCl₂ and deionized water at iron loading on bentonite showed that more than 90 wt% of the iron is irreversibly sorbed, probably due to the fixation of the iron by isomorphous replacement in the crystal lattice of the sorbent.     

Effect of heterogeneity on radionuclide retardation in the alluvial aquifer near Yucca Mountain, Nevada

The U.S. Department of Energy is currently studying Yucca Mountain, Nevada, as a potential site for a geological high-level waste repository. In the current conceptual models of radionuclide transport at Yucca Mountain, part of the transport path to pumping locations would be through an alluvial aquifer. Interactions with minerals in the alluvium are expected to retard the downstream migration of radionuclides, thereby delaying arrival times and reducing ground water concentrations. We evaluate the effectiveness of the alluvial aquifer as a transport barrier using the stochastic Lagrangian framework. A transport model is developed to account for physical and chemical heterogeneities and rate-limited mass transfer between mobile and immobile zones. The latter process is caused by small-scale heterogeneity and is thought to control the macroscopic-scale retardation in some field experiments. A geostatistical model for the spatially varying sorption parameters is developed from a site-specific database created from hydrochemical measurements and a calibrated modeling approach (Turner and Pabalan 1999). Transport of neptunium is considered as an example. The results are sensitive to the rate of transfer between mobile and immobile zones, and to spatial variability in the hydraulic conductivity. Chemical heterogeneity has only a small effect, as does correlation between hydraulic conductivity and the neptunium distribution coefficient. These results illustrate how general sensitivities can be explored with modest effort within the Lagrangian framework. Such studies complement and guide the application of more detailed numerical simulations.     

Remediation of Radionuclide Pollutants through Biosorption – an Overview

The development of nuclear science and technology has led to the increase of nuclear wastes containing radionuclides to be released and disposed in the environment. Pollution caused by radionuclides is a serious problem throughout the world. To solve the problem, substantial research efforts have been directed worldwide to adopt sustainable technologies for the treatment of radionuclide containing wastes. Biosorption represents a technological innovation as well as a cost effective excellent remediation technology for cleaning up radionuclides from aqueous environment. A variety of biomaterials viz. algae, fungi, bacteria, plant biomass, etc. have been reported for radionuclide remediation with encouraging results. This paper reviews the achievements and current status of radionuclide remediation through biosorption which will provide insights into this research frontier.     

Assessment of radionuclide transport uncertainty in the unsaturated zone of Yucca Mountain

The present study assesses the uncertainty of flow and radionuclide transport in the unsaturated zone at Yucca Mountain using a Monte Carlo method. Matrix permeability, porosity, and sorption coefficient are considered random. Different from previous studies that assume distributions of the parameters, the distributions are determined in this study by applying comprehensive transformations and rigorous statistics to on-site measurements of the parameters. The distribution of permeability is further adjusted based on model calibration results. Correlation between matrix permeability and porosity is incorporated using the Latin Hypercube Sampling method. After conducting 200 Monte Carlo simulations of three-dimensional unsaturated flow and radionuclide transport for conservative and reactive tracers, the mean, variances, and 5th, 50th, and 95th percentiles for quantities of interest (e.g., matrix liquid saturation and water potential) are evaluated. The mean and 50th percentile are used as the mean predictions, and their associated predictive uncertainties are measured by the variances and the 5th and 95th percentiles (also known as uncertainty bounds). The mean predictions of matrix liquid saturation and water potential are in reasonable agreement with corresponding measurements. The uncertainty bounds include a large portion of the measurements, suggesting that the data variability can be partially explained by parameter uncertainty. The study illustrates propagation of predictive uncertainty of percolation flux, increasing downward from repository horizon to water table. Statistics from the breakthrough curves indicate that transport of the reactive tracer is delayed significantly by the sorption process, and prediction on the reactive tracer is of greater uncertainty than on the conservative tracer because randomness in the sorption coefficient increases the prediction uncertainty. Uncertainty in radionuclide transport is related to uncertainty in the percolation flux, suggesting that reducing the former entails reduction in the latter.     

Spatial moments for colloid-enhanced radionuclide transport in heterogeneous aquifers

We consider colloid facilitated radionuclide transport by steady groundwater flow in a heterogeneous porous formation. Radionuclide binding on colloids and soil-matrix is assumed to be kinetically/equilibrium controlled. All reactive parameters are regarded as uniform, whereas the hydraulic log-conductivity is modelled as a stationary random space function (RSF). Colloid-enhanced radionuclide transport is studied by means of spatial moments pertaining to both the dissolved and colloid-bounded concentration. The general expressions of spatial moments for a colloid-bounded plume are presented for the first time, and are discussed in order to show the combined impact of sorption processes as well as aquifer heterogeneity upon the plume migration. For the general case, spatial moments are defined by the aid of two characteristic reaction functions which cannot be expressed analytically. By adopting the approximation for the longitudinal fluid trajectory covariance valid for a flow parallel to the formation bedding suggested by Dagan and Cvetkovic [Dagan G, Cvetkovic V. Spatial Moments of Kinetically Sorbing Plume in a Heterogeneous Aquifers. Water Resour Res 1993;29:4053], we obtain closed form solutions.     

Incorporation of conceptual and parametric uncertainty into radionuclide flux estimates from a fractured granite rock mass

Detailed numerical flow and radionuclide simulations are used to predict the flux of radionuclides from three underground nuclear tests located in the Climax granite stock on the Nevada Test Site. The numerical modeling approach consists of both a regional-scale and local-scale flow model. The regional-scale model incorporates conceptual model uncertainty through the inclusion of five models of hydrostratigraphy and five models describing recharge processes for a total of 25 hydrostratigraphic–recharge combinations. Uncertainty from each of the 25 models is propagated to the local-scale model through constant head boundary conditions that transfer hydraulic gradients and flow patterns from each of the model alternatives in the vicinity of the Climax stock, a fluid flux calibration target, and model weights that describe the plausibility of each conceptual model. The local-scale model utilizes an upscaled discrete fracture network methodology where fluid flow and radionuclides are restricted to an interconnected network of fracture zones mapped onto a continuum grid. Standard Monte Carlo techniques are used to generate 200 random fracture zone networks for each of the 25 conceptual models for a total of 5,000 local-scale flow and transport realizations. Parameters of the fracture zone networks are based on statistical analysis of site-specific fracture data, with the exclusion of fracture density, which was calibrated to match the amount of fluid flux simulated through the Climax stock by the regional-scale models. Radionuclide transport is simulated according to a random walk particle method that tracks particle trajectories through the fracture continuum flow fields according to advection, dispersion and diffusional mass exchange between fractures and matrix. The breakthrough of a conservative radionuclide with a long half-life is used to evaluate the influence of conceptual and parametric uncertainty on radionuclide mass flux estimates. The fluid flux calibration target was found to correlate with fracture density, and particle breakthroughs were generally found to increase with increases in fracture density. Boundary conditions extrapolated from the regional-scale model exerted a secondary influence on radionuclide breakthrough for models with equal fracture density. The incorporation of weights into radionuclide flux estimates resulted in both noise about the original (unweighted) mass flux curves and decreases in the variance and expected value of radionuclide mass flux.     

Evaluation of Hydrogeo-chemical Conditions for Development of Nuclear Criticality in Low-Level Waste Disposal Facilities

The under ground disposal of fissile isotope-bearing wastes poses some unique issues. Specifically, radionuclides such as ²³⁵U disposed in low-level waste facilities, if present in the correct concentration and geometry, can create a nuclear criticality event that releases radioactivity to ground water. This paper reports the results of a study of the potential for ²³⁵U to be transported by ground water within low-level waste facilities and to concentrate to form a critical mass. Coupled hydrologic and geochemical modeling was used to investigate two possible mechanisms for concentrating mobile uranium: sorption on high capacity sites and precipitation in a reducing zone. The hydrogeochemical modeling showed that (1) it is difficult to mobilize uranium from sorption sites then re-deposit it; (2) if uranium is already in solution it can accumulate in zones of high sorption, and (3) reducing zones can accumulate sufficient uranium in the presence of oxygenated ground water. Site-specific disposal practices, such as the commingling of large quantities of depleted (nonfissile) uranium and the difficulty of bringing sufficient mass together in the correct geometry, limit the potential for criticality safety concerns. In order to determine appropriate disposal practices, hydrogeochemical modeling can be used to study the future mobility and accumulation of the waste.     

Sorption site capacities for Cs on the sedimentary rock in Horonobe area

The sorption behavior of radionuclides depends on the content of minerals in geological media. The sorption of radionuclides on minerals has been interpreted as the uptake on the sorption sites on mineral surfaces. However, conventional investigations such as X-ray diffraction analysis cannot avoid large errors in quantification of minerals. Furthermore, the discrepancies of sorption behavior have been often found even on the same kind of minerals. Therefore, the sorption site capacity cannot be effectively estimated by the quantification of minerals. In this study, the sorption site on sedimentary rock sampled in Horonobe area, where the Horonobe Underground Research Center, JAEA, is located, was estimated from the Cs sorption isotherms obtained by sorption experiments. To deduce the fitting parameters, illite content estimated from the amount of extracted K by alkylammonium treatment and smectite content estimated from the cation exchange capacity measurement were introduced to the fitting procedure. The result shows that the sorption site capacities of smectite and illite in the sedimentary rock in Horonobe area are 1.3–1.7 × 10⁻⁴ and 1.4–4.0 × 10⁻⁵ eq/g, respectively.     

Radionuclide Sorption on Well Construction Materials

Laboratory experiments were conducted to measure the extent to which trace concentrations of radioactive materials would sorb on well construction materials and to assess the rapidity with which sorption would occur. The radionuclides employed in these studies were tritium, Cs-137, and Co-57, Solutions with trace concentrations of these radionuclides were contracted with casings of PVC, fiberglass-epoxy, stainless steel, carbon steel, and steel rods coated wtih expoy. The PVC showed no interaction with the tritium or Cs-137 during contact times of two hours to these weeks; however, it did sorb Co-57. The fiberglass-epoxy also interacted only with the cobalt. The stainless steel sorbed cesium and cobalt. The carbon steel (or the ferric hydroxide forming on its surface) also sorbed both cesium and cobalt. The epoxy-coated steel rods did not interact measurably with day of the radio-nuclides so long as the coating was intact. The sorption reactions generally were apparent after a few days of contact: in the case of carbon steel, they were detectable in a few hours.     

Uptake of radioactivity by marine sediments and implications for monitoring metal pollutants

The value of studying artificially-produced radionuclides in the marine environment is discussed in the wider context of monitoring sediments for other metal pollutants. Differences in the dispersion of selected radionuclides discharged from the same known source are used to illustrate the sort of changes in phase or speciation which must occur with other metal pollutants, but which cannot be demonstrated directly because of the multiplicity of sources. Various chemical and physical procedures are discussed which can be applied to a study of heavy metal associations with marine sediments, as are questions such as the existence, or otherwise, of mechanisms for the slow release of adsorbed material from the buried sediment back into the water column. Suggestions are made as to how radionuclide studies may be helpful in answering questions such as these, which are considered to be vital for the meaningful interpretation of sediment analyses.     

Utilizing Natural Liner Materials for Heavy Metal Removal in Simulated Landfill Conditions

Inorganic industrial waste landfills have the potential to contaminate subsurface groundwater supplies through migration of leachates down to the water table and into groundwater aquifers, despite the use of compacted low permeability clay or polyethene liners. This paper aims the removal of Cu²⁺ and Zn²⁺ in the leachate from an industrial waste landfill using natural materials (natural zeolite, expanded vermiculite, pumice, illite, kaolinite, and bentonite) as a liner material. Cu²⁺ and Zn²⁺ concentrations for all treatments decreased during the process. Of all the different natural materials, natural zeolite, expanded vermiculite and pumice, with bentonite, were effective in removing Cu²⁺ and Zn²⁺ present in the leachate. However, the use of illite and kaolinite with bentonite as liner materials could be of disadvantage in Cu²⁺ and Zn²⁺ removal from leachate. The adsorption kinetic models were also tested for the validity. The second order kinetics with the high correlation coefficients best described adsorption kinetic data.     

Production of selected cosmogenic radionuclides by muons 1. Fast muons

To investigate muon-induced nuclear reactions leading to the production of radionuclides, targets made of C₉H₁₂, SiO₂, Al₂O₃, Al, S, CaCO₃, Fe, Ni, Cu, Gd, Yb and Tl were irradiated with 100 and 190 GeV muons in the NA54 experimental setup at CERN. The radionuclide concentrations were measured with accelerator mass spectrometry and γ-spectroscopy. Results are presented for the corresponding partial formation cross-sections. Several of the long-lived and short-lived radionuclides studied are also produced by fast cosmic ray muons in the atmosphere and at depths underground. Because of their importance to earth sciences investigations, calculations of the depth dependence of production rates by fast cosmic ray muons have been made.     

Spatial variability in sedimentation rates and artificial radionuclide storage in alluvial banks of the lower Rh?ne River

This paper analyzes the relationship between bank sediment storage and radionuclide content in six alluvial sites located in different geomorphic contexts along the lower Rh?ne River. The ¹³⁷Cs, ²³⁸Pu, ^239+240Pu, ²⁴¹Am and ²¹⁰Pb profiles show different patterns, which indicates a differential storage of contaminated sediment in the banks. Three sites record historical nuclear releases in the river and give evidence for long-term retention of particle-reactive long-lived radionuclides. Two sites record only atmospheric global fallout. Only one site, connected to the river groundwater, provides some evidence for desorption of particle-bound contaminants, with a low and constant ¹³⁷Cs activity profile. The history of the releases from the Marcoule spent-fuel reprocessing plant—the main source of artificial radioactivity—provides a reliable chronology of the last 50?years. Sediment grain size and bank topography are important factors in determining where artificial radionuclides are stored, but these two parameters cannot be used alone to determine variations in high concentrations of radionuclides. The chronology of fluvial geomorphic “metamorphosis” during the twentieth Century, especially after 1960, is also a critical factor affecting the spatial variability in sedimentation rates and artificial radionuclide storage; the timing of channel deepening and bank sedimentary accretion interfere with the chronology of major floods and the short period of low discharge during the height of contamination from nuclear liquid effluents. The reach-scale adjustment described in this paper can contribute to determining what the local history may have been. This result has important implications for river management decisions.     

The role of the water/soil distribution coefficient in the watershed transport of environmental radionuclides

The concept of the distribution coefficient is invoked to rationalize the observed dependence of the watershed residence time of a radionuclide on its nature. A mathematical model is presented to show that this residence time is proportional to the dimensionless field distribution coefficient of the radionuclide. The proportionality constant, β, is defined as the ratio of the volume of rain-impacted soil in the watershed and the annual volume of rainfall in the watershed or expressed as the ratio between the water penetration depth in soil and the annual thickness of water above the soil surface. An empirical evaluation of β supports our assumption of its constancy in a given watershed. The described model may be very useful in deciphering the impact of atmospherically delivered pollutants on watershed quality. Expressions are also derived to estimate the value of soil erosion constant using naturally occurring radionuclides.     

Evaluating Long-Term Evolution of Radionuclide Migration Conditions from a Repository at the Yenisei Site (Krasnoyarsk Krai)

The article considers the procedure aimed to identify and select the factors, events, and processes that can have an effect on the long-term safety of radioactive waste repository to be constructed at The Yenisei Site (Krasnoyarsk krai). The geological factors to be taken into account in the development of scenarios for safety assessment are determined. Tentative quantitative forecasts of radionuclide migration are made taking into account possible climate evolution and vertical rise of the territory. The sensitivity of radionuclide migration model to variations in these factors is assessed.     

An operational model to simulate post-accidental radionuclide transfers in Toulon marine area: preliminary development

As part of its development of post-accident management tools, the French Institute for Radiological Protection and Nuclear Safety is setting up a model to simulate radionuclide dispersion in the Toulon marine area (one of France’s main military ports). The model is based on the MARS 3D code developed by IFREMER. It reproduces hydro-sedimentation phenomena in the Bay of Toulon with a horizontal spatial resolution of 100 m and 30 vertical sigma levels and also factors in radioactive decay and dissolved/particulate distribution of the radionuclides studied. With no tide, the major currents in this area are generated by the wind. The model effectively reproduces the resulting hydrodynamic phenomena, which were measured throughout the summer of 2009 in the channel that links the Little Bay to the Large Bay of Toulon. When the Mistral (wind from the West/Northwest) blows, a surface current quickly appears, which pushes water southwards from the Little Bay, and which is offset by a bottom current (upwellings). When the wind blows from the East, the currents move in the opposite direction, and southeasterly waves, dependent on wind strength and fetch, occur in the Large Bay. Here, we give an example of the simulated dispersion of radionuclides released directly into the surface waters near the Arsenal, demonstrating the constraint relative to dispersion generated by the half-closed configuration of the Little Bay. Sediment in the Little Bay also forms an area where the most highly reactive radionuclides would accumulate, and where the lack of waves has the effect of considerably limiting the phenomena of resuspension.     

Sorption of heavy oil onto Jiaozhou Bay sediment

The sorption of heavy oil onto sediment collected from Jiaozhou Bay was studied in a series of kinetic and equilibrium experiments using NaCl solutions. The effects of temperature, salinity, and pH of the medium on sorption behavior were investigated.Sorption equilibrium of the heavy oil and sediment was established within 60 min. The process was shown to follow a pseudo-second-order kinetic rate model. The sorption rate decreased with increasing initial heavy oil concentration in the solution. Batch equilibrium experiments showed that the sorption isotherm could be described by the Freundlich model. The standard free energy change and enthalpy change at the temperatures studied (283, 288, 293, and 298 K) were negative. These findings indicated that the process was spontaneous and exothermic. Salinity, pH and temperature influenced sorption performance. Sorption was favored by higher concentrations of NaCl, by lower pH values and by lower temperatures.     

Radionuclides and large particles in estuarine sediments

Radionuclides, released into the north-east Irish Sea from the British Nuclear Fuels plc uranium reprocessing plant at Sellafield, Cumbria, UK and which are present in sediments of the Esk estuary, Cumbria, are initially associated with large (i.e. >0.5 mm) rather than fine grained (i.e. <63 μm) particles. I call these macro particles organoliths. They consist of an agglomerate of sediment grains held together with an organic iron rich matrix; their surfaces are coated with a patina of iron and manganese oxides with which the radionuclides are associated. Concentration factors (Kd's) for plutonium, americium, and other radionuclides, together with various stable elements in the patina are orders of magnitude greater than those found in bulk sediments. Some implications concerning the radionuclide content of organoliths are discussed in relation to geochemical process, pollution studies and the requirements of radiological protection.     

Stochastic study of solute transport in a nonstationary medium

A Lagrangian stochastic approach is applied to develop a method of moment for solute transport in a physically and chemically nonstationary medium. Stochastic governing equations for mean solute flux and solute covariance are analytically obtained in the first-order accuracy of log conductivity and/or chemical sorption variances and solved numerically using the finite-difference method. The developed method, the numerical method of moments (NMM), is used to predict radionuclide solute transport processes in the saturated zone below the Yucca Mountain project area. The mean, variance, and upper bound of the radionuclide mass flux through a control plane 5 km downstream of the footprint of the repository are calculated. According to their chemical sorption capacities, the various radionuclear chemicals are grouped as nonreactive, weakly sorbing, and strongly sorbing chemicals. The NMM method is used to study their transport processes and influence factors. To verify the method of moments, a Monte Carlo simulation is conducted for nonreactive chemical transport. Results indicate the results from the two methods are consistent, but the NMM method is computationally more efficient than the Monte Carlo method. This study adds to the ongoing debate in the literature on the effect of heterogeneity on solute transport prediction, especially on prediction uncertainty, by showing that the standard derivation of solute flux is larger than the mean solute flux even when the hydraulic conductivity within each geological layer is mild. This study provides a method that may become an efficient calculation tool for many environmental projects.