Radionuclide release and transport from nuclear underground tests performed at Mururoa and Fangataufa — predictions under uncertainty

In the context of a study by the International Geomechanical Commission (IGC) and the International Atomic Energy Agency (IAEA) on the effects of nuclear tests at the atolls of Mururoa and Fangataufa, release to the biosphere is estimated for 35 radionuclides originating from 147 nuclear underground tests. Based on a qualitatively characterised hydrogeological situation of atolls and relatively scarce site-specific data, a model chain was developed to conservatively estimate the radionuclide fluxes via groundwater, from their sources, the explosion cavities, towards the biosphere, the ocean or lagoon.Finite element hydro-thermal modelling was used to describe water flow. Parameters were calibrated by a very few measured pre-test temperature profiles in bore holes. The impact of the tests on groundwater flow and mechanical impact on rock was considered. Estimates were made to quantify spatial extensions and temporal evolution of impact by using measurements on refilling rate of the cavities. Tests were categorised according to their specific yield and location although detailed data were missing. A base case parameter set was defined for the hydraulic conditions and for the initial radionuclide inventory of individual tests. Models were used to describe the concentration of radionuclides in the cavities as a function of time. Radionuclide transport from the cavities to the biosphere was represented by two different approaches: a double porosity model for the fractured volcanic rock and a single porosity model for the overlaying, highly porous carbonates. Results consist of conservative estimates on radionuclide release into the environment, or concentration in the lagoon or ocean water. Their sensitivity was investigated using different models and parameters. A few measured data (concentrations in a few cavities, in the deep carbonates and in the lagoons for selected radionuclides, such as ³H, ¹⁴C, ³⁶Cl, ⁹⁰Sr, ¹²⁹I, ¹³⁷Cs²³⁹, ²⁴⁰Pu and ²⁴¹Am) were available for a comparison with the calculations. In view of the lack and uncertainty of site-specific data, the agreement is of acceptable quality.     

Modeling the long-term transport and accumulation of radionuclides in the landscape for derivation of dose conversion factors

To evaluate the radiological impact of potential releases to the biosphere from a geological repository for spent nuclear fuel, it is necessary to assess the long-term dynamics of the distribution of radionuclides in the environment. In this paper, we propose an approach for making prognoses of the distribution and fluxes of radionuclides released from the geosphere, in discharges of contaminated groundwater, to an evolving landscape. The biosphere changes during the temperate part (spanning approximately 20,000 years) of an interglacial period are handled by building biosphere models for the projected succession of situations. Radionuclide transport in the landscape is modeled dynamically with a series of interconnected radioecological models of those ecosystem types (sea, lake, running water, mire, agricultural land and forest) that occur at present, and are projected to occur in the future, in a candidate area for a geological repository in Sweden. The transformation between ecosystems is modeled as discrete events occurring every thousand years by substituting one model by another. Examples of predictions of the radionuclide distribution in the landscape are presented for several scenarios with discharge locations varying in time and space. The article also outlines an approach for estimating the exposure of man resulting from all possible reasonable uses of a potentially contaminated landscape, which was used for derivation of Landscape Dose Factors.     

Field investigation into unsaturated flow and transport in a fault: model analyses

Results of a fault test performed in the unsaturated zone of Yucca Mountain, Nevada, were analyzed using a three-dimensional numerical model. The fault was explicitly represented as a discrete feature and the surrounding rock was treated as a dual-continuum (fracture-matrix) system. Model calibration against seepage and water-travel-velocity data suggests that lithophysal cavities connected to fractures can considerably enhance the effective fracture porosity and therefore retard water flow in fractures. Comparisons between simulation results and tracer concentration data also indicate that matrix diffusion is an important mechanism for solute transport in unsaturated fractured rock. We found that an increased fault-matrix and fracture-matrix interface areas were needed to match the observed tracer data, which is consistent with previous studies. The study results suggest that the current site-scale model for the unsaturated zone of Yucca Mountain may underestimate radionuclide transport time within the unsaturated zone, because an increased fracture-matrix interface area and the increased effective fracture porosity arising from lithophysal cavities are not considered in the current site-scale model.     

Laboratory migration experiments with radionuclides and natural colloids in a granite fracture

Natural colloids in groundwater could facilitate radionuclide transport, provided the colloids are mobile, are present in sufficient concentrations and can adsorb radionuclides. This paper describes the results of a laboratory migration study carried out with combinations of radionuclides and natural colloids within a fracture in a large granite block to experimentally determine the impact of colloids on radionuclide transport. The 85Sr used in this study is an example of a moderately sorbing radionuclide, while the 241Am is typical of a strongly sorbed radionuclide with very low solubility. The natural colloids used in this study were isolated from granite groundwater from Atomic Energy of Canada (AECL) Underground Research Laboratory (URL), and consisted of mostly 1-10 nm organic colloids, along with lesser amounts of 10-450 nm colloids (organics and aluminosilicates). The measured coefficients for radionuclide sorption onto these colloids were between 3 x 10(2) and 1 x 10(3) ml/g for 85Sr, and between 7 x 10(4) and 7 x 10(5) mg/l for 241Am. The 85Sr sorption on the natural colloids appeared to be reversible. Migration experiments in the granite block were carried out by establishing a flow field between two boreholes (out of a total of nine) intersecting a main horizontal fracture. These experiments showed that dissolved 85Sr behaved as a moderately sorbing tracer, while dissolved 241Am was completely adsorbed by the fracture surfaces and showed no evidence of transport. However, when natural colloids were injected together with dissolved 241Am, a small amount of 241Am transport was observed, demonstrating the ability of natural colloids to facilitate the transport of radionuclides with low solubility. Natural colloids had only a minor effect on the transport of 85Sr. In a separate experiment to test the effect of higher colloid concentrations on 85Sr migration, synthetic colloids were produced from Avonlea bentonite. The introduction of a relatively high concentration of bentonite colloids actually reduced 85Sr transport because, compared to natural colloids, the bentonite colloids were less mobile and they sorbed 85Sr more strongly.     

Mobile fission and activation products in nuclear waste disposal

When disposing nuclear waste in clay formations it is expected that the most radiotoxic elements like Pu, Np or Am move only a few centimetres to meters before they decay. Only a few radionuclides are able to reach the biosphere and contribute to their long-term exposure risks, mainly anionic species like I129, Cl36, Se79 and in some cases C14 and Tc99, whatever the scenario considered. The recent OECD/NEA cosponsored international MOFAP workshop focussed on transport and chemical behaviour of these less toxic radionuclides. New research themes have been addressed, such as how to make use of molecular level information for the understanding of the problem of migration at large distances. Diffusion studies need to face mineralogical heterogeneities over tens to hundreds of meters. Diffusion rates are very low since the clay rock pores are so small (few nm) that electrostatic repulsion limits the space available for anion diffusion (anion exclusion). The large volume of traversed rock will provide so many retention sites that despite weak retention, even certain of these “mobile” nuclides may show significant retardation. However, the question how to measure reliably very low retention parameters has been posed. An important issue is whether redox states or organic/inorganic speciation change from their initial state at the moment of release from the waste during long term contact with surfaces, hydrogen saturated environments, etc.     

A serendipitous, long-term infiltration experiment: Water and tritium circulation beneath the CAMBRIC trench at the Nevada Test Site

Underground nuclear weapons testing at the Nevada Test Site introduced numerous radionuclides that may be used subsequently to characterize subsurface hydrologic transport processes in arid climates. In 1965, a unique, 16-year pumping experiment designed to examine radionuclide migration away from the CAMBRIC nuclear test, conducted in the saturated zone beneath Frenchman Flat, Nevada, USA, gave rise to an unintended second experiment involving radionuclide infiltration through the vadose zone, as induced by seepage of pumping effluents beneath an unlined discharge trench. The combined experiments have been reanalyzed using a detailed, three-dimensional numerical model of transient, variably saturated flow and mass transport in a heterogeneous subsurface, tailored specifically for large-scale and efficient calculations. Simulations have been used to estimate tritium travel and residence times in various parts of the system for comparison with observations in wells. Model predictions of mass transport were able to clearly demonstrate radionuclide recycling behavior between the trench and pumping well previously suggested by isotopic age dating information; match travel time estimates for radionuclides moving between the trench, the water table, and monitoring and pumping wells; and provide more realistic ways in which to interpret the pumping well elution curves. Collectively, the results illustrate the utility of integrating detailed numerical modeling with diverse observational data in developing more accurate interpretations of contaminant migration processes.     

Bages-Sigean and Canet-St Nazaire lagoons (France): physico-chemical characteristics and contaminant concentrations (Cu,Cd, PCBs and PBDEs) as environmental quality of water and sediment

Environmental characteristics in water and sediments of two contrasted coastal Mediterranean lagoons, Bages-Sigean and Canet-St Nazaire, were measured over a three season survey. The urban pollution (treatment plant discharges) is very important in Canet-St Nazaire lagoon reflecting untreated sewages, while in Bages-Sigean, the northern part appears more impacted due to larger anthropogenic inputs. Dissolved Cd concentrations are on the whole similar in both lagoons, whereas Cu concentrations are by far higher in lagoon Canet-St Nazaire. Cu concentrations appear to be highly dependent on dissolved organic carbon whereas salinity seems to control Cd variations. Concerning the sediments, the confined northern part of lagoon Bages-Sigean shows organic carbon and total nitrogen enrichment whereas lipid concentrations are much higher in the Canet-St Nazaire lagoon. Cu complexation seems to be strongly related to organic matter as evidenced by the two significant positive relationships, on one hand between Cu and organic carbon, and on the other hand, between Cu and lipids. On the contrary, Cd concentrations appear to be mainly controlled by carbonates. PCBs and PBDEs were detected only in sediments and show relatively low concentrations compared to similar lagoon environments. Regarding the sediment quality guidelines, Cd, Cu and PCBs in both lagoons did not exceed any Probable Effect Concentration (PEC).     

Modelling radionuclide distribution and transport in the environment

Mathematical models of radionuclide distribution and transport in the environment have been developed to assess the impact on people of routine and accidental releases of radioactivity from a variety of nuclear activities, including: weapons development, production, and testing; power production; and waste disposal. The models are used to estimate human exposures and doses in situations where measurements have not been made or would be impossible or impractical to make. Model results are used to assess whether nuclear facilities are operated in compliance with regulatory requirements, to determine the need for remediation of contaminated sites, to estimate the effects on human health of past releases, and to predict the potential effects of accidental releases or new facilities. This paper describes the various applications and types of models currently used to represent the distribution and transport of radionuclides in the terrestrial and aquatic environments, as well as integrated global models for selected radionuclides and special issues in the fields of solid radioactive waste disposal and dose reconstruction. Particular emphasis is placed on the issue of improving confidence in the model results, including the importance of uncertainty analysis and of model verification and validation.     

Evaluation of transport and storage of 60Co, 134Cs, 137Cs and 65Zn by river sediments in the lower Susquehanna River

The Peach Bottom Atomic Power Station (PBAPS) has contributed measurable quantities of radioactivity to Conowingo Reservoir, an impoundment of the lower Susquehanna River. As part of an ongoing radiological assessment program, concentrations of plant-related radionuclides in sediments have been monitored in spring and fall since 1980. Mass balance estimates derived from grab samples of surface sediments (< 10 cm) indicate that less than 20% of reactor released (60)Co, (65)Zn, (134)Cs and (137)Cs is present in these sediments. Significant seasonal variations in radionuclide trapping efficiency by the reservoir are not apparent. Deep core samples (c. 200 cm) confirm that some, but not all, of this surface sediment radionuclide inventory remains within the reservoir-trapped in discrete locations by subsequent sediment accumulation. The remaining radionuclide mass, in dissolved or particle-associated form, appears to be transported downstream, through Conowingo Dam, to upper Chesapeake Bay. The detection of PBAPS-derived radionuclides in the sediments of upper Chesapeake Bay, primarily the Susquehanna Flats, confirms the transport of these radionuclides from the lower Susquehanna River.     

Analysis of water flow paths: methodology and example calculations for a potential geological repository in Sweden

Safety assessment related to the siting of a geological repository for spent nuclear fuel deep in the bedrock requires identification of potential flow paths and the associated travel times for radionuclides originating at repository depth. Using the Laxemar candidate site in Sweden as a case study, this paper describes modeling methodology, data integration, and the resulting water flow models, focusing on the Quaternary deposits and the upper 150 m of the bedrock. Example simulations identify flow paths to groundwater discharge areas and flow paths in the surface system. The majority of the simulated groundwater flow paths end up in the main surface waters and along the coastline, even though the particles used to trace the flow paths are introduced with a uniform spatial distribution at a relatively shallow depth. The calculated groundwater travel time, determining the time available for decay and retention of radionuclides, is on average longer to the coastal bays than to other biosphere objects at the site. Further, it is demonstrated how GIS-based modeling can be used to limit the number of surface flow paths that need to be characterized for safety assessment. Based on the results, the paper discusses an approach for coupling the present models to a model for groundwater flow in the deep bedrock.     

Kinematic analysis of solute mass flows in rock fractures with spatially random parameters

Field data of physical properties in heterogeneous crystalline bedrock, like porosity and fracture aperture, is associated with uncertainty that can have a significant impact on the analysis of solute transport in rock fractures. Solutions to the central temporal moments of the residence time probability density function (PDF) are derived in a closed form for a solute Dirac pulse. The solutions are based on a model that takes into account advection along the fracture plane, diffusion into the rock matrix and sorption kinetics in the rock matrix. The most relevant rock properties including fracture aperture and several matrix properties as well as flow velocity are assumed to be spatially random along transport pathways. The mass transport is first solved in a general form along one-dimensional pathways, but the results can be extended to multi-dimensional flows simply by substituting the expected travel time for inert water parcels. Based on data obtained with rock samples taken at Asp? Hard Rock Laboratory in Sweden, the solutions indicate that the heterogeneity of the rock properties contributes to increasing significantly both the variance and the skewness of the residence time probability density function for a pulse travelling in a fracture. The Asp? data suggests that the bias introduced in the variance of the residence time PDF by neglecting the effect of heterogeneity of the rock properties on the radionuclide migration is very large for fractures thinner than a few tenths of a millimetre.     

Seasonal variation of radionuclides in Fucus vesiculosus L. from the Oresund, Southern Sweden

The activity concentrations of radionuclides (60Co, 54Mn, 137Cs, 40K) in whole plants of Fucus vesiculosus of different ages, and also in tissues of different ages from the same plants were investigated in the vicinity of the Barseb?ck nuclear power plant in southern Sweden. Activity concentration differed between the tissues of different age of the plants, depending on the radionuclide as well as the time of year. The highest concentrations of 60Co and 54Mn were measured in the older parts of the plants in spring and summer, while the activity concentrations of 137Cs and 40K were highest in receptacles and new vegetative fronds. The discharge of radionuclides from the nuclear power plant was reflected in the measured activity concentration in the algae. For 60Co, the response seemed to be smoothed out when considering the whole plant, while the new vegetative tissue better reflected the discharge during the autumn. Thus, it is important to have knowledge about the autecology of the organism when it is used as an indicator for radionuclides.     

Use of X-ray absorption imaging to examine heterogeneous diffusion in fractured crystalline rocks

Heterogeneous diffusion in different regions of a fractured granodiorite from Japan has been observed and measured through the use of X-ray absorption imaging. These regions include gouge-filled fractures, recrystallized fracture-filling material and hydrothermally altered matrix. With the X-ray absorption imaging technique, porosity, relative concentration, and relative mass of an iodine tracer were imaged in two dimensions with a sub-millimeter pixel size. Because portions of the samples analyzed have relatively low porosity values, imaging errors can potentially impact the results. For this reason, efforts were made to better understand and quantify this error. Based on the X-ray data, pore diffusion coefficients (Dp) for the different regions were estimated assuming a single diffusion rate and a lognormal multirate distribution of Dp. Results show Dp for the gouge-filled fractures are over an order of magnitude greater than those of the recrystallized fracture-filling material, which in turn is approximately two times greater than those for the altered matrix. The recrystallized fracture-filling material was found to exhibit the greatest degree of variability. The results of these experiments also provide evidence that diffusion from advective zones in fractures through the gouge-filled fractures and recrystallized fracture-filling material could increase the pore space available for matrix diffusion. This evidence is important for understanding the performance of potential nuclear waste repositories in crystalline rocks as diffusion is thought to be an important retardation mechanism for radionuclides.     

Sources and pathways of artificial radionuclides to soils at a High Arctic site

Activity concentrations, inventories and activity ratios of ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m² for ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The ²³⁸Pu/^239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The ²³⁸Pu/^239?+?240Pu and ^239?+?240Pu/¹³⁷Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.     

Occurrence and sources of selected phenolic endocrine disruptors in Ria de Aveiro,Portugal

Background, aim and scope  

Ria de Aveiro (Portugal) is a shallow coastal lagoon of high economic and ecological importance. Hardly any data on its chemical pollution by polar organic pollutants are available in literature. This study focused on the presence and sources of a series of phenolic endocrine-disrupting compounds (EDCs) in this area, including parabens, alkylphenolic compounds and bisphenol-A (BPA). A number of possible sources of pollution are present in the area, including the large harbours present in the lagoon, the city of Aveiro and the rivers discharging into the area. A recently constructed submarine wastewater outfall, located a few kilometres from the lagoon inlet has also been suggested as a possible source of pollution to Ria de Aveiro in several publications. The aim of the current field study was to investigate the occurrence and main sources of phenolic endocrine disruptors in Ria de Aveiro.     

Radionuclides in some edible and medicinal macrofungal species from Tara Mountain,Serbia

Edible and medicinal macrofungi used in human diet represent not only important sources of nutritive elements but toxic substances as well (heavy metals and radionuclides). Radioactivity levels of four radionuclides (⁴⁰K, ¹³⁷Cs, ²²⁶Ra, ²²⁸Ra) were determined in the basidiomata (fruiting bodies of a Basidiomycetes) of six lignicolous (Fomitopsis pinicola, Ganoderma applanatum, Hericium clathroides, Megacollybia platyphylla, Pluteus cervinus, Trametes gibbosa) and three mycorrhizal (Boletus luridus, Boletus sp. 1, Boletus sp. 2) species as well as their soil (wood) substrates by gamma spectrometry (high-resolution high-purity germanium (HPGe) detector). The aim was to investigate their ability for radionuclide absorption according to transfer factors (from soil and wood), to predict potential bioindicator species as well as species with potential risk for human use. Samples were taken during years 2011 and 2012, at two sites in forest ecosystem of Tara Mountain (Serbia). Observed concentration ranges per dry weight were as follows: 29–3,020 Bq/kg (⁴⁰K), 21.9–735 Bq/kg (¹³⁷Cs), 3–39 Bq/kg (²²⁶Ra), and 2.0–18 Bq/kg (²²⁸Ra). Obtained results indicate that the type of basidiome (fleshy/tough), most likely due to a different metabolic rate, has a very important role in radionuclide accumulation. The highest activity concentrations of all analyzed radionuclides were found in species with fleshy basidiomata—P. cervinus, H. clathroides, M. platyphylla, and Boletus species. A species-specific influence on radionuclide uptake was more prominent comparing to habitat differences and the role of fungal trophic mode. No significant variations were observed regarding radionuclide activity among the same fungal species from different sampling sites.     

Migration of acidic groundwater seepage from uranium-tailings impoundments, 2. Geochemical behavior of radionuclides in groundwater

In this second paper of a series on groundwater seepage from uranium tailings, the general geochemical behavior of radionuclides is described and then applied to data from the field site, Seepage Area A of the Nordic Main impoundment near Elliot Lake, Ontario. The delineation of radionuclide behavior requires (1) the calculation of total element concentration by the summation of concentrations of each element's isotopes (the isotopic concentrations are calculated from the isotopes' radioactivities), (2) the evaluation of solid-liquid interactions using total element concentrations, and (3), for particular isotopes, the evaluation of the extent to which parental geochemical behavior causes a deviation in the isotope's behavior from that of its total element. A computerized speciation program, WATRAD, is used to evaluate aqueous complexation and mineral saturation indices of radium, actinium, thorium, and uranium. Data from Seepage Area A on isotopes of these four elements plus ²¹⁰Pb show that the geochemical behavior of radionuclides can be best defined on an individual isotopic basis rather than on an elemental basis.     

Distribution coefficients (Kd) and desorption rates of 137Cs and 241Am in Black Sea sediments

The distribution coefficients (K_d) and desorption rates of ¹³⁷Cs and ²⁴¹Am radionuclides in bottom sediments at different locations in the Black Sea were studied under laboratory conditions. The K_d values were found to be 500 for ¹³⁷Cs and 3800 for ²⁴¹Am at the steady state and described exponential curves. Rapid uptake of the radionuclides occurred during the initial period and little accumulation happened after four days. The desorption rates for ¹³⁷Cs in different bottom sediments were best described by a three-component exponential model. The desorption half-times of ¹³⁷Cs ranged from 26 to 50 d at the slow components. However, the desorption rate of ²⁴¹Am described one component for all sediment samples and desorption half-time was found to be 75 d. In general, the results showed that the ²⁴¹Am radionuclide is more effectively transferred to bottom sediment and has longer turnover time than ¹³⁷Cs under Black Sea conditions.     

Model of the Long-Term Transport and Accumulation of Radionuclides in Future Landscapes

Assessments of radiological impacts on humans and other biota from potential releases to the biosphere from a deep geologic repository for spent nuclear fuel are associated with several challenges. Releases, if any, will likely occur in a far future and to an environment that will have experienced substantial transformations. Such releases would occur over very long periods during which environmental conditions will vary continuously due to climate change and ecosystem succession. Assessments of radiological impacts must therefore be based on simulations using models that can describe the transport and accumulation of radionuclides for a large variety of environmental conditions. In this paper we describe such a model and show examples of its application in a safety assessment, taking into account results from sensitivity and uncertainty analyses of the model predictions.     

A carbon budget of a small humic lake: an example of the importance of lakes for organic matter cycling in boreal catchments

Lakes play an important role in the cycling of organic matter in the boreal landscape, due to the frequently high extent of bacterial respiration and the efficient burial of organic carbon in sediments. Based on a mass balance approach, we calculated a carbon budget for a small humic Swedish lake in the vicinity of a potential final repository for radioactive waste in Sweden, in order to assess its potential impact on the environmental fate of radionuclides associated with organic matter. We found that the lake is a net heterotrophic ecosystem, subsidized by organic carbon inputs from the catchment and from emergent macrophyte production. The largest sink of organic carbon is respiration by aquatic bacteria and subsequent emission of carbon.dioxide to the atmosphere. Although the annual burial of organic carbon in the sediment is a comparatively small sink, it results in the build-up of the largest carbon pool in the lake. Hence, lakes may simultaneously disperse and accumulate organic-associated radionuclides leaking from a final repository.