Assessing field-scale migration of radionuclides at the Nevada Test Site: "mobile" species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides ((3)H, (14)C, (36)Cl, (99)Tc and (129)I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and (36)Cl showed little evidence of retardation, while the transport of (14)C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially (99)Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of (129)I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some "mobile" radionuclides (especially (99)Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Review and assessment of models for predicting the migration of radionuclides through rivers

The present paper summarises the results of the review and assessment of state-of-the-art models developed for predicting the migration of radionuclides through rivers. The different approaches of the models to predict the behaviour of radionuclides in lotic ecosystems are presented and compared. The models were classified and evaluated according to their main methodological approaches. The results of an exercise of model application to specific contamination scenarios aimed at assessing and comparing the model performances were described. A critical evaluation and analysis of the uncertainty of the models was carried out. The main factors influencing the inherent uncertainty of the models, such as the incompleteness of the actual knowledge and the intrinsic environmental and biological variability of the processes controlling the behaviour of radionuclides in rivers, are analysed.     

Radiological risk assessment and biosphere modelling for radioactive waste disposal in Switzerland

Long-term safety assessments for geological disposal of radioactive waste in Switzerland involve the demonstration that the annual radiation dose to humans due to the potential release of radionuclides from the waste repository into the biosphere will not exceed the regulatory limit of 0.1 mSv. Here, we describe the simple but robust approach used by Nagra (Swiss National Cooperative for the Disposal of Radioactive Waste) to quantify the dose to humans as a result to time-dependent release of radionuclides from the geosphere into the biosphere. The model calculates the concentrations of radionuclides in different terrestrial and aquatic compartments of the surface environment. The fluxes of water and solids within the environment are the drivers for the exchange of radionuclides between these compartments. The calculated radionuclide concentrations in the biosphere are then used to estimate the radiation doses to humans due to various exposure paths (e.g. ingestion of radionuclides via drinking water and food, inhalation of radionuclides, external irradiation from radionuclides in soils). In this paper we also discuss recent new achievements and planned future work.     

Distribution of fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) in soils of Taiwan

Depth profiles and cumulative deposition of four fallout radionuclides (7Be, 137Cs, 210Pb and 239,240Pu) were determined in presumably undisturbed soils in Taiwan. Inventories of these radionuclides in different areas correlate significantly with each other (except 7Be) and with mean annual rainfall, providing a necessary condition for the development of soil erosion studies in Taiwan. However, the data show very large spatial variability between and within landscape units, reflecting the steep topographic and meteorological gradients in the island. Thus, the application of fallout radionuclides to study soil conservation in Taiwan is expected to be a demanding task; it will call for dense sampling even at undisturbed reference sites.     

Variability in background levels of surface soil radionuclides in the vicinity of the US DOE waste isolation pilot plant

Concentrations of radionuclides were measured in soils from a grid of locations surrounding the US Department of Energy Waste Isolation Pilot Plant (WIPP) in southeastern New Mexico and from a grid on a reference site approximately 20 km southeast of the WIPP site. Each of the two grids has 16 sampling locations (grid nodes) systematically distributed within an area of 16.580 ha. Sampling was conducted prior to the arrival of the first waste shipment at WIPP. Thus, the 137Cs and 23,240Pu in the soil are expected to have been deposited as global fallout, although the Gnome Site, 8.8 km southwest of the WIPP, is also a potential source of 239,240Pu and fission products. The reference grid has significantly higher concentrations of fallout and natural radionuclides than the WIPP grid. Up to 80% of the total variability in radionuclide concentrations across the two grids is attributable to differences between grid nodes. Differences between replicates within a location account for 44-50% of the variability in concentrations of the uranium isotopes, but only 11-17% of the variability in the concentrations of the other radionuclides. Samples having similar abundance of radionuclides were spatially aggregated across the terrain. The activity concentrations of the radionuclides were strongly correlated with the concentrations of Al and Pb, and with the percentages of sand, silt and clay in the soil. Normalizing radionuclide concentrations to the concentration of Al or percent fine particles can help adjust for differences in soil textures among samples and facilitate the detection of gradients or temporal changes in soil concentrations.     

Assessing field-scale migration of radionuclides at the Nevada Test Site: “mobile” species

Many long-lived radionuclides are present in groundwater at the Nevada Test Site (NTS) as a result of 828 underground nuclear weapons tests conducted between 1951 and 1992. In conjunction with a comprehensive geochemical review of radionuclides (³H, ¹⁴C, ³⁶Cl, ⁹⁹Tc and ¹²⁹I) that are presumably mobile in the subsurface, we synthesized a body of radionuclide activity data measured from groundwater samples collected at 18 monitoring wells, to qualitatively assess their migration at the NTS over distances of hundreds of meters and over timescales of decades. Tritium and ³⁶Cl showed little evidence of retardation, while the transport of ¹⁴C may have been retarded by its isotopic exchange with carbonate minerals in the aquifer. Observed local reducing conditions (either natural or test-induced) will impact the mobility of certain redox-sensitive radionuclides (especially ⁹⁹Tc) that were otherwise soluble and readily transported under oxidizing conditions. Conversely, strongly oxidizing conditions may impact the mobility of ¹²⁹I which is mobile under reducing conditions. The effect of iodine speciation on its transport deserves further attention. Indication of delayed transport of some “mobile” radionuclides (especially ⁹⁹Tc) in the groundwater at the NTS suggested the importance of redox conditions of the natural system in controlling the fate and transport of radionuclides, which has implications in the enhanced performance of the potential Yucca Mountain repository, located adjacent to the NTS, to store high-level nuclear wastes as well as management of radionuclide contamination in legacy nuclear operations facilities.     

Radionuclide fluxes at a plant manufacturing dicalcium phosphate for domestic animals

We have studied a phosphate rock plant which produces dicalcium phosphate (DCP), used as a source of calcium and phosphorus for domestic animals. A by-product in the manufacturing process is calcium chloride which is used in the oil industry, the food industry and as road-salt. The objectives of our study were to describe the fluxes of radionuclides from the 238U decay series and to estimate the radiation doses to workers at the plant. The radionuclides in the phosphate rock were found to be in secular radioactive equilibrium with 238U, with an average activity concentration of 837 Bq kg-1. Separation and concentration processes were observed at different stages in the plant. Most of the 226Ra was found in the calcium chloride, while the major part of the 238U, about 950 Bq kg-1, was found in the dicalcium phosphate. The annual occupational effective dose to the workers was found to be below the 1 mSv limit recommended by ICRP (1991a) for the public. This study has shown a good example of an important non-nuclear industry with a high input of natural radionuclides with several conceivable pathways to man.     

Problems of sustainable development and ecological indication in radioactively contaminated areas

Lands that have become unusable because of contamination with long-lived artificial radionuclides require special measures aimed at their monitoring and rehabilitation. In such areas, specific processes in the biota are associated with the direct effect of ionizing radiation on some species, secondary changes depending on the ecology of organisms trophically connected with these species, and side effects explained by the regime of isolation established in radiation reserves. The dynamics of floras and faunas in radiation reserves are determined by successional changes in plant communities, migration of radionuclides, and the protective status of these territories.     

Simulating transport of non-Chernobyl (137)Cs and (90)Sr in the North Atlantic-Arctic region

The spatial and temporal distributions of the anthropogenic radionuclides (137)Cs and (90)Sr, originating from nuclear bomb testing and the Sellafield reprocessing plants in the Irish Sea, are simulated using a global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysed fields for the period 1950 to present. Comparison of temporal evolution of observed and simulated concentrations of (137)Cs have been conducted for the regions east of Scotland, west of central Norway and at the entrance of the Barents Sea. It follows that the radionuclides from the Sellafield discharge reach the Barents Sea region after 4-5 years, in accordance with observations. The simulation provides a detailed distribution and evolution of the radionuclides over the integration time. For the Atlantic waters off the coast of Norway and in the southern Barents Sea, the atmospheric fallout dominates over the Sellafield release up to the mid 1960s and from the early 1990s, whereas Sellafield is the main source for the two radionuclides in the 1970s and 1980s. It is furthermore argued that model systems like the one presented here can be used for future prediction of radioactive contaminations in the Nordic Seas and the Arctic Ocean, for instance under various global warming scenarios.     

Chemical associations of artificial radionuclides in Cumbrian soils

The distributions of radionuclides in the surface layer of four soils of contrasting types from west Cumbria, UK, have been studied in detail. All the soils contain enhanced levels of artificial radionuclides derived from low-level discharges both to sea and to atmosphere from the British Nuclear Fuels reprocessing plant at Sellafield. The bulk of the activity is held in the top 15 cm of soil profiles, suggesting that radionuclide mobility is limited. Sequential extraction experiments have identified major associations of plutonium with organic matter and of caesium with silicates but there is no preferential association of ruthenium with any single soil component.     

Radioactivity from coal-fired power plants: A review

The radioactivity contents of coal and of the different types of ash formed during its combustion are reviewed. Also, the radiological impact of coal-fired plants and the plant features causing this impact are discussed. The depletion or enrichment of radionuclides in the different types of ash is interpreted in terms of the combustion temperature, the size of ash particles and the chemical forms of the radionuclides. The volatilization-condensation process as the postulated mechanism of radionuclide enrichment is also discussed.Past studies of the release of radionuclides from coal-fired plants are compared and the environmental pathways of the radionuclides are highlighted. Individual and collective radiation doses calculated for various coal-fired plants are evaluated and the importance of the different pathways to man is outlined.     

Fractionation of natural radionuclides in soils from a uranium mineralized area in the south-west of Spain

A new version of a classical method was applied to study the distribution of natural radionuclides (238U, 230Th, and 226Ra) in the soil fractions obtained by a sequential extraction procedure. The potential significance of the fractions obtained with this method was tested on two very similar soils but with very different contents of the three radionuclides, collected in the proximity of a disused uranium mine located in the Extremadura region in the south-west of Spain. The results confirmed that, if only non-residual fractions are considered, the sequential method applied shows a characteristic speciation pattern of these natural radionuclides in this soil matrix, i.e., the distribution of each of the three radionuclides was very similar for the two soil samples.     

Kinetics of the adsorption and desorption of radionuclides of Co, Mn, Cs, Fe, Ag and Cd in freshwater systems: experimental and modelling approaches

The sorption and release kinetics of 54Mn, 58Co, 59Fe, 109Cd, 110mAg and 134Cs by freshwater suspended particles were investigated to better identify the biogeochemical processes involved and to obtain suitable data for improving models describing radionuclide migration in freshwater streams. In order to observe any seasonal variability in the interaction of radionuclides with natural particles, experiments were performed both in winter and in summer during a phytoplanktonic bloom. Two kinetic models are compared in this paper: the "one-step reversible" model, based on the hypothesis that the transfer of radionuclides between water and suspended solids is governed by a reversible reaction, and the "two-successive-step reversible" model, which assumes two distinct types of sites or reactions on the solid phase. The "one-step reversible" model is generally unable to describe properly the exchange kinetics; this result shows that at least two processes are generally involved in radionuclide exchange between water and suspended particles. On the contrary, a model involving the existence of two successive reversible reactions properly simultes both the sorption and release kinetics. The determination of the kinetic coefficients allows quantitative assessment of the relative importance and kinetics of the processes. In particular, it has been shown that, except for Cs and Cd, major fractions of the radionuclides are associated at equilibrium with particulate sites involving strong interactions. The kinetics to reach this equilibrium depend on seasonal conditions, especially for Co and Mn: the transfer of Co and Mn to particulate sites involving strong interactions is much slower in winter. The distribution of the radionuclides between water and particulate sites involving weak interactions also shows seasonal variations for Co, Mn, Fe and Ag: the capacity to associate radionuclides is much higher in summer for Co and Mn, while the inverse tendency is observed for Fe and Ag. For Cs and Cd, no significant seasonal differences were observed.     

Intra-cultivar variability of the soil-to-grain transfer of fallout 137Cs and 90Sr for winter wheat

Differences between the root uptake of fallout radionuclides by different cultivars ('inter-cultivar' variability) growing on the same field may be influenced not only by genetic differences of the cultivars, but also by the spatial variability of the soil-to-grain transfer within the cultivation area of each cultivar. This 'intra-cultivar' variability was investigated in 2001 and 2002 for 137Cs and 90Sr using three winter wheat cultivars with four replicates for each cultivar at three different sites in Bavaria, Germany. The intra-cultivar variability proved to be in the same range as the inter-cultivar variability which was determined earlier at the same sites for both radionuclides. An ANOVA of the 137Cs data set revealed that the variability of the 137Cs soil-to-grain transfer was caused by the soil and climate (year) at the field sites and the interaction of cultivar and field. A significant contribution of the factor 'cultivar' alone to the variability could not be detected. This may be due to the complex environmental conditions to which plants are exposed in field experiments. To find wheat cultivars with minimal uptake of fallout radionuclides it may be better to examine the molecular mechanisms of their root uptake in order to identify targets for breeding "safer" plants.     

Vertical profiles and enrichment pattern of natural radionuclides in monazite areas of coastal Kerala

Detailed studies on radionuclides concentration in different environmental matrices of high background areas were undertaken in the coastal areas of Karunagapalli, Chavara, Neendakara and Kollam to study the distribution and enrichment of the radionuclides in the region. The sand samples collected at different distances from sea waterline and at different depths, were analysed for primordial radionuclides by gamma spectrometry. The activity of primordial radionuclides was determined for the different size fractions of sand to study the enrichment pattern. The highest activity was found confined in 125-63 microm particle size fraction in sand. The minimum (232)Th activity was 9.4 Bq kg(-1), found in Kollam at a depth of 10-20 cm, 40 m away from waterline in 500-250 microm particle size fraction and maximum activity of 136,811.2 Bq kg(-1) was observed in Chavara in grains of size 125-63 microm at a depth of 0-10 cm for a sample collected 20 m away from waterline. The lowest (226)Ra activity observed was 29.6 Bq kg(-1) at Kollam beach for a sample 40 m away from waterline in grains of size 1000-500 microm and at a depth of 20-30 cm and the highest activity observed was 10,309 Bq kg(-1) in grains of size 125-63 microm for a sample collected at a distance 20 m away from waterline and at a depth of 0-10 cm. The activity of (40)K was below detectable level in most of the samples collected from the high background monazite area. The (232)Th, (226)Ra activities decrease with depth for the samples collected 20 m away from the waterline and increase with depth for the samples collected 40 m away from the waterline at Chavara and Kollam beaches. No definite correlation was found between variation of the concentrations of (232)Th and (226)Ra with depth at Karunagapalli and Neendakara beach sands. There exists a strong correlation between (226)Ra and (232)Th activities in the region. The results of these investigations are presented and discussed in this paper.     

Transfer of radioactivity to fruit: significant radionuclides and speciation

One of the roles of the BIOMASS Theme 3 Fruit Working Group was to identify significant radionuclides to support its work programme. This paper provides a short review of radionuclide emissions to atmosphere together with comments on their relative dosimetric impacts to identify those radionuclides most relevant to the Fruit Working Group. Speciation of the identified radionuclides is also discussed to identify the most likely chemical forms to which fruits might be exposed. It is noted that no information currently exists on radionuclide speciation in regard to the uptake and retention of radionuclides in fruit crops.     

Assessment of the radiological impacts of historical coal mining operations on the environment of Ny-Alesund, Svalbard

Mineral extraction activities, such as those conducted by oil, gas and coal industries, are widespread throughout the Arctic region. Waste products of these activities can result in significant contributions to the radioactive burden of the surrounding environment due to increased concentrations of naturally occurring radioactive materials (NORM) to levels that would not normally be found in the environment. Coal mining operations commenced in the early 1900s on Svalbard and have been conducted at a variety of locations on the archipelago since then. Coal contains radionuclides of the uranium and thorium series as well as 40K. Extraction and processing of coal can result in releases of these radionuclides to the broader environment with subsequent impact on the human and non-human inhabitants of the area. This paper presents the results of a study on environmental radioactivity resulting from historical coal mining operations conducted at Ny-Alesund, Spitsbergen, in the Svalbard archipelago. Activity concentrations of radionuclides found in materials associated with these operations are presented as well as the results of a spatial dosimetric survey conducted over an area affected by coal mining.     

Nuclide migration and the environmental radiochemistry of Florida phosphogypsum

Phosphogypsum, a waste by-product derived from the wet process production of phosphoric acid, represents one of the most serious problems facing the phosphate industry in Florida today. This by-product gypsum precipitates during the reaction of sulfuric acid with phosphate rock and is stored at a rate of about 40 million tons per year on several stacks in central and northern Florida. The main problem associated with this material concerns the relatively high levels of natural uranium-series radionuclides and other impurities which could have an impact on the environment and prevent its commercial use. We have studied the potential release of radionuclides from phosphogypsum by: (i) analysis of stack fluids, groundwaters, and soils associated with gypsum stacks; and (ii) geochemical modeling. Stack fluids were observed to be very high in dissolved uranium and 210Pb with only moderate concentrations of 226Ra. Underlying soils tend to be enriched in U and 210Pb indicating precipitation when acidic stack fluids enter a buffered environment. Modeling results showed significant increases in radionuclide complexes with sulfate and phosphate, resulting in relatively mobile uncharged or negatively charged solution species within the stacks with likely precipitation of multicomponent solids with increasing pH below the stack. Our evidence thus suggests that, while phosphogypsum stacks do contain significant quantities of dissolved radionuclides, removal mechanisms appear to prevent large-scale migration of radionuclides to the underlying aquifer.     

Distribution of 90Sr and 137Cs in Arctic soil profiles polluted by heavy metals

Effects of industrial pollution on the behaviour of radionuclides in spruce forest ecosystems were studied along a gradient from of a copper-nickel smelter in Monchegorsk, NW Russia. A reference site was situated in Lapland, Finland, 152 km west of Monchegorsk. Most of the total 137Cs activity in soil was in mineral (E and B) horizons, except at the reference site where the major part was still in the organic surface layer. Most of the total 90Sr activity still remaining in the soil profile was found in the surface layer, but the relative amount decreased with increasing level of industrial pollution. Pollutants from the smelter clearly affected the chemical speciation of radionuclides. Smaller amounts of exchangeable radionuclides were present in the organic surface layer at the most polluted sites. The decline of 137Cs with decreasing distance from the smelter correlated strongly with a similar depletion in exchangeable K and Mg. Total concentrations of 137Cs and 90Sr showed high correlations with exchangeable cations, particularly in the E and upper B horizon. A sudden change in behaviour of 137Cs in the lower B horizon may be associated with changes in clay mineralogy along the soil profile caused by weathering.