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.     

An inventory of long-lived radionuclides residual from underground nuclear testing at the Nevada test site, 1951-1992

An inventory of long-lived radionuclides produced by 828 underground nuclear tests conducted at the Nevada test site (NTS) from 1951 to 1992 includes residual tritium, fission products, actinides, and activation products. Recently, the US Department of Energy approved the declassification of the NTS radionuclide inventory by principal geographic test centers. This permits unclassified publication of radionuclide totals for the Yucca Flat, Pahute Mesa-Area 19, Pahute Mesa-Area 20, Frenchman Flat, and Rainier Mesa/Shoshone Mountain testing locations. Activities are reported as of September 23, 1992, the date of the last underground nuclear test conducted at the NTS, and September 23, 2492, after 500 years of radioactive decay. The availability of these data affords an opportunity for the analysis of the radiologic source term within the boundaries of local hydrogeologic units and provides insight to where radionuclides are sited relative to potential exposure pathways.     

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.     

Review and assessment of models for predicting the migration of radionuclides from catchments

The present paper summarises the results of the review and assessment of models developed for predicting the migration of radionuclides from catchments to water bodies. The models were classified and evaluated according to their main methodological approaches. A retrospective analysis of the principles underpinning the model development in relation to experimental finding and results was carried out. It was demonstrated that most of the various conceptual approaches of different modellers can be integrated in a general, harmonised perspective supported by a variety of experimental evidences. Shortcomings and advantages of the models were discussed.     

A general methodology for structuring models to predict the long-term migration of radionuclides from catchments

In the present paper a generic model for predicting the long-term migration of radionuclides and heavy metals from catchments is described. The model subdivides the catchment into a number of homogeneous, infinitesimal sub-catchments and integrates the radionuclide contributions from such sub-catchments to calculate the total flux of contaminant. It relates the radionuclide behaviour to the statistical distribution of the pollutant partition coefficient on the "ensemble" of sub-catchments. The methodology was validated for 90Sr and 137Cs by using data for water contamination in some European rivers. Values of migration parameters for Pu, Tc, I and Cd isotopes were obtained.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides (⁹⁰Sr, ¹³⁷Cs and ^239+240Pu) in seabed sediment in the Japan Sea were collected during the period 1998–2002. Concentration of ⁹⁰Sr, ¹³⁷Cs and ^239+240Pu in seabed sediment was 0.07–1.6 Bq kg⁻¹, 0.4–9.1 Bq kg⁻¹ and 0.002–1.9 Bq kg⁻¹, respectively. In the northern basin of the sea (Japan Basin), ^239+240Pu/¹³⁷Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher ^239+240Pu/¹³⁷Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38°N), both inventories and ^239+240Pu/¹³⁷Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

Anthropogenic radionuclides in sediment in the Japan Sea: distribution and transport processes of particulate radionuclides

Distributions of anthropogenic radionuclides ((90)Sr, (137)Cs and (239+240)Pu) in seabed sediment in the Japan Sea were collected during the period 1998-2002. Concentration of (90)Sr, (137)Cs and (239+240)Pu in seabed sediment was 0.07-1.6 Bq kg(-1), 0.4-9.1 Bq kg(-1) and 0.002-1.9 Bq kg(-1), respectively. In the northern basin of the sea (Japan Basin), (239+240)Pu/(137)Cs ratios in seabed sediment were higher and their variation was smaller compared to that in the southeastern regions of the sea. The higher (239+240)Pu/(137)Cs ratios throughout the Japan Basin were considered to reflect production of Pu-enriched particles in the surface layer and substantial sinking of particulate materials in this region. In the southern regions of the Japan Sea (<38 degrees N), both inventories and (239+240)Pu/(137)Cs ratios in sediment were larger than those in the other regions. In the southern Japan Sea, observations suggested that supply of particulate radionuclides by the Tsushima Warm Current mainly enhanced accumulation of the radionuclides in this region.     

The influence of the development of temperate fruit tree species on the potential for their uptake of radionuclides

This paper reviews the published literature that describes the phenological development of above and below ground organs of temperate fruit trees (top fruit), particularly with respect to apple (Malus domestica). Critical information is presented which is considered appropriate in developing an understanding of the potential for top fruit species to take up radionuclide contaminants from the atmosphere and the soil. Information is cited on how climatic and edaphic factors influence the growth and development of temperate fruit trees, the phenological production of their leaf area and the development and growth of their fruit and hence the potential for foliar and fruit uptake of radionuclides from the atmosphere. The study also reports on the importance of the distribution and phenological development of roots in the soil and the potential for their uptake of radionuclides from the soil. The effects of above and below ground management procedures, within temperate fruit orchards, on potential radionuclide uptake are also considered. It is concluded that the potential for the uptake of radionuclides by temperate fruit tree species will depend on a number of phenological and physiological factors. For uptake from the soil these factors include; root distribution and density in the soil profile, seasonal changes in the production and distribution of roots, and the presence and amount of water in the soil. These factors are themselves influenced by rootstock type and its growth vigour, scion type and its growth vigour, tree age, spacing of trees in the orchard, orchard management practices (presence or absence of weeds or grass under the trees) and soil type and depth. Direct uptake by the shoot, however, will be influenced by the climatic conditions at the time of exposure and the presence of foliage. Deposition and uptake are likely to change with leaf area development and the ability of radionuclides to penetrate the cuticle of the leaf changes with seasonal development. Transport of radionuclides to the fruit may also depend on the time of season, as the importance of the xylem and phloem transport routes can change with the growth and development of the fruit.     

Occurrence and behaviour of radionuclides in the Moselle River—Part III: Dispersion of radionuclides along the river course

Knowledge about propagation of radionuclides from nuclear power plants (NPPs) along the course of a river is of great interest in radioecological assessments. By use of a model previously applied in the cases of the Rhine and Weser Rivers, the distribution of various radionuclides released into the Moselle from the NPP Cattenom at normal operation is described with ⁵⁸Co, ⁶⁰Co and ^110mAg as tracers. A comparison of field measurements with calculated values revealed that the radionuclide concentrations in suspended matter and nuclide loads calculated from emission rates agreed with the measured data by a factor of less than two on average.Radionuclide concentrations and loads along the river course decrease mainly due to deposition of particulate radioactive matter in high-sedimentation areas and due to dilution with uncontaminated material from tributaries and other sources. The rate constants of both processes were evaluated, and the mean range of suspended radioactive particles in the Moselle was estimated. Moreover, this study showed anew that suspended matter has to be considered as the main carrier by which the radionuclides from NPPs may be transported over long distances.     

Natural radionuclides as tracers of the dispersal of dredge spoil dumped at sea.

Monitoring large (underwater) surfaces, with rapidly varying composition, requires a sampling density which exceeds the capabilities of standard techniques. These techniques involve sample collection and a number of treatments and measurements in the laboratory; both steps are laborious, tedious and costly. This paper presents an in situ method in which a detector system is trailed over the surface and measures continuously the gamma rays emitted by the natural radionuclides in the sediment. Since each sediment component has its own characteristic set of activity-concentration values (radiometric fingerprint), the composition of the sediment can be deduced quantitatively. This paper shows the application of this technique for monitoring the dispersal of dredge spoil from Rotterdam harbour, dumped in the North Sea. In addition to a qualitative picture of dredge spoil dispersal, a mass balance equation has been used to quantitatively assess the dredge spoil transport with time.     

Occurrence and behaviour of radionuclides in the Moselle River—Part I: Entry of natural and artificial radionuclides

Various sources contribute to the radioactive contamination of the Moselle River, among which the French NPP Cattenom with four units of 1300 M We represents the most important. Appropriate operational precautions were taken in order to monitor the nuclide transfer on different pathways under normal and accidental conditions and the effectiveness of these measures has been tested using natural (²¹⁴Pb/²¹⁴Bi, ⁷Be, ⁴⁰K) and artificial radionuclides. (³H, ⁵⁸Co, ⁶⁰Co, ¹³¹I, ¹³⁷Cs) as tracers. Measurements of suspended matter have revealed that the inputs of natural nuclides exceed the discharges of the NPP Cattenom. In 1992 the annual loads of ⁷Be and ⁴⁰K in suspended matter at Palzem amounted to 21 and 130 GBq year⁻¹, whereas the emission rates of ⁶⁰Co and ¹³⁷Cs were about 2.6 and 1.0 GBq year⁻¹. The total nuclide load of ¹³⁷Cs at Palzem reached 6.2 GBq year⁻¹, which is about six times the quantity emitted by the NPP Cattenom in the same year. This excess is due to the accident at Chernobyl and to a lesser extent to prior atmospheric weapons tests.     

Bioavailability of sediment-associated and low-molecular-mass species of radionuclides/trace metals to the mussel Mytilus edulis

Sediments can act as a sink for contaminants in effluents from industrial and nuclear installations or when released from dumped waste. However, contaminated sediments may also act as a potential source of radionuclides and trace metals to the water phase due to remobilisation of metals as dissolved species and resuspension of particles. The marine mussel Mytilus edulis is a filter-feeding organism that via the gills is subjected to contaminants in dissolved form and from contaminants associated to suspended particles via the digestive system. In this paper the bioavailability of sediment-associated and seawater diluted Cs, Co, Cd and Zn radioactive tracers to the filtering bivalve M. edulis has been examined. The mussels were exposed to tracers diluted in ultrafiltered (<10 kDa) seawater (Low Molecular Mass form) or to tracers associated with sediment particles from the Stepovogo Fjord at Novaya Zemlya in short-term uptake experiments, followed by 1-month depuration experiments in flow-through tanks. A toxicokinetic model was fitted to the uptake and depuration data, and the obtained parameters were used to simulate the significance of the two uptake pathways at different suspended sediment loads and sediment-seawater distribution coefficients. The results of the model simulations, assuming steady state conditions, suggest that resuspended particles from contaminated sediments can be a highly significant pathway for mussels in the order ¹⁰⁹Cd ≌ ⁶⁵Zn < ¹³⁴Cs < ⁶⁰Co. The significance increases with higher suspended sediment load and with higher K_d. Furthermore, the experimental depuration data suggest that Cs is retained longer and Co, Cd and Zn shorter by the mussels when associated with ingested sediments, than if the metals are taken up from the low molecular mass (LMM) phase.     

Sources of anthropogenic radionuclides in the environment: a review

Studies of radionuclides in the environment have entered a new era with the renaissance of nuclear energy and associated fuel reprocessing, geological disposal of high-level nuclear wastes, and concerns about national security with respect to nuclear non-proliferation. This work presents an overview on sources of anthropogenic radionuclides in the environment, as well as a brief discussion of salient geochemical behavior of important radionuclides. We first discuss the following major anthropogenic sources and current developments that have lead, or could potentially contribute, to the radionuclide contamination of the environment: (1) nuclear weapons program; (2) nuclear weapons testing; (3) nuclear power plants; (4) uranium mining and milling; (5) commercial fuel reprocessing; (6) geological repository of high-level nuclear wastes that include radionuclides might be released in the future, and (7) nuclear accidents. Then, we briefly summarize the inventory of radionuclides ⁹⁹Tc and ¹²⁹I, as well as geochemical behavior for radionuclides ⁹⁹Tc, ¹²⁹I, and ²³⁷Np, because of their complex geochemical behavior, long half-lives, and presumably high mobility in the environment; biogeochemical cycling and environment risk assessment must take into account speciation of these redox-sensitive radionuclides.     

Occurrence and behaviour of radionuclides in the Moselle River-Part II: Distribution of radionuclides between aqueous phase and suspended matter

Most of the radionuclides released from nuclear power plants ( NPPs) into rivers are primarily adsorbed onto suspended matter. To describe this nuclide transfer, a model was used which takes the total suspended matter load as solid phase into account. The necessary partition factors of various radionuclides were determined in river water/suspended matter of the Moselle in laboratory investigations. By use of this model, a conservative estimate of the radionuclide concentration of the solid phase could be obtained which proved to be more realistic than the results based on the distribution law.Furthermore, the influence of grain-size on the specific activity of single fractions of a Moselle sediment was demonstrated using ¹³⁷Cs, ¹⁰⁶Ru and ¹⁴⁴Ce from the Chernobyl nuclear accident as tracers. The grain-size pattern is considered to be a main factor which may seriously distort the determination of distribution coefficients and concentration factors that are needed in applying the model based on the distribution law.     

Modelling the reworking effects of bioturbation on the incorporation of radionuclides into the sediment column: implications for the fate of particle-reactive radionuclides in Irish Sea sediments

A microcosm laboratory experiment was conducted to determine the impact of biological reworking by the ragworm Nereis diversicolor on the redistribution of particle-bound radionuclides deposited at the sediment-water interface. Over the course of the 40-day experiment, as much as 35% of a ¹³⁷Cs-labelled particulate tracer deposited on the sediment surface was redistributed to depths of up to 11 cm by the polychaete. Three different reworking models were employed to model the profiles and quantify the biodiffusion and biotransport coefficients: a gallery-diffuser model, a continuous sub-surface egestion model and a biodiffusion model. Although the biodiffusion coefficients obtained for each model were quite similar, the continuous sub-surface egestion model provided the best fit to the data. The average biodiffusion coefficient, at 1.8 ± 0.9 cm² y⁻¹, is in good agreement with the values quoted by other workers on the bioturbation effects of this polychaete species. The corresponding value for the biotransport coefficient was found to be 0.9 ± 0.4 cm y⁻¹. The effects of non-local mixing were incorporated in a model to describe the temporal evolution of measured ⁹⁹Tc and ⁶⁰Co radionuclide sediment profiles in the eastern Irish Sea, influenced by radioactive waste discharged from the Sellafield reprocessing plant. Reworking conditions in the sediment column were simulated by considering an upper mixed layer, an exponentially decreasing diffusion coefficient, and appropriate biotransport coefficients to account for non-local mixing. The diffusion coefficients calculated from the ⁹⁹Tc and ⁶⁰Co cores were in the range 2-14 cm² y⁻¹, which are consistent with the values found by other workers in the same marine area, while the biotransport coefficients were similar to those obtained for a variety of macrobenthic organisms in controlled laboratories and field studies.     

Development of a Test System for Assessing the Toxicity of Multicomponent Wastes Stored in the Natural Environment

A biological test system is proposed for assessing the toxicity of multicomponent wastes stored in the natural environment, with sewage sludge being used as an example. The principles of creating a test system and ranking the samples of multicomponent masses with respect to environmental hazard are discussed.     

Impact of global warming on European tidal estuaries: some evidence of northward migration of estuarine fish species

The aim of this study was to determine whether the latitudinal distribution of fish species that use estuaries to complete their entire life cycle has shifted northward as an expected consequence of global warming. The mean latitude of past fish species distributions found in 1970s’ literature was compared with the mean latitude of distributions today based on fish density indices collected in 55 tidal estuaries along the Atlantic European seaboard, from Portugal to Scotland. Among the 15 most common species, 11 displayed a positive difference between current and past mean latitudes suggesting a northward shift of the populations. Using the occurrence of subtropical species in temperate areas as an indicator of water warming, the northernmost range limit of 10 subtropical species was subsequently focused on. Six of them were recorded up to their past northern latitudinal limit. These results reinforced the idea that a number of fish species associated to estuaries have migrated northwards over the last 30 years, possibly due to water warming. These ecological changes can get important managerial implications, i.e. in the assessment of the ecological status in European directives.     

Watershed wash-off of atmospherically deposited radionuclides: review of the fluxes and their evolution with time

Radionuclide transport with water from contaminated watersheds is an intermittent flux--also called watershed wash-off--which causes radionuclide redistribution in terrestrial ecosystems, and more critically radionuclide delivery to downstream waterbodies. Mean wash-off fluxes and their evolution with time have been generally quantified with transfer functions, which can be seen as transfer factors varying with time. But unfortunately the published quantifications rely on many analytical formulations for the transfer function. This paper aims at unifying the heterogeneous information concerning radionuclide wash-off. A generic transfer function model was proposed. Published wash-off quantifications were gathered in a database and converted within this new framework. This extensive review covered various radionuclides, source terms, processes, time and space scales reported in the literature since 1960. It demonstrated the feasibility of a generic wash-off model. Intervals of variations for the introduced coefficients were summarised and the influence of wash-off conditions were discussed. In some cases, the influence of wash-off conditions should be clarified to propose narrower parameter intervals for practical assessments.