Sources and pathways of Sr in the North Atlantic–Arctic region: present day and global warming

The spatial and temporal distributions of the anthropogenic radionuclides ¹³⁷Cs and ⁹⁰Sr, originating from nuclear bomb testing, the Sellafield reprocessing plant in the Irish Sea (UK), and from the Ob and Yenisey river discharges to the Arctic Ocean, have been simulated using the global version of the Miami Isopycnic Coordinate Ocean Model (MICOM). The physical model is forced with daily atmospheric re-analysis fields for the period of 1948–1999. Comparison of the temporal evolution of the observed and the simulated concentrations of ⁹⁰Sr has been performed in the Kara Sea. The relative contributions of the different sources on the temporal and spatial distributions of the surface ⁹⁰Sr are quantified over the simulated period. It follows that the Ob river discharge dominated the surface ⁹⁰Sr over most of the Arctic Ocean and along the eastern and western coasts of Greenland before 1960. During the period of 1980–1990, the atmospheric fallout and the Ob river discharge were equally important for the ⁹⁰Sr distribution in the Arctic Ocean. Furthermore, an attempt has been made to explore the possible dispersion of accidental released ⁹⁰Sr from the Ob and Yenisey rivers under a global warming scenario (2 × CO₂). The difference between the present-day and the global warming scenario runs indicates that more of the released ⁹⁰Sr from the Ob and Yenisey rivers is confined to the Arctic Ocean in the global warming run, particularly in the near coastal, non-European part of the Arctic Ocean.     

Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

Numerical simulation of 137Cs and (239,240)Pu concentrations by an ocean general circulation model

We simulated the spatial distributions and the temporal variations of 137Cs and (239,240)Pu concentrations in the ocean by using the ocean general circulation model which was developed by National Center of Atmospheric Research. These nuclides are introduced into seawaters from global fallout due to atmospheric nuclear weapons tests. The distribution of radioactive deposition on the world ocean is estimated from global precipitation data and observed values of annual deposition of radionuclides at the Meteorological Research Institute in Japan and several observed points in New Zealand. Radionuclides from global fallout have been transported by advection, diffusion and scavenging, and this concentration reduces by radioactive decay in the ocean. We verified the results of the model calculations by comparing simulated values of 137Cs and (239,240)Pu in seawater with the observed values included in the Historical Artificial Radionuclides in the HAM database, which has been constructed by the Meteorological Research Institute. The vertical distributions of the calculated 137Cs concentrations were in good agreement and are in good agreement with the observed profiles in the 1960s up to 250 m, in the 1970s up to 500 m, in the 1980s up to 750 m and in the 1990s up to 750 m. However, the calculated 137Cs concentrations were underestimated compared with the observed 137Cs at the deeper layer. This may suggest other transport processes of 137Cs to deep waters. The horizontal distributions of 137Cs concentrations in surface water could be simulated. A numerical tracer release experiment was performed to explain the horizontal distribution pattern. A maximum (239,240)Pu concentration layer occurs at an intermediate depth for both observed and calculated values, which is formed by particle scavenging. The horizontal distributions of the calculated (239,240)Pu concentrations in surface water could be simulated by considering the scavenging effect.     

MEAD (part II)-Predictions of radioactivity concentrations in the Irish Sea

The predictions from MEAD, a model that simulates the transport of radionuclides in the marine environment, are presented for the Irish Sea. MEAD predictions for (137)Cs and Pu(alpha) are presented following discharges from BNFL Sellafield and the predictions compared to measured data from near the discharge location and further a field in the Irish Sea. The model performs well in most circumstances given the uncertainties involved in both modelling and data collection although some inconsistencies in the predictions are found. MEAD is also compared to other models of radionuclide transport in the Irish Sea.     

Anthropogenic radionuclides in the Japan Sea: their distributions and transport processes

The anthropogenic radionuclides, (90)Sr, (137)Cs and (239+240)Pu, were measured in the water column of the Japan Sea/East Sea during 1997-2000. The vertical profiles of radionuclide concentrations showed: exponential decrease with depth for (90)Sr and (137)Cs, and surface minimum/subsurface maximum for (239+240)Pu. These results do not differ substantially from results reported previously. The area-averaged concentrations of radionuclides in the Japan Sea are higher than those found in the Northwest Pacific Ocean below surface layer showing the accumulation of the radionuclides in the deep waters in the Japan Sea. Concerning spatial distributions, the area of high (137)Cs inventory extends from the Japan Basin into the Yamato Basin. It is suggested that wintertime convection of water, occurring mainly in the Japan Basin, causes the radionuclides to sink. The nuclides then advect into the Yamato Basin after detouring around the Yamato Rise.     

The transfer of radionuclides from saltmarsh vegetation to sheep tissues and milk

Radionuclides released into the Irish Sea by the Sellafield reprocessing plant are deposited onto tide-washed pastures along the western coast of the United Kingdom. Many of these pastures are grazed by sheep or cattle. This paper describes a controlled feeding study, in which saltmarsh vegetation harvested from close to the Sellafield plant, was fed to lambs and adult female sheep for a period of 8 weeks. Activity concentrations of (60)Co, (95)Nb, (106)Ru, (134)Cs, (137)Cs, (238)Pu, (239,240)Pu and (241)Am were determined in edible tissues and transfer parameters estimated. The activity concentrations of some of the radionuclides will not have been in equilibrium with those in the diet. Nevertheless, the study was reasonably realistic in terms of agricultural management as the period of the study was similar to that for which lambs graze on the saltmarshes. A field study to determine the activity concentrations of (137)Cs and (239,240)Pu in the milk of ewes grazing a saltmarsh close to Sellafield is also described.     

137Cs in the Danish Wadden Sea: contrast between tidal flats and salt marshes

The 137Cs activity of salt marsh and tidal flat sediments of the northern part of the European Wadden Sea was studied based on a comprehensive dataset of 210Pb dated cores. The 137Cs inventory of salt marsh sediments shows a major peak corresponding to the Chernobyl accident in 1986, and a minor peak located in the late 1960s interpreted as the combined effect of atmospheric testing of nuclear weapons. Emissions from the nuclear reprocessing plant Sellafield are not reflected as peaks in 137Cs activity, but may contribute to the rising 137Cs activity in the years prior to 1986. The 137Cs activity of tidal flat sediments differs from salt marsh sediment in two respects. First, the activity is much lower and, second, the major peak in the 1980s is located in the beginning instead of in the middle of the decade. The differences in 137Cs inventory between the two environments are interpreted to result from repeated cycles of deposition/resuspension and mixing on tidal flats. A simple model illustrating the consequence of mixings returns an apparent shift of major peaks in 137Cs activities backwards in time corresponding to the mixing depth divided by the deposition rate.     

Three-dimensional modelling of the tide-induced dispersion of radionuclides in the sea

A three–dimensional marine dispersion model for radionuclieds has been developed. The model solves the three–dimensional hydrodynamic equations and, simultaneously, the three–dimensional advective–diffusive dispersion equations. Thus the tide–induced dispersion of radionuclides is obtained. The equations are solved using a finite difference explicit scheme using a time step of a few seconds with appropriate boundary conditions. As an example the model has been applied to study the dispersion of ¹³⁷Cs in the Irish Sea which is released from the nuclear fuel reprocessing plant at Sellafield. Tidal amplitudes and current profiles obtained with the model have been compared with observations in the Irish Sea: both sets of data are in good agreement. Observed and computed ¹³⁷Cs distributions in waters have also been compared. The model gives a good representation of the dispersion of this radionuclide in the Irish Sea.     

The marine impact of caesium-134 and -137 from the Chernobyl reactor accident

¹³⁴Cs and ¹³⁷Cs from the Chernobyl reactor accident were detected in UK shoreline seawater very quickly after activity from the accident reached this country. Concentrations were highest in areas adjacent to those where deposition over land was highest, but they declined quickly and did not reach radiologically significant levels in terms of public radiation exposure. Subsequently, the distribution in seawater was investigated further afield. Radiocaesium attributable to the Chernobyl accident was found to be widespread: it was readily distinguished from other sources by having a different ¹³⁷Cs:¹³⁴Cs ratio (about 2:1). Its presence was especially noticeable in northern UK waters rather than those to the south; much of the North Sea has been surveyed as well as the Norwegian Sea. Evidence of Chernobyl radiocaesium was found as far north as 70°N and in many of these areas, including the northern North Sea, it overshadowed the effect of BNFL (British Nuclear Fuels plc) Sellafield discharges, previously the main source of these radionuclides.     

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

A dynamic model of plutonium behaviour in the marine environment has been developed, representing the oxidation state distribution and partitioning of plutonium between the soluble, colloidal, suspended particulate and seabed sediment fractions. With simple re-parameterisation, this model can also be applied to (137)Cs. The model, which is calibrated and validated against field data, has been used to predict concentrations of Pu(alpha) and (137)Cs in both water and seabed sediments from the vicinity of the Sellafield Ltd. reprocessing plant in Cumbria, UK. The model predicts that sediment reworking and transport are the key environmental processes as the Sellafield Pu(alpha) and (137)Cs discharge continues to decline. Inventory calculations generated by the model are consistent with previous estimations. For a hypothetical post-discharge scenario, the concentrations of these radionuclides in both seawater and surface sediments are predicted to decrease sharply, concurrent with a downward vertical migration of the activity retained in sediments.     

Temporal trends for 99Tc in Norwegian coastal environments and spatial distribution in the Barents Sea

The objective of this study was to reassess 99Tc transit times and transfer factors, from Sellafield to northern Norway, and to determine the extent of 99Tc migration to the Barents Sea. Filtered seawater samples were collected on a monthly basis from Hilles?y, northern Norway, and in February 1999 from the Barents Sea. Results showed an increase in levels of 99Tc at Hilles?y where activity concentrations have increased from a baseline of 0.2-0.4Bq m(-3) to a maximum of 1.6 Bq m(-3). A transit time of 42 months and a transfer factor of 6Bq m(-3) per PBq a(-1) have been derived, using cross-correlation analysis. The current study predicts that future levels are unlikely to increase dramatically over the levels observed in 1998. Levels of 99Tc in the Barents Sea ranged from 0.2 Bq m(-3) to 1.1 Bq m(-3) showing the influence of new 99Tc inputs by early 1999.     

Seasonal variations in activity concentrations of 99Tc and 137Cs in the edible meat fraction of crabs and lobsters from the central Irish Sea

Discharges of most radionuclides into the Irish Sea from the BNFL site at Sellafield have decreased over the past 20 years or so. For a few radionuclides, however, discharges have peaked more recently. Notably, operation of the Enhanced Actinide Removal Plant (EARP) since 1994 has led to an increase in discharges of (99)Tc, as a result of the treatment of previously stored waste, with consequent increases in (99)Tc activity concentrations in a number of marine species, particularly in crustaceans such as lobsters. Previous research has considered the significance of factors such as sex and body weight on radionuclide concentrations. The current project set out to investigate whether seasonal variations in radionuclide concentrations in crabs and lobsters occur, with particular emphasis on the dynamics of (99)Tc and (137)Cs. Organisms were obtained from a site off the Isle of Man, where radionuclide concentrations were measurable but the site was sufficiently distant from Sellafield that the radionuclides were well mixed in the water column and not likely to be influenced by the pulsed nature of discharges of (99)Tc. Crab and lobster samples were collected monthly, between February 2000 and February 2001. Fifteen or 16 individuals (evenly split as male and female) of each species were collected on each occasion. Seawater samples were also collected over the 12-month period. Activity concentrations of (99)Tc in the edible meat fraction (both brown and white meat) ranged from 0.23 to 2.46 Bq kg(-1) (fresh weight (fw)) in crabs and 124 to 216 Bq kg(-1) (fw) in lobsters, with no observed seasonal variations. Activity concentrations of (137)Cs in both crab and lobster were lower, ranging from <0.16 to 0.85 Bq kg(-1) for crab meat (fw) and <0.3 to 3.3 Bq kg(-1) for lobster meat (fw). A statistically significant increase in activity concentrations of (137)Cs in the meat was observed in the summer months for both crab and lobster. The cause has not been investigated but may be related to the laying down of energy reserves during the active feeding period over the summer. At all times, uptake of (99)Tc is higher in the brown meat fraction of both crabs and lobsters, whilst (137)Cs is more uniformly distributed. These results are used to discuss the implications for sampling and monitoring programmes.     

Present background levels of surface 137Cs and (239,240)Pu concentrations in the Pacific

The present levels of anthropogenic radionuclides, 137Cs and (239,240)Pu, in surface waters of the Pacific are estimated using the HAM database, which is a comprehensive data set of 137Cs, (239,240)Pu and other anthropogenic radionuclides. The time-series data of surface 137Cs and (239,240)Pu suggests that surface 137Cs and (239,240)Pu concentrations in the Pacific since 1971 decrease exponentially in each sea area, although the temporal changes of surface 137Cs and (239,240)Pu differed between sea areas of the Pacific. The calculated 137Cs concentrations in the Pacific surface waters in 2000 are homogeneous in the Pacific, comparing with that in the 1960s and 1970s, although they are still high in the North Pacific and low in the South Pacific. The biogeochemical and physical processes are significant factors to control present levels of surface (239,240)Pu concentrations, which are high in the Subarctic and equatorial Pacific and low in the mid-latitude region of the eastern North Pacific.     

Behaviour and transport of radionuclides in soil and vegetation of a sand dune ecosystem

A sand dune ecosystem in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK was used to examine the spatial, temporal and depth distributions of 134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am in soil and in two species of vegetation (Festuca rubra, Ammophila arenaria). Core samples showed evidence of the accumulation of radionuclides derived mainly from sea-to-land transfer. Accumulated deposits of radioactivity (0-0.1 m) lie within the range: 1.1-3.4 Bq kg-1 (134Cs), 260-440 Bq kg-1 (137Cs), 31-40 Bq kg-1 (238Pu), 150-215 Bq kg-1 (239 + 240Pu) and 190-240 Bq kg-1 (241Am). Soil profiles showed greater activity concentrations in their deeper regions and this is attributed to leaching of radionuclides in percolating drainage water accentuated by the coarse texture, low organic matter and clay mineral content of coastal sands. Radionuclide activity concentrations in F. rubra and A. arenaria were similar, in the ranges 20-70 Bq kg-1 (137Cs), 1-5 Bq kg-1 (238Pu), 10-30 Bq kg-1 (239 + 240Pu) and 10-65 Bq kg-1 (241Am). Clear temporal and spatial variations were observed in both species of vegetation, reflecting the weather conditions antecedent to the sampling period and the influence of sea-to-land transfer. Concentration ratios (vegetation:soil) for activity concentrations in the two species were similar, in the ranges: 0.05-0.14 (137Cs), 0.025-0.097 (238Pu), 0.022-0.057 (239 + 240Pu) and 0.025-0.212 (241Am).     

MEAD (part I)--a mathematical model of the long-term dispersion of radioactivity in shelf sea environments

A mathematical model (MEAD) that simulates the transport of radioactivity in shelf-sea environments is presented. In the model it is assumed that the radioactivity can be present in three phases and transport both within and between the phases is captured. The set-up of the model for the Irish Sea is described and results from a simple discharge scenario are presented for (137)Cs and (239)Pu. From these results it appears that MEAD provides a good representation of the transport of radionuclides in the Irish Sea.     

Tracing anthropogenic nuclear activity with (129)I in lake sediment

This study reports the first data of (129)I fallout in Scandinavia, covering the last 80 years. The investigation is based on sediment sections from a lake in central Sweden. In addition to analysis of (129)I, a combination of several radionuclides ((210)Pb, (137)Cs and (14)C) was used to establish an accurate chronology of the sediment profile. The concentration of (129)I exhibits an increasing trend ( approximately 10(7) to approximately 10(9)atoms/g) during the last 40 years, suggesting a significant atmospheric input from the nuclear reprocessing facilities in Sellafield (UK) and La Hague (France). A peak corresponding to fallout from the Chernobyl accident (1986) is clearly distinguishable, whereas the impact of fallout from the nuclear weapons' tests since the early 1950s is not distinguished.     

Radionuclides deposition over Antarctica

A detailed and comprehensive map of the distribution patterns for both natural and artificial radionuclides over Antarctica has been established. This work integrates the results of several decades of international programs focusing on the analysis of natural and artificial radionuclides in snow and ice cores from this polar region. The mean value (37+/-20 Bq m(-2)) of (241)Pu total deposition over 28 stations is determined from the gamma emissions of its daughter (241)Am, presenting a long half-life (432.7 yrs). Detailed profiles and distributions of (241)Pu in ice cores make it possible to clearly distinguish between the atmospheric thermonuclear tests of the fifties and sixties. Strong relationships are also found between radionuclide data ((137)Cs with respect to (241)Pu and (210)Pb with respect to (137)Cs), make it possible to estimate the total deposition or natural fluxes of these radionuclides. Total deposition of (137)Cs over Antarctica is estimated at 760 TBq, based on results from the 90-180 degrees East sector. Given the irregular distribution of sampling sites, more ice cores and snow samples must be analyzed in other sectors of Antarctica to check the validity of this figure.     

Seabed gamma-ray spectrometry: applications at IAEA-MEL

The technique of underwater gamma-ray spectrometry has been developed to complement or replace the traditional sampling-sample analysis approach for applications with space-time constraints, e.g. large areas of investigation, emergency response or long-term monitoring. IAEA-MEL has used both high-efficiency NaI(Tl) and high-resolution HPGe spectrometry to investigate contamination with anthropogenic radionuclides in a variety of marine environments. Surveys at the South Pacific nuclear test sites of Mururoa and Fangataufa have been used to guide sampling in areas of high contamination around ground zero points. In the Irish Sea offshore from the Sellafield nuclear reprocessing plant, a gamma-ray survey of seabed sediment was carried out to obtain estimates of the distribution and subsequently, for the inventory of 137Cs in the investigated area.     

A modelling study on 137Cs and 239,240Pu behaviour in the Alborán Sea, western Mediterranean

A model for simulating the dispersion processes of 137Cs and 239,240Pu in the Alborán Sea is described. The model consists of two hydrodynamic models: a 2D depth-averaged model and a two-layer model which provide tidal and geostrophic currents, respectively; a sediment transport model which provides suspended particle concentrations and sedimentation rates over the domain; and the radionuclide dispersion model including interactions of dissolved radionuclides with suspended particles and bed sediments. These processes are formulated using kinetic transfer coefficients. The hydrodynamic and sediment models are run and validated in advance, and their results are then used to simulate the dispersion of 137Cs and 239,240Pu, which are introduced from atmospheric fallout. Radionuclide concentrations in the water column and distributions in bed sediments have been compared with measurements in the sea. Both set of data are, in general, in agreement. The model has also been applied to calculate radionuclide fluxes through the Strait of Gibraltar. These computed fluxes have been compared with previous estimations as well.     

Mesoscale modelling of radioactive contamination formation in Ukraine caused by the Chernobyl accident

This work is devoted to the reconstruction of time-dependent radioactive contamination fields in the territory of Ukraine in the initial period of the Chernobyl accident using the model of atmospheric transport LEDI (Lagrangian-Eulerian DIffusion model). The modelling results were compared with available 137Cs air and ground contamination measurement data. The 137Cs atmospheric transport over the territory of Ukraine was simulated during the first 12 days after the accident (from 26 April to 7 May 1986) using real aerological information and rain measurement network data. The detailed scenario of the release from the accidental unit of the Chernobyl nuclear plant has been built (including time-dependent radioactivity release intensity and time-varied height of the release). The calculations have enabled to explain the main features of spatial and temporal variations of radioactive contamination fields over the territory of Ukraine on the regional scale, including the formation of the major large-scale spots of radioactive contamination caused by dry and wet deposition.