Long-term study of 99Tc in the marine environment on the Swedish west coast

The activity concentration of (99)Tc in brown seaweed (Fucus vesiculosus and Fucus serratus) and seawater were analysed in samples collected in 1991, 1995 and 2001 at several stations along the Swedish west coast. In addition to these locations, a well-defined site (S?rdal, 56.76 degrees N, 12.63 degrees E) was included with (99)Tc activity concentration data in seaweed from 1967 to 2000. Over the years, the major source of (99)Tc in the coastal waters of western Sweden has been the radioactive liquid discharge from the nuclear fuel reprocessing plant in Sellafield (UK) transported via ocean currents in the North Sea. The (99)Tc activity concentration in seaweed at the S?rdal site increased from approximately 30 Bq kg(-1) up to 230 Bq kg(-1) (dry weight) between 1997 and 2000 due to the Sellafield EARP (Enhanced Actinide Removal Plant) discharges in 1995-1996, yielding an approximate transport time of 4-5 years between the Irish Sea and the Kattegat. Due to the very sharp gradient in (99)Tc concentration between the Baltic Sea and the North Sea, (99)Tc is presently one of the best transit tracers for the recent ventilation events in the Baltic Sea.     

Trends in the spatial and temporal distribution of 129I and 99Tc in coastal waters surrounding Ireland using Fucus vesiculosus as a bio-indicator

Spatial and temporal trends in (129)I and (99)Tc concentrations around the Irish coastline have been evaluated using Fucus vesiculosus as a bio-indicator. (129)I concentrations in a recent set of seawater samples have also been recorded and reveal an identical spatial pattern. Concentrations of (129)I in Fucus from the northeast coast of Ireland proved to be at least two orders of magnitude higher than concentrations in Fucus from the west coast. The (129)I content of Fucus increased significantly between 1985 and 2003, in line with increases in discharges of (129)I from the Sellafield nuclear reprocessing plant. Similar trends were observed in the case of (99)Tc. (129)I/(99)Tc ratios in Irish seawater were deduced from the Fucus data, and compared to ratios in discharges from Sellafield and from the French reprocessing plant at Cap de la Hague. Levels of (129)I and (99)Tc in Fucus from the west coast were found to be enhanced with respect to levels in seaweeds from other regions in the Northern Hemisphere unaffected by discharges from nuclear installations such as those referred to.     

Sea-to-land transfer of technetium-99 through the use of contaminated seaweed as an agricultural soil conditioner

The use of seaweed as an agricultural soil conditioner gives rise to a potential pathway for the transfer of Technetium-99 ((99)Tc) from marine to terrestrial ecosystems and thence to man. However, to date there is little information on the extent of the release of (99)Tc from seaweed into soil and the mechanisms involved. This pot experiment has shown that (99)Tc is released fairly rapidly from Fucus vesiculosus into a sandy coastal soil. Despite low temperature conditions, 60% of the (99)Tc added with the seaweed had accumulated in the soil 15 weeks after addition. Concurrent CO(2) monitoring (used as a measure of microbial decomposition or catabolism) suggested that the initial (99)Tc release (up to 40% in the first 8 weeks) was due to leaching from the seaweed and that microbial decomposition was responsible for the release of the remaining (99)Tc in the latter phase (12-15 weeks).     

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.     

The dispersion of 99Tc in the Nordic Seas and the Arctic Ocean: a comparison of model results and observations

The radionuclide (99)Tc had been discharged from the nuclear reprocessing facility in Sellafield (UK) into the Irish Sea in increased amounts in the 1990s. We compare the simulated dispersion of (99)Tc in surface water as calculated by a hydrodynamic model and an assessment box model with field-observations from 1996 to 1999 to study concentrations, pathways and travel times. The model results are consistent with the observations and show the typical pathway of dissolved radionuclides from the Irish Sea via the North Sea along the Norwegian Coast. Subsequently the contaminated water separates into three branches of which the two Arctic branches bear the potential for future monitoring of the signal in the next decades. The results of the hydrodynamic model indicate a large variability of surface concentrations in the West Spitsbergen Current which has implications for future monitoring strategies. According to the observed and simulated distributions we suggest an improved box model structure to better capture the pattern for concentrations at the surface.     

Studies of Np and Pu in the marine environment of Swedish-Danish waters and the North Atlantic Ocean

The long-lived anthropogenic radionuclides (237)Np, (239)Pu and (240)Pu were determined in marine environmental samples (seaweed and seawater) collected from Swedish-Danish waters and the North Atlantic Ocean at various locations on different occasions during the period 1991-2001. The measurements were performed with sector field Inductively Coupled Plasma Mass Spectrometry (ICP-MS) and conventional alpha spectrometry. The (237)Np activity concentrations in Fucus vesiculosus and surface seawater from the Swedish west coast and Danish waters ranged from 0.16+/-0.02 to 1.02+/-0.09 mBq kg(-1) (dry weight) and 0.65+/-0.02 to 1.69+/-0.02 mBq m(-3), respectively, depending on the location and sampling year. Most of the (237)Np in these waters is believed to originate from the Sellafield nuclear reprocessing plant, with some contribution from global fallout. The (240)Pu/(239)Pu atomic ratios in F. vesiculosus samples are reported in this study with an overall average of 0.17+/-0.03. The (237)Np and (239)Pu activity concentrations observed in surface seawater collected in North Atlantic waters ranged from 0.16+/-0.01 to 0.62+/-0.08 mBq m(-3) and from 0.64+/-0.05 to 4.27+/-0.08 mBq m(-3), respectively, and the (237)Np/(239)Pu atomic ratios were a good indicator of conservative behaviour of Np in marine waters.     

Spatio-temporal variations in the technetium-99 content of fucus serratus in the english channel during 1982–1984

Spatio-temporal variations in the technetium-99 content of Fucus serratus samples from the French coast of the English Channel were studied between 1982 and 1984 using various sampling strategies. The lack of constancy in measurements from within the seaweed zone of the same station is revealed by a variation of 18% in the mean contents of samples collected from different sampling levels, a variation which reaches 41% if the extreme values of all results are taken into account. Regional variations over the Channel as a whole show an asymmetric diminution of the ⁹⁹Tc content of the seaweed on the two sides of the liquid effluent discharge outlet from the reprocessing plant at La Hague and this confirms a predominant drift of Channel waters towards the North Sea. Variations with time at three stations during 1983 and 1984 have revealed that there is a time-lag between fluctuations observed in the discharges and those in F. serratus. In addition, a periodic component observed at the Roscoff and Wimereux stations, where the ⁹⁹Tc content of the seaweed varies by a factor of 2–3 between winter and summer periods, could be correlated with seasonal changes both in the metabolic state of F. serratus and in the currents to the south-west of Cap de La Hague. ⁹⁹Tc, which here has no radiological impact on man, would thus appear to be a radioactive label for sea waters and one which is particularly sensitive to variations in environmental conditions.     

Evaluation of 20 years of environmental monitoring data around Swedish nuclear installations

Twenty years of environmental monitoring data around the Swedish nuclear power plants and the Studsvik research facilities have been evaluated. In the marine environment, Fucus vesiculosus generally has high activity concentrations and the presence of a large variety of radionuclides in comparison with other bioindicators. However, for single nuclides the detection frequency was higher for 110mAg in Littorina spp and for 152Eu in Macoma baltica in comparison with other bioindicators. Close to the discharge point the activity concentration of 60Co in F. vesiculosus and in the discharge water were correlated. In the terrestrial environment, few radionuclides were detected and the activity concentrations were generally low. Of the terrestrial indicators, mosses had the highest activity concentrations and also comprised the largest variety of radionuclides. The radiation doses to humans based on measurements of released activity were small. Based on the results from the evaluation, alternative sampling strategies for the monitoring program are discussed.     

Vertical distributions of (99)Tc and the (99)Tc/(137)Cs activity ratio in the coastal water off Aomori, Japan

Using a sector-field ICP-MS the vertical distributions of the ⁹⁹Tc concentration and ⁹⁹Tc/¹³⁷Cs activity ratio were measured in the coastal waters off Aomori Prefecture, Japan, where a spent-nuclear-fuel reprocessing plant has begun test operation. The ⁹⁹Tc concentrations in surface water ranged from 1.8 to 2.4 mBq/m³, no greater than the estimated background level. Relatively high ⁹⁹Tc/¹³⁷Cs activity ratios (10-12 × 10⁻⁴) would be caused by the inflow of the high-⁹⁹Tc/¹³⁷Cs water mass from the Japan Sea. There is no observable contamination from the reprocessing plant in the investigated area. The ⁹⁹Tc concentration and the ⁹⁹Tc/¹³⁷Cs activity ratio in water column showed gradual decreases with depth. Our results implied that ⁹⁹Tc behaves in a more conservative manner than ¹³⁷Cs in marine environments.     

129I/127I, 129I/137Cs and 129I/99Tc in the Norwegian coastal current from 1980 to 1998

Discharges of the nuclides 129I, 137Cs and 99Tc from the nuclear reprocessing facilities at Sellafield (UK) and La Hague (France) are very useful as oceanic tracers. On the basis of 129I/127I, 137Cs and 99Tc measurements in archived seaweeds, the ratios of 129I/127I, 129I/137Cs and 129I/99Tc have been estimated in seawater at two locations (Utsira and Kiberg) in the Norwegian Coastal Current from 1980 to 1998. These ratios, which vary up to two orders of magnitude over this period, are potentially very interesting for determining "transit times" in the Arctic and North Atlantic oceans. While the long-term trends in these ratios are quite clear, measurements in monthly and bimonthly samples show considerable structure. Further studies are required to determine the exact origin of this structure, which may be a limiting factor in the time resolution that can be obtained with these parameters.     

99Tc in the sub-arctic food chain Lichen-Reindeer-man

The deposition, migration and annual variations of ⁹⁹Tc fallout in carpets of lichen collected during the period 1956–1981 have been investigated. The transfer of ⁹⁹Tc to reindeer and man has also been studied. Technetium showed a shorter mean residence time than ¹³⁷Cs in the lichen carpet. The activity ratio ⁹⁹Tc/¹³⁷Cs was generally lower than the theoretical fission ratio of 1·43 × 10⁻⁴. The maximum concentration of ⁹⁹Tc in lichens occurred in 1967 (ca. 60 mBq kg⁻¹) but in 1975 higher values were found than would have been predicted from fallout. The average depth integrated concentration of ⁹⁹Tc at 62·3°N, 12·4° E in 1972 was 540 ± 100 mBq m⁻². The studies of reindeer tissues show that technetium has a short mean residence time in the muscle tissues (ca. 5 days) and is not accumulated like ¹³⁷Cs. The committed dose equivalent from ⁹⁹Tc to the local Lapp population engaged in reindeer breeding is negligible.     

Changing patterns of radionuclide distribution in Irish Sea subtidal sediments

This paper presents new data on the distribution of long-lived radionuclides in Irish Sea subtidal sediments, contaminated as a result of the BNFL Sellafield discharges. The results from different sampling campaigns in 1999 have been combined to assess the extent of radionuclide mobility relative to earlier surveys, in both the eastern and western Irish Sea areas, and to investigate changes in radionuclide distribution over time. The results appear to confirm the trend of continuing re-distribution and transfer of contamination away from the English coast. West of the Isle of Man, radionuclide concentrations and inventories have remained more or less constant. The inventory of radionuclides in sandy sediments in the eastern Irish Sea is still under-represented by current sampling, but could be improved by deeper and more extensive vibrocoring.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.     

Radionuclides in marine macroalgae from Amchitka and Kiska Islands in the Aleutians: establishing a baseline for future biomonitoring

Levels of radionuclides in seven species of marine brown algae and Ulva were determined to establish a baseline for the Northern Pacific Ocean/Bering Sea (Aleutian Islands). There were differences in levels among algal species and locations (Amchitka Island vs Kiska Island). No values were above the minimum detectable activity (MDA) level for (137)Cs, (129)I, (60)Co, (152)Eu, (90)Sr, and (99)Tc. There were interspecific differences in some radionuclides: Ulva lactuca (=Ulva fenestrata) had the highest levels of (241)Am, Alaria fistulosa had the highest levels of (239,240)Pu, and Fucus distichus (=Fucus gardneri) had the highest levels of (234)U, (235)U, and (238)U. However, levels of all radionuclides were generally low and near the MDA for all isotopes. Although Amchitka Island had higher levels of (239,240)Pu than Kiska, the differences were very small and not significant biologically. The data indicate that algae can be useful bioindicators of actinides because they accumulate them at very low environmental levels, allowing them to provide early warning of any potential seepage of radionuclides into the marine environment. Further, the data indicate that some species (the intertidal Fucus) are better accumulators than others, and these should be used as bioindicators in future monitoring schemes.     

Heavy metals in organisms and sediments from Turkish Coast of the Black Sea, 1997-1998

During the period 1997-1998, macroalgae, sea snail, mussel, fish and sediment samples were collected at different stations of the Turkish Black Sea coast in order to establish the concentration of selected heavy metals. Heavy metals analyzed were Cd, Co, Cr, Ni, Zn, Fe, Mn, Pb and Cu. The results showed that the Turkish Black Sea coast is facing heavy metal pollution. The metal concentrations in macroalgae, sea snail, mussel and sediment samples are very high. However, Cd, Pb and Cu concentrations in anchovy fish decreased, while Co, Fe, Zn, Cr, Mn and Ni contents had changed when compared previous data. The metal levels in macroalgae did not follow the same pattern as concentrations in sediments at the same station. On the other hand, concentrations of Cd, Co, Cr, Zn, Fe, Mn and Cu in sea snail, mussel and fish samples were related to sediment data in the examined stations.     

Accumulation of 99Tc in duckweed Lemna minor L. as a function of growth rate and 99Tc concentration.

This study focuses on the question of whether short-term studies can be used to forecast the accumulation of the long-lived fission product 99Tc in duckweed, Lemna minor L., grown in the field; in other words, are the accumulation parameters independent of changing growth rates typical of natural populations of duckweed. Two processes determine the 99Tc accumulation: (i) uptake and release of 99TcO4-, characterised by a concentration factor, Kd, and (ii) first-order reduction and complexation of TcVII, characterised by kred. At various 99Tc concentrations, the growth, total Tc and TcO4- accumulation were monitored over 10 days; parameters were fitted and compared with earlier results. Both Kd and kred turn out to be independent of time, concentration and growth rate up to a concentration of 10(-6)mol l(-1) 99TcO4-. Concentrations above this level result in toxic effects. The Tc accumulation in field populations of duckweed at Tc concentrations which generally occur in the environment can be forecasted by using the results from short-term experiments.     

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.     

Estimating biological half-lifes of radionuclides in marine compartments from environmental time-series measurements

Modelling radionuclide transfers between seawater and marine species on a short time scale basis requires being able to take into account the transfer kinetics. This means (1) to implement the effect of the biological half-lives of radionuclides together with the concentration factor in the calculation of transfers and (2), to get these kinetic parameters for each element and species. Biological half-lives are usually determined from laboratory labelling experiments with the challenge to match natural environmental conditions. The present work proposes a simple model that implements the effect of kinetic parameters in the calculation of transfers. This model is also used to derive the biological half-life and the concentration factor for 137Cs from time-series measurements of environmental concentrations in seawater and in the brown alga Fucus serratus, as an example. These transfer parameters are finally used to predict the Cs activities in Fucus serratus on the English Channel shores.     

99Tc in seawater in the West Spitsbergen Current and adjacent areas

99Tc levels were measured in seawater samples collected between 2000 and 2002 in the West Spitsbergen Current (WSC) and along the western coast of Svalbard or Spitzbergen and compared with available oceanographic 3-D modelling results for the late 1990s. Additional data from related regions are also presented in order to support the data interpretation. The seawater in the Arctic fjord Kongsfjorden on the western coast of Svalbard is influenced by the WSC, as shown by the 99Tc levels in surface water. By means of the WSC, 99Tc reaches the Eastern Fram Strait, where one branch of the WSC turns west into the East Greenland Current (EGC), and another branch continues northwards into the Arctic Ocean. Surface seawater collected in the central part of the WSC during a cruise on board the R/V "Polarstern" in the summer of 2000, showed higher levels of (99)Tc than samples measured in Kongsfjorden in the spring of 2000. However, all levels measured in surface water are of the same order of magnitude. Data from sampling of deeper water in the WSC and EGC provide information pertaining to the lateral distribution of 99Tc. In all vertical profiling surveys (conducted in spring and summer), the highest levels of 99Tc were found in surface water. Comparison with oceanographic 3-D modelling indicates both significant seasonal variations in the lateral stratification of the WSC and variations with depth over shorter vertical distances. This information can be applied in sampling strategies, environmental monitoring, long-range transport of pollutants and physical oceanography.