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.     

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.     

Artificial radionuclides in sediments of the Don River Estuary and Azov Sea

The Don River Estuary-Azov Sea system is an extension of the shallow continental shelf area of the Black Sea. A large data set of artificial radionuclides in bottom sediments of the Azov Sea has been compiled in order to examine the storage and migration of radionuclides within this highly restricted inland sea and to estimate the annual dose received by individuals in the local population who regularly consume fish. In recent years (1997-1999), the radionuclide content of surface sediments has been: 137Cs < or = 0.5-100 Bq/kg d.w. (mean = 33.8 +/- 25.9 Bq/kg d.w., n = 57), 90Sr = 0.2-5.7 Bq/kg d.w. (mean = 2.1 +/- 1.4 Bq/kg d.w., n = 34) and 239,240Pu = 0.31-0.51 Bq/kg d.w. (n = 2). In general, 137Cs activities increase with distance from the mouth of the Don River and correlate negatively with sediment grain size (r2 = 0.77, n = 21). The annual 137Cs-derived dose received by an individual through the trophic chain water-fish-humans (approximately 10(-6) Sv/yr) is well below regulatory recommended limits, indicating that current levels of radioactivity in the environment pose no threat to commercial fisheries operations for the bordering nations of Russia and Ukraine.     

Variability in the edible fraction content of 60Co, 99Tc, 110mAg, 137Cs and 241Am between individual crabs and lobsters from Sellafield (north eastern Irish Sea)

We investigated the variability of anthropogenic radionuclide content of the edible fractions of individual edible crabs (Cancer pagurus L.) and European lobsters (Homarus gammarus L.) caught commercially in the Sellafield offshore area. Sixteen female and 18 male crabs and 20 female and 17 male lobsters were selected from commercial catches made between 25 May and 5 June 1997. Each gender group was selected to be within the known weight range for commercially caught crustacea from the area. Four artificial radionuclides (60Co, 110mAg, 137Cs or 241Am) were detected by gamma-spectrometry. The edible fraction content of these radionuclides between males and females for either species were not statistically significantly different. 99Tc was analysed by chemical separation and beta-counting. 99Tc concentrations in female crabs tended to be higher (172 +/- 205 (16) Bq kg-1(wet); mean +/- standard deviation (n samples)) than those in males (85 +/- 58 (18) Bq kg-1 (wet)), although this was not a statistically significant difference. For both male and female crabs, 99Tc concentrations tended to decrease with increasing whole live weights. For 99Tc in lobsters the picture is less clear. Female lobsters contained more activity (14800 +/- 7400 (20) Bq kg-1 (wet)) than males (7100 +/- 3900 (17) Bq kg-1 (wet)). The results were used to discuss the implications for sampling and monitoring.     

Effect of low continuous 99Tc intake on its absorption and metabolism in young rats

A continuous daily oral dose of (99)TcO(4)(-) (5 Bq g(-1) day(-1)) was given to young rats for 56 days. In one group the intake was continued for 98 days, while in the other the intake was stopped to facilitate the determination of biological half lives in different organs and tissues. The absorbed fraction of (99)Tc increased from 0.7 to 0.9 during the experimental period (m=0.85 sigma=0.02). The whole body retained fraction (m=0.15 sigma=0.05) indicated a storage in the tissues. The liver and kidneys showed increasing concentrations of (99)Tc until a plateau was reached after 6 and 9 weeks, then a rapid decline after the intake was stopped (half life of 6 and 5 days respectively). In hair and thyroid tissue, the accumulation of (99)Tc increased linearly then declined very slowly after the intake was stopped and did not reach a plateau during the experiment. No significant amounts of (99)Tc were detected in the muscular tissues or in the walls of the digestive tract. After the contamination period, urinary and fecal excretions fell off very quickly (1 week), but significant, though low, quantities of urinary and fecal excretions were still observed 6 weeks after stopping intake.     

Variation of the activity concentrations and fluxes of natural (210Po, 210Pb) and anthropogenic (239,240Pu, 137Cs) radionuclides in the Strait of Gibraltar (Spain)

The activity concentrations and fluxes of natural (210Pb, 210Po) and anthropogenic (239,240Pu, 137Cs) radionuclides have been determined in the different water masses crossing the Strait of Gibraltar. New data have been gathered during four multidisciplinary and multinational sampling campaigns, performed between 1997 and 1999 within the framework of the CANIGO-FLUGIST Project. Mean activity concentrations of 210Po (1.53+/-0.34 Bq m(-3), n = 30) and 210Pb (1.16+/-0.50 Bq m(-3), n = 31) in the Atlantic water entering the Mediterranean basin are about double those measured in the Mediterranean outflow, namely 0.84+/-0.34 Bq m(-3) (n = 22) for 210Po and 0.66+/-0.34 Bq m(-3) (n = 22) for 210Pb. The opposite trend is observed for 231,240Pu, with average concentrations of 9.9+/-3.0 mBq m(-3) (n = 29) in the incoming Atlantic flow and 22.0+/-3.0 mBq m(-3) (n = 22) in the outpouring Mediterranean water. In the case of 137Cs, the same concentrations were quantified in the waters moving inwards (2.52+/-0.28 Bq m(-3), n = 27) and outwards (2.14+/-0.52 Bq m(-3), n = 21) from the Mediterranean Sea. On this basis, the Mediterranean basin experiences a net annual input flux of 14 TBq of 210Pb and 19 TBq of 210Po, and a net annual loss of 0.34 TBq of 239,240Pu, while--at present--137Cs input and output fluxes appear to be balanced.     

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.     

A nationwide survey of outdoor radon concentration in Japan

Nationwide outdoor radon (222Rn) concentrations in Japan were measured to survey the environmental outdoor 222Rn level and to estimate the effective dose to the general public from 222Rn and its progeny. The 222Rn concentration was measured with a passive-type radon monitor. The 222Rn monitors were installed at about 700 points throughout Japan from 1997 to 1999. The annual mean 222Rn concentration in Japan was estimated from four quarters measurements of 47 prefectures in Japan. Nationwide outdoor mean 222Rn concentration was 6.1 Bq m(-3). This was about 40% of the indoor 222Rn concentration in Japan. The 222Rn concentration in Japan ranged from 3.3 Bq m(-3) in the Okinawa region to 9.8 Bq m(-3) in the Chugoku region, reflecting geological characteristics. Seasonal variation of outdoor 222Rn concentration was also found to be lowest in July to September, and highest in October to December. From the results of this 222Rn survey and previous indoor 222Rn survey program, the effective dose to the general public from 222Rn and its progeny was estimated to be 0.45 mSv y(-1).     

Comparative studies of health hazard from radon (Rn-222) in two selected lithologic formations in the Suwałki region (in Poland)

The aim of this work was to make a comparison of indoor radon concentrations in dwellings and in soil air in the area of two geological formations in the Suwa?ki region (Poland). The mean arithmetic airborne concentration was found to be the highest (301 Bq m (-3)) in the basements of buildings in the gravel and sand areas, whereas in the boulder clay areas it reached 587 Bq m (-3). Out of 54 measurements of radon concentrations performed at the ground floor, in eight cases concentrations were found to exceed 200 Bq m (-3) - permissible radon level in new-built houses in Poland and in three cases these values were even higher than 400 Bq m (-3). The highest radon levels were noted in houses with earthen basement floors and with direct entrance from the basement to rooms or kitchens. The mean arithmetic radon concentration in the soil air in the sandy and gravel formations was 39.7 kBq m (-3) and in clay formation it was 26.5 kBq m (-3). Higher radon levels were also found in the water obtained from household wells reaching 8367 Bq m (-3) as compared with tap water (2690 Bqm (-3)). The mean indoor concentration for the whole area under study was found to be 169.4 Bq m (-3), which is higher than the mean value for Poland (49.1 Bq m (-3)) by a factor of 3.5.     

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.     

Distribution and inventories of fallout radionuclides (239+240Pu, 137Cs) and 210Pb to study the filling velocity of salt marshes in Doñana National Park (Spain)

Within an extensive multinational and multidisciplinary project carried out in Do?ana National Park (Spain) to investigate its preservation and regeneration, the filling velocity of the salt marshes has been evaluated through the calculation of their average sediment accumulation rates. (239+240)Pu and (137)Cs from weapons testing fallout and total (210)Pb distribution profiles and inventories have been determined in some of the most characteristic zones of the park, namely, the ponds (or "lucios") and the waterjets (or "ca?os"). Plutonium inventories range from 16 to 101 Bq m(-2), (137)Cs values fluctuate between 514 and 3,758 Bq m(-2) and unsupported (210)Pb values comprise between 124 and 9398 Bq m(-2). Average sedimentation rates range from 3 to 5 mm y(-1) (1952-2002). These data are higher than those obtained by carbon dating for the period 6,500 AD-present, estimated as 1.5-2 mm y(-1), suggesting an increase in the accumulation of sediments and the alteration of the park's hydrodynamics caused by the re-channeling of the major rivers feeding the salt marshes.     

An overview of an indoor radon study carried out in dwellings in India and Bangladesh during the last decade using solid state nuclear track detectors

This paper reports on radon concentrations in dwellings from fifty different locations of India. The incorporated data were obtained using the passive solid state nuclear track detector technique. The estimated geometric mean value for India is 67.1 Bq m(-3). Chuadanga in Bangladesh had the lowest observed indoor radon concentration of 27.3 Bq m(-3) and Una in the northern part of India had the highest concentration of 281.5 Bq m(-3). This paper discusses the national geometrical mean value in terms of the national geometric mean values of other countries and also in terms of the geological influence. The estimated indoor radon levels are compared with the indoor radon levels as recommended by the International Commission on Radiation Protection (ICRP). It was observed that there are several locations in India where dwellings have higher indoor radon levels than the ICRP recommended value and requires some sort of intervention from regulating authorities. The mean value for indoor radon level given in the report of UNSCEAR 2000 for India needs to be revised.     

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.     

Bioaccumulation of 137Cs in pelagic food webs in the Norwegian and Barents Seas

Knowledge and documentation of the levels of radioactive contamination in fish stocks important to Norwegian fisheries is of major importance to Norwegian consumers and fish export industry. In the present study, the bioaccumulation of caesium-137 ((137)Cs) has been investigated in marine food webs in the Barents and Norwegian Seas. The contents of (137)Cs in the different organisms were generally low (<1 Bq kg(-1) wet weight), but a marked bioaccumulation was apparent: The concentration of (137)Cs was about 10-fold higher in the harbour porpoise Phocoena phocoena, representing the upper level of the food web, than in the amphipod Themisto sp., representing the lower level of the food web. The Concentration Factors (CF=Bq kg(-1) wet weight/Bq l(-1) seawater) increased from 10+/-3 for a mixed sample of krill and amphipods to 165+/-5 for harbour porpoises.     

Radon-222 signatures of natural ventilation regimes in an underground quarry

Radon-222 activity concentration has been monitored since 1999 in an underground limestone quarry located in Vincennes, near Paris, France. It is homogeneous in summer, with an average value of 1700 Bq m(-3), and varies from 730 to 1450 Bq m(-3) in winter, indicating natural ventilation with a rate ranging from 0.5 to 2.4 x 10(-6) s(-1) (0.04-0.22 day(-1)). This hypothesis is supported by measurements in the vertical access pit where, in winter, a turbulent air current produces a stable radon profile, smoothly decreasing from 700 Bq m(-3) at 20 m depth to 300 Bq m(-3) at surface. In summer, a thermal stratification is maintained in the pit, but the radon-222 concentration jumps repeatedly between 100 and 2000 Bq m(-3). These jumps are due to atmospheric pressure pumping, which induces ventilation in the quarry at a rate of about 0.1 x 10(-6) s(-1) (0.009 day(-1)). Radon-222 monitoring thus provides a dynamical characterisation of ventilation regimes, which is important for the assessment of the long-term evolution of underground systems.     

The application of phosphogypsum in agriculture and the radiological impact

Radium-226 in phosphogypsum produced in a phosphate industry, SICNG operating at Thessaloniki, Northern Greece since May 1966, varied from 261 to 688 Bq kg(-1) (mean value 508 Bq kg(-1)). This radionuclide in soil tilled with phosphogypsum used for agricultural purposes varied from 50 to 479 Bq kg(-1) (average 205 Bq kg(-1)), while in the regular soil of cultivated fields it varied from 37 to 54 Bq kg(-1) (average 48 Bq kg(-1)). Radium-226 in rice originated from cultivated fields tilled with phosphogypsum or not varied from 0.36 to 1.98 Bq kg(-1) (average 1.53 Bq kg(-1)) with the higher values observed in samples originated from cultivated fields tilled with phosphogypsum. Radium-226 transfer factors, TF, from soil tilled with phosphogypsum to plants for the case of rice varied from 6.5 x 10(-3) to 2.0 x 10(-2) (geometric mean: 1.1 x 10(-2)). A mean (226)Ra content in rice 1.53 Bq kg(-1) results in a daily intake of (226)Ra by humans in Greece 0.0084 Bq day(-1) leading to an annual effective dose for adults 0.86 microSv y(-1) which is much less in contributing to the average exposure to natural radiation sources (2.4 mSv y(-1)) and particularly to the part due to ingestion (0.29 mSv y(-1)). It is necessary to continuously control (monitoring) (226)Ra in phosphogypsum before any use for agricultural purposes.     

Contamination of the southern Baltic Sea with 137Cs and 90Sr over the period 2000-2004

Changes of the (137)Cs activity concentrations in the southern Baltic Sea waters were investigated over the period 2000-2004 and distribution of the (90)Sr concentrations was determined in 2004. In the discriminated period further decrease of (137)Cs concentrations was observed. The average activity concentration of (137)Cs declined from 59.4Bq/m(3) in 2000 to 45.1Bq/m(3) in 2004. The greatest changes of (137)Cs activities occurred in 2003 as a consequence of the medium-size inflow of a saline waters from the North Sea. This inflow affected (137)Cs activities as well as its distribution in the Baltic Sea. Changes in (90)Sr activity concentrations proceeded at much slower rate. The average activity concentration of (90)Sr was equal to 8.7Bq/m(3) in 2004. The annual fluvial (137)Cs fluxes from the Vistula river were also estimated. In 2000, the (137)Cs load from Vistula was of an order of 0.15TBq/year, and in 2004 0.05TBq/year.     

Monitoring and modelling of indoor radon concentrations in a multi-storey building at Mumbai,India

Radon (Rn(222)) levels in an indoor atmosphere of a multi-storey building at Mumbai have been measured for one year covering all the four seasons. Monitoring was carried out using the time-integrated passive detector technique, using Kodak-115 type Solid State Nuclear Track Detector (SSNTD) films of 2.5x2.5 cm size. Measured indoor radon levels showed a decreasing trend with height with concentration ranging from 41 Bq m(-3) at ground floor level to 15 Bq m(-3) at 19th floor level. Using the dose conversion factors, the inhalation dose due to breathing of radon gas is estimated to be 1.03 mSv y(-1) at the ground floor to 0.38 mSv y(-1) at the 19th floor level. Measured indoor radon concentrations on each floor were compared with the computed values using a mathematical model. The agreement between measured values and calculated values of indoor concentrations at different floors was very good within the limitations of various field parameter values.     

Natural radioactivity measurements in the city of Ptolemais (Northern Greece)

Specific activities of the natural radionuclides (238)U, (226)Ra, (232)Th and (40)K were measured by means of gamma-ray spectrometry in surface soil samples collected from the city of Ptolemais, which is located near lignite-fired power plants. The mean activity values for (238)U, (226)Ra, (232)Th and (40)K were found to be 42+/-11, 27+/-6, 36+/-5 and 496+/-56 Bq kg(-1), respectively. These values fall within the range of typical world and Greek values for soil. The indoor radon concentration levels, which were also measured in 66 dwellings by means of SSNTD, ranged from 12 to 129 Bq m(-3), with an average value of 36+/-2 Bq m(-3). This value is close to world and Greek average values for indoor radon concentrations. The total effective dose due to outdoor external irradiation of terrestrial origin and to indoor internal irradiation from the short-lived decay products of (222)Rn was estimated to be 1.2 mSv y(-1) for adults, which is lower than the global effective dose due to natural sources of 2.4 mSv y(-1).     

Indoor radon levels and influencing factors in houses of Patras,Greece

Measurements of indoor radon concentrations were performed in 28 low-rise houses and 30 apartments in Patras area from December 1996 to November 1997, using nuclear track detectors. The investigation was focused on the effects of season and floor number, as well as on the existence of a basement in low-rise houses on indoor radon levels. It was found that the differences in mean radon concentrations between adjacent seasons, in a number of 61 selected sampling sites distributed in 28 houses, were statistically significant. As expected, a maximum was found in winter and a minimum in summer. The differences in mean radon concentration on different floors of the same houses were also statistically significant and followed a linear decrease from underground to 2nd floor. In addition, indoor radon concentrations in the ground floor were found to be influenced by the existence or not of a basement. The average annual radon concentration was found to be 41 Bq m(-3) for the houses, 28 Bq m(-3) for the apartments and 38 Bq m(-3) for all the dwellings. These values lead to an average effective dose equivalent of 1.1, 0.7 and 0.9 mSv y(-1), respectively. Residents living on the underground in low-rise houses, during winter, where the average effective dose equivalent is 2.1 mSv y(-1), attain the higher risk.