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.     

Levels of natural radionuclides in some Nigerian cereals and tubers

The activities of radionuclides in the two major groups of foodstuff widely consumed in Nigeria have been determined. The 40K concentration range from 9.9+/-3.6 Bq kg-1 to 298+/-14 Bq kg-1 (av. 130+/-8.12 Bq kg-1). (238)U concentration range from 1.47+/-0.91 Bq kg-1 to 39.5+/-9.9 Bq kg-1 (av. 11.5+/-3.86 Bq kg-1), and 232Th range from 3.50+/-1.85 Bq kg-1 to 10.5+/-2.13 Bq kg-1 (av. 6.78+/-2.13 Bq kg-1). 137Cs was not detected in any of the foodstuffs analysed.     

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).     

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.     

Norm and associated radiation hazards in bricks fabricated in various localities of the North-West Frontier Province (Pakistan).

The activity concentrations of natural gamma-emitting radionuclides and associated radiation hazards due to 40K, 226Ra and 232Th have been measured in baked brick samples, collected from six highly populated areas of the North-West Frontier Province (NWFP) of Pakistan. For the detection, analysis and data acquisition, a high purity germanium (HPGe) detector coupled with a high resolution multichannel analyser (MCA) was used. The range of the average values of the activity concentrations due to 40K, 226Ra and 232Th were found to be 680.3 +/- 22.2-784.4 +/- 30.7 Bq kg(-1), 36.9 +/- 3.5-51.9 +/- 3.3 Bq kg(-1) and 52.5 +/- 3.6-67.6 +/- 3.1 Bq kg(-1), respectively. Radium equivalent (Ra(eq)) activities and various hazard indices were also calculated to assess the radiation hazards. All the brick samples showed Ra, activities within the limit (370 Bq kg(-1)) set by the Organization for Economic Cooperation and Development (OECD) countries. The results of different criterion formulae also complemented each other in this study. The derived data have been compared with the reported values for other countries of the world.     

Radioactive contamination in the marine environment adjacent to the outfall of the radioactive waste treatment plant at ATOMFLOT,northern Russia

RTP "ATOMFLOT" is a civilian nuclear icebreaker base located on the Kola Bay of northwest Russia. The objectives of this study were to determine the distributions of man-made radionuclides in the marine environment adjacent to the base, to explain the form of the distributions in sediments and to derive information concerning the fate of radionuclides discharged from ATOMFLOT. Mean activity concentrations (d.w.) for surface sediment, of 63 Bq kg(-1 137Cs, 5.8 Bq kg(-1) 90Sr and 0.45 Bq kg(-1 239,240)Pu were measured. Filtered seawater activity levels were in the range of 3--6.9 Bq m(-3) 137Cs, 2.0-11.2 Bq m(-3) 90Sr, and 16-40 m Bq m(-3), 239,240Pu. Short-lived radionuclides were present at sediment depths in excess of 10cm indicating a high degree of sediment mixing. Correlations of radionuclide activity concentrations with grain-size appear to be absent; instead, the presence of relatively contaminated sediment appears to be related to the existence of radioactive particles.     

Evaluation of technologically enhanced natural radiation near the coal-fired power plants in the Lodz region of Poland

Radionuclide releases together with escaping fly ashes (from 45 x 10(6) kg in previous decades to 8 x 10(6) kg annually in 1996) from the main local and several small coal-fired power plants resulted in a relatively small increase in natural radioactivity levels in the Lodz region. The natural gamma terrestrial radiation dose rates (1 m above ground level) were measured at 82 points including in the vicinity of power plants, in the center of the town and on edge of the town. The average dose rate value for the first area was 36 +/- 1.2 nGy h (-1), whereas the same dose rate for the edge of town was slightly lower 30 +/- 0.9 nGy h (-1) but this difference was statistically significant. Further confirmation of the technologically slightly enhanced exposure of the local population to natural radionuclides was achieved by gamma-spectrometry measurement of the uranium and thorium decay series radionuclides in the surface soil profiles (up to 30 cm depth). The average increase of 226Ra and 232Th radionuclides in the top layer of soil (0-10 cm) according to the 20+/-30 cm depth layer was 21% and 17%, respectively. However, due to the relatively low levels of 232Th (14.3 Bq kg (-1)) and 238U (16.8 Bq kg (-1)) in this area, the annual average effective dose from the natural terrestrial radiation for the local population is also relatively low, 0.28 mSv only.     

Concentrations of natural radionuclides in imported mineral substances

Levels of natural radionuclides, such as thorium-232 (232Th), radium-226 (226Ra) and potassium-40 (40K), were determined in about 2,000 samples of imported mineral substances using gamma spectrometry. The maximum concentration levels of 232Th, 226Ra and 40K were 1,260 +/- 54, 13,400 +/- 94 and 1,256 +/- 260 Bq kg(-1), respectively, in zirconium compounds. Due to relatively high concentrations of the above-mentioned radionuclides in some imported mineral substances, the National Radiation Protection Department (NRPD), as the competent authority, has established national limits (900 Bq kg(-1) for 232Th, 1800 Bq kg(-1) for 226Ra and 11,000 Bq kg(-1) for 40K), based on the external exposures, for general importation permits of these materials.     

Natural activities of 40K, 238U and 232Th in elephant grass (Pennisetum purpureum) in Ibadan metropolis, Nigeria

Samples of elephant grass collected at some pasturing farmlands across different locations in Ibadan metropolis were analyzed for their natural radioactivity concentrations due to 40K, 238U and 232Th radionuclides. Radioactivity measurements were carried out using gamma-ray spectroscopy. The average radioactivity concentration of 40K was found to be 25.7+/-5.5 Bq kg(-1) for 238U and 33.4+/-3.9 Bq kg(-1) for 232Th. The radiological health implication to the population that may result from these values is found to be very low and almost insignificant. No artificial radionuclide, however, was detected in any of the samples, hence, measurements have been taken as representing baseline values of these radionuclides in the grass in the metropolis.     

Aerial measurements on uranium ore mining, milling and processing areas in Germany

The paper describes aerial measurements at several sites containing residues from uranium mines, waste rock dumps and tailings ponds of the Wismut company in Saxony and Thuringia. For the measurements, a computerized gamma-ray spectrometer equipped with a HPGe-detector and a NaI(Tl)-detector array with a volume of 121 was used. Radioactive anomalies from natural radionuclides have been detected and mapped. The activity concentrations of 226Ra, 228Th and 40K in areas with elevated radioactivity from natural radionuclides were determined from aerial measurements. Ground-based measurements--as far as available--confirmed these results. The mean 226Ra activity concentrations in the different waste rock dumps were found to be in the range 370 to 1600 Bq kg-1. The highest mean 226Ra activity concentrations were measured for the tailings ponds with values up to 1300 Bq kg-1. For 40K and 208Tl, activity concentrations of 860 and 40 Bq kg-1, respectively, were obtained as averages of all measurements. These values are commonly found in the environment. In general, there is reasonable agreement between the results measured with different detectors and measuring methods.     

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.     

Natural radioactivity and dose assessment for phosphate rocks from Wadi El-Mashash and El-Mahamid Mines, Egypt

The activity concentrations of (226)Ra, (232)Th and (40)K have been measured by gamma spectroscopy (sodium iodide NaI(Tl) detector) in phosphate rock samples, collected from the Wadi El-Mashash, a site located in the central eastern desert, and El-Mahamid in the Nile valley, Egypt. The average activity concentrations of (226)Ra, (232)Th and (40)K (Bq kg(-1)) in phosphate rocks were 665.8+/-33.4, 329.4+/-17 and 587.6+/-29.4 for Wadi El-Mashash and 566.8+/-28.6, 217.3+/-11.8 and 560.1+/-28 for El-Mahamid, respectively. The corresponding values for shale rocks were 85.2+/-5.7, 93.3+/-5.6 and 303.1+/-15.2 Bq kg(-1), respectively. As a measure of radiation hazard to the occupational workers and public, the Ra equivalent activities, representative level index and dose rates due to natural radionuclides at 1 m above the ground surface were estimated. The calculated external gamma-radiation dose received by the workers of the phosphate mine are 538 and 418 microSv/y, which is far below the permitted dose of 20 mSv/y recommended by the International Commission of Radiation Protection [ICRP-60, 1990. Radiation Protection: 1990 Recommendation of the International Commission on Radiological Protection, Oxford, Pergamon Preis.] for workers.     

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.     

A model for the bioaccumulation of (99)Tc in lobsters (Homarus gammarus) from the West Cumbrian coast

A biokinetic model is presented that simulates the uptake and release of (99)Tc by the European lobster (Homarus gammarus). This organism is of significant radioecological interest since lobsters, in contrast to most other organisms, have a high affinity for (99)Tc. The model is designed to represent annually averaged (99)Tc concentrations in lobsters from the Cumbrian coast, where significant levels of (99)Tc have been released under authorisation by the nuclear fuel reprocessing plant at BNFL Sellafield.This paper describes the construction of the model, how it was calibrated using data from published literature, and preliminary results indicating that model output agrees well with the available monitoring data. Given that this model successfully combines laboratory and field data, this research could potentially make a significant contribution to the field, as, to date, it has been difficult to predict and explain concentrations of (99)Tc in lobsters.     

Natural radioactivity in farm soil and phosphate fertilizer and its environmental implications in Qena governorate, Upper Egypt

Samples of phosphate fertilizers and farm soils, taken to a depth of up to 30 cm in cultivated land, were collected over the Qena governorate, Upper Egypt. Activity concentration of background radionuclides such as (226)Ra, (232)Th and (40)K of these samples were determined by gamma-ray spectrometry. The results show that these radionuclides were present in concentrations of 366+/-10.5, 66.7+/-7.3 and 4+/-2.6 Bq/kg for phosphate fertilizers. For farm soil and Nile island's soil the corresponding values were 13.7+/-7, 12.3+/-4.6, 1233+/-646 and 11.9+/-6.7, 10.5+/-6.1, 1636+/-417 Bq/kg, respectively. The radium equivalent activity (Ra(eq)), the representative level index, I(gamma r), and absorbed dose in air for all samples were calculated. The data were discussed and compared with those given in the literature.     

Influence of rainfall characteristics on elimination of aerosols of cesium, strontium, barium and tellurium deposited on grassland

This work is aimed at quantifying foliar transfer of cesium, strontium, barium and tellurium under the influence of rainfall characteristics (intensity, frequency and time elapsed between contamination and first rainfall). Grassland boxes were contaminated by dry deposition of multi-element aerosols of (137)Cs, (85)Sr, (133)Ba and (123m)Te. They were grown in a greenhouse under controlled conditions. The treatments consisted of mowing and applying rainfalls (8 and 30 mmh(-1)) at different times after the contamination. At a leaf area index of 5.9+/-1.9, interception of the aerosols was similar for the 4 radionuclides (83.8+/-5.9%). Dew produced significant radionuclide accumulation in the base of the vegetation and transfer to the soil. For moderate intensity, an early (2 days after contamination) first rainfall was as efficient, in terms of leaf wash-off, as a longer rainfall occurring later (6 days after contamination). For early rainfalls, eliminated activities were comparable because the influence of rain intensity was compensated by rain duration. However, for late rainfalls, wash-off efficiency increased with rainfall intensity. Total transfer factors (TTF) were determined on whole grass immediately after 4 rainfalls and at harvest. After 4 medium intensity rainfalls, rain frequency did not influence total transfer factors (TTF) of strontium, barium and tellurium (about 0.2, 0.3 and 0.35 Bq kg(fresh weight)(-1) by Bq m(-2), respectively). Cesium TTF value was lower in the case of a weekly rain (0.1 against 0.2 Bq kg(fresh weight)(-1) by Bqm(-2)). TTF values were similar for twice-a-week rainfalls, whatever their intensity. They were higher for weekly rains of high intensity (between 0.3 and 0.75 Bq kg(fresh weight)(-1) by Bqm(-2) against 0.1-0.35 Bq kg(fresh weight)(-1) by Bq m(-2), depending on the radionuclides). TTF values attested that wash-off was more efficient when rainfalls lasted longer. Field loss on the top of the leaves was well described by an offset exponential model. The half-lives varied with rainfall characteristics from 4 days for cesium, strontium and barium to 20 days for tellurium. The offset value varied between 0% for tellurium (high intensity rainfalls) and 14% for cesium (medium intensity rainfalls).     

Radon flux at King George Island, Antarctic Peninsula

Fluxes of 222Rn from the ice-free terrain to the atmosphere were measured directly, for the first time, at the Brazilian Antarctic Station Ferraz during the summer field campaign of 1998/99. Average value for the flux was 7.7 +/- 4.8 x 10(-2) atoms cm(-2) s(-1) and it ranged between 0.21 x 10(-2) atoms cm(-2) s(-1) and 28 x l0(-2) atoms cm(-2) s(-1). The average flux of 220Rn was estimated to be 23 atoms cm(-2) s(-1), using a combination of two techniques: nuclear track detection and alpha spectrometry of radon daughters. It was found that the production of radon by uranium (41.54 + /-7.17 Bq kg(-1)) and thorium (57.97 +/- 12.14 Bq kg(-1)) equivalent soil contents, and a diffusion coefficient derived from experimental data for the local terrain could account for this average flux. Nevertheless, the large surges of 222Rn in the atmosphere frequently observed for that area could not be explained by this flux only.     

Natural radioactivity and radiation exposure in the high background area at Chhatrapur beach placer deposit of Orissa, India

A high natural background radiation area is reported for the Chhatrapur beach placer deposit of Orissa state, on the southeastern coast of India, due to the presence of radiogenic heavy minerals. The average activity concentrations of radioactive elements 232Th, 238U and 40K were measured by gamma-ray spectrometry using a HPGe detector, and found to be 2500 +/-1850, 230 +/- 140 and 120 +/- 35 Bq kg-1, respectively, for the bulk sand samples. The absorbed gamma dose rates in air due to the naturally occurring radionuclides varied from 375 to 5000 nGy h-1, with an average value of 1625 +/- 1200 nGy h-1. The external annual effective dose rate of the region ranged from 0.46 to 6.12 mSv y-1, with an average value of 1625 +/- 1200 mSv y-1. The absorbed gamma dose rate levels of Chhatrapur beach area were similar to the monazite sand-bearing high background radiation areas of southern and southwestern coastal tracts of India and other similar areas of the world. The major contributors to the enhanced level of radiation are monazite and zircon sands.     

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.     

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.