Areal distribution of 129I in west cumbrian solis

¹²⁹I has been released during operations at the BNFL nuclear fuel reprocessing plant at Sellafield in west Cumbria over the past thirty years with about 95% being discharged into the sea and 5% into the atmosphere. Soil samples have been taken within a 40 km radius of Sellafield to determine the extent to which the ¹²⁹I is deposited in the immediate vicinity of the plant. The ¹²⁹I content has been determined by a sensitive neutron activation technique and levels in soil were found to be elevated above global levels in all samples. The areal distribution of ¹²⁹I was consistent with direct deposition following release to the atmosphere from Sellafield and the relationship between ¹²⁹I activity and the distance from Sellafield was of a form predicted by atmospheric dispersion models. The absence of any observable return of ¹²⁹I from the sea has implications for assessments of dose.     

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).     

Modelling radioactivity in the Irish Sea: From discharge to dose

In order to support authorised discharges of low level radioactive liquid effluent into coastal regions, mathematical models are required to robustly predict radiological impacts on critical groups of current and proposed changes to liquid discharges. The grid model presented here simulates the long term dispersion and transport of radioactivity discharged from the Sellafield site in Cumbria, UK, and the subsequent exposure of critical groups in Cumbria and across the Irish Sea in Northern Ireland. The fine grid of the model allows a good resolution of the seabed sediment distribution. This benefits the predictions for the last decades of low discharge level, when bed sediment can become a source of contamination by bringing back the legacy of past high discharges. This is highlighted by the dose comparison, where the predicted dose to Cumbria critical group follows well the dose estimated from environmental data during the low discharge level period.     

Chemical associations of artificial radionuclides in Cumbrian soils

The distributions of radionuclides in the surface layer of four soils of contrasting types from west Cumbria, UK, have been studied in detail. All the soils contain enhanced levels of artificial radionuclides derived from low-level discharges both to sea and to atmosphere from the British Nuclear Fuels reprocessing plant at Sellafield. The bulk of the activity is held in the top 15 cm of soil profiles, suggesting that radionuclide mobility is limited. Sequential extraction experiments have identified major associations of plutonium with organic matter and of caesium with silicates but there is no preferential association of ruthenium with any single soil component.     

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.     

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.     

Airborne radioactivity on the Scottish Solway coast

A brief survey of the concentrations of radionuclides in surface air at five locations along the Scottish shoreline of the Irish Sea has been made in response to concern that airborne resuspension of marine radioactivity may be causing an inhalation hazard. Airborne concentrations of ⁴⁰K, ¹⁰⁶Ru, ¹³⁷Cs, ¹⁴⁴Ce, ²³⁸Pu, ^{239 + 240}Pu and ²⁴¹Am are reported. Plutonium isotopic ratios indicate the presence of radioactivity of marine origin attributable to low-level waste disposals from the fuel-reprocessing plant at Sellafield in Cumbria. Calculation of the dose resulting from inhalation shows that the risks to members of the public are negligible. Suggestions are made for development of these studies in future.     

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.     

Carbon-14 discharges from the nuclear fuel cycle: 2. Local effects

Environemtnal ¹⁴C levels around various types of nuclear installations within the UK have been monitored during recent years. Enhanced ¹⁴C levels have been detected around both the nuclear fuel reprocessing plant as Sellafield and the thermal nuclear power station complex at Hunterston. From these measurements, the radiological impact of the ¹⁴C discharges on the local population is assessed. It is conservatively estimated that the ¹⁴CO₂ emissions from Sellafield between 1952 and 1985 could have delivered an 8·4 man Sv collective effective dose equivalent commitment to the population living within 40 km of the site. The maximum possible collective dose to the population within 15 km of Hunterston in 1984 was 15 × 10⁻³ man Sv. Conservative estimates of maximum annual effective dose equivalents to individuals around Sellafield and Hunterston are 0·2 mSv (in 1982) and 12 μSv (in 1984), respectively. These dose levels do not exceed the limits recommended by ICRP but the former value clearly indicates that, for the larger discharges at least, consideration and optimisation of ¹⁴C releases are fully justified. The same ¹⁴C measurements are also used to test the validity of two atmospheric dispersion models, the Gaussian plume and the so-called ‘hyperbolic’ models. The former is excellent in predicting downwind ¹⁴C levels around Hunterston but is unsatisfactory when applied to Sellafield, whereas the latter proves reliable at both sites. Further investigations suggest that the Gaussian plume model's poor performance at Sellafield can be explained by inaccurate input data.     

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.     

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.     

Reconstructing the history of 14C discharges from Sellafield: part 1--atmospheric discharges

14C specific activities, above ambient background levels, were determined in individual treerings (corresponding to the years 1950-1999) sectioned from an oak tree that was felled in autumn 1999, from a location 1.5 km east of the Sellafield nuclear fuel reprocessing plant in Cumbria. north-west England. The data were used to produce a new, improved, reconstruction of Sellafield's annual atmospheric 14C discharges between 1951 and 1999, using the most reliable discharge data set (1994-1999) as the primary basis for the determination of a new calibration factor that relates excess 14C activity in individual tree rings to the annual discharge during the corresponding year. The results indicate that the current British Nuclear Fuels plc (BNFL) estimate of total 14C discharges to the atmosphere prior to 1978 is significantly overestimated, while the current estimate of total 14C discharges after 1978 is very similar to that determined in this study. In this study, the total activity of 14C discharged to the atmosphere from Sellafield between 1951 and 1999 is estimated to be 259+/-63 TBq (at 2 std. dev.). The BNFL current estimate is 360TBq.     

An improved and validated dispersion model for the North Sea and adjacent waters

We present a successful attempt to determine transfer coefficients in a compartment model by computer-assisted fitting of simulated compartment contents to measurements. The procedure was applied to a fusion of previously published models of the North Sea and adjacent regions and resulted in an improved and validated model for the dispersion of a conservative effluent from, in particular, Sellafield.     

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.     

Geochemical associations of plutonium and γ-emitting radionuclides in caithness soils and marine particulates

Geochemical associations of plutonium and artificial γ-emitting radionuclides have been investigated in soils and marine particulate material from the immediate vicinity of the Dounreay Nuclear Power Development Establishment (DNPDE) Caithness. The artificial radionuclides present in these materials arise from a variety of sources: world-wide nuclear weapons test fallout, direct deposition from atmospheric discharges at DNPD, and the return to land of activity previously discharged to sea (containing contributions from Dounreay and Sellafield). The levels, although sufficient to permit satisfactorily low counting errors, are of negligible radiological significance, the plutonium being more than 1000 times less than the NRPB Generalised Derived Limit (GDL) for well-mixed soil. Sequential leaching using selective extractants was performed to quantify the percentages of each nuclide in the following notional fractions: (a) readily available, (b) exchangeable and bound at specific adsorption sites, (c) chelated as insoluble organic complexes, (d) associated with sesquioxides, and (e) residual. Plutonium was found to be associated mainly with phases (c) and (d), while the γ-emitters present in the marine particulate material showed quite varied distributions. The degree of chemical fixation in the particulates follows the sequence ⁴⁰K¹³⁷Cs¹⁰⁶Ru¹²⁵Sb^239,240Pu¹⁴⁴Ce⁶⁰Co^154,155Eu.     

Aspects of the uptake of radionuclides by sheep grazing on an estuarine saltmarsh. 1. The influence of grazing behaviour and environmental variability on daily intake

Sea water contaminated with diluted radioactive effluent originating from the Sellafield reprocessing plant inundates saltmarshes in the Esk estuary in west Cumbria (UK). Much of the radioactivity on the saltmarsh vegetation was found to be associated with a surface deposit of silt, brought onto the area during tidal inundation. Large temporal variations in the radionuclide concentrations of the vegetation were found, these being due probably to seasonal fluctuation in the extent of silt deposition.The grazing habits of sheep were studied on one of these saltmarshes and the consequent ingestion of radionuclides by the sheep was estimated. The sheep ingested different quantities of radionuclides according to time of year as a result of a combination of two factors; the considerable temporal variation in the concentration of radionuclides on the saltmarsh vegetation and the seasonal grazing behaviour of the sheep.     

Radioactivity in fossils at the Hagerman Fossil Beds National Monument

Since 1996, higher than background levels of naturally occurring radioactivity have been documented in both fossil and mineral deposits at Hagerman Fossil Beds National Monument in south-central Idaho. Radioactive fossil sites occur primarily within an elevation zone of 900-1000 m above sea level and are most commonly found associated with ancient river channels filled with sand. Fossils found in clay rich deposits do not exhibit discernable levels of radioactivity. Out of 300 randomly selected fossils, approximately three-fourths exhibit detectable levels of natural radioactivity ranging from 1 to 2 orders of magnitude above ambient background levels when surveyed with a portable hand held Geiger-Muller survey instrument. Mineral deposits in geologic strata also show above ambient background levels of radioactivity. Radiochemical lab analysis has documented the presence of numerous natural radioactive isotopes. It is postulated that ancient groundwater transported radioactive elements through sand bodies containing fossils which precipitated out of solution during the fossilization process. The elevated levels of natural radioactivity in fossils may require special precautions to ensure that exposures to personnel from stored or displayed items are kept as low as reasonably achievable (ALARA).     

Development and application of marine gamma-ray measurements: a review

The development of instruments to measure gamma radiation in the marine environment, particularly on the sea floor, and the range of uses to which they have been put is reviewed. Since the first steps in the late 1950s, systems have been developed in at least 10 countries with the main thrust occurring in the 1970s. Development has continued up to the present, primarily in Europe and the USA. Marine gamma-ray spectrometers have been used for a range of applications including the mapping of rocks and unconsolidated sediments, mineral exploration (mainly for heavy minerals and phosphorites), sediment transport studies and investigations in relation to discharged and dumped nuclear wastes and at nuclear weapon test sites.     

Radioactivity of the soil in Vojvodina (northern province of Serbia and Montenegro)

The widespread public belief that during the bombardment of Vojvodina (Yugoslavia) this region was contaminated by depleted uranium has recently raised public concern with respect to the potential contamination of agricultural products due to soil radioactivity. Based on the gamma-spectrometric analysis of 50 soil samples taken from the region of Vojvodina we concluded that there is no increase of radioactivity that could endanger the food production. Taking into account the transfer factors of 137Cs to plants, the measured activity concentrations of this isotope should not endanger the health safety of the produced food. No traces of depleted uranium have been found. The natural radioactivity levels are compared with the results form other countries.     

Plutonium in sheep faeces as an indicator of deposition on vegetation

In order to study the deposition on vegetation of plutonium arising from the testing of nuclear weapons and discharges from nuclear facilities, sheep faeces were collected from the South-west and North of England. The plutonium content of faeces has been shown to be a reproducible and sensitive indicator of deposition on herbage and, with this technique, plutonium discharged from the Sellafield Works of British Nuclear Fuels LImited can be detected 60 km from the site. On moorland pastures the concentration of ^239+240Pu in faeces, expressed as activity per gram of ash, is roughly equal numerically to the deposit of plutonium on 1 m² of vegetation.Some of the plutonium ingested by a grazing sheep is absorbed and the highest concentrations are found in liver. The liver of a sheep grazing on pasture where the ^239+240Pu concentration in faeces was about 2 pCi (74 mBq) g⁻¹ of ash, was found to contain <1% of the Generalised Derived Limit for mutton and offal, and the meat <0·001%.