An estimate of the inventory of technetium-99 in the sub-tidal sediments of the Irish Sea.

Published results from earlier studies have provided indications that measurable quantities of technetium-99 ((99)Tc) have accumulated in the sub-tidal sediments of the Irish Sea. This is due to the enhanced discharges from the Sellafield nuclear reprocessing plant in Cumbria, UK (between 1994 and 2004). Depth distributions of (99)Tc concentrations in sub-tidal sediments have been determined from a limited number of Irish Sea sites, following the collection of deep sediment cores (up to 2 m in depth), sampled in two research cruise surveys in 2005 and 2006. Vertical concentration profiles of (99)Tc from a range of substrates in the Irish Sea are presented here and these have been used to produce an estimate of the total inventory of (99)Tc residing in the sub-tidal sediments of the Irish Sea. Significant variation was observed between (99)Tc concentrations in the sediment samples, as well as in the shape of individual depth profiles. As anticipated, concentrations tended to be greater on fine-grained (muddy) substrates and showed a general decrease with distance from Sellafield. Vertical concentration profiles of (137)Cs, and (137)Cs data from published work, have also been considered to evaluate the use of the relatively few (99)Tc core data (upon which to determine the (99)Tc inventory). The inventories of (99)Tc and (137)Cs are estimated to have been of the order of 30 and 455 terabecquerels (TBq), respectively, or ∼2% of the total cumulative Sellafield discharge for each of the two radionuclides. The residence half-time of (137)Cs in the sub-tidal sediments of the Irish Sea is estimated to be in the order of ∼16 years. Therefore, as the Kd values for (99)Tc and (137)Cs are similar, this also provides an indicative value to predict future losses of (99)Tc from the sediment reservoir.

Solid-solution partitioning of plutonium in surface waters at the Atomic Weapons Establishment Aldermaston (UK).

The Atomic Weapons Establishment (AWE) at Aldermaston (Berkshire, UK) has provided and maintained the warheads for the UK's nuclear deterrent for more than 50 years. Whilst the site is radiologically safe, in a few locations the soil contains specific activities of plutonium (Pu) above background arising from a legacy of historic operations. Run-off water (a mixture of rainwater and groundwater) from part of the site is routed into a water management system, and after analysis and radiological assessment, released into local streams. Water and sediment samples have been collected from a number of closely spaced locations within this system to assess the solid-solution partitioning of Pu. Survey work was complemented by batch type desorption experiments to assess redissolution from 'contaminated' sediment into 'uncontaminated' water. The survey data indicate that specific activities of both dissolved and particle bound 239 + 240Pu varied by roughly two orders of magnitude, ranging from approximately 0.7 microBq kg(-1) up to approximately 44 microBq kg(-1), and approximately 1.2 Bq kg(-1) up to approximately 400 Bq kg(-1), respectively, consistent with water originating from different parts of the site. Apparent Kd values varied by an order of magnitude (from 0.7-16 x 10(6)) with an average value of 4 x 10(6). Results from the desorption experiments indicated the extent of redissolution was very small and the derived Kd's corroborated values obtained from the survey work. Kd's given here are compared with other literature values, and are the greatest reported to date. Results are also provided describing the variation in water quality parameters in shallow groundwater samples. Alkalinity values ranged from 120 to 388 mg l(-1) CaCO3 with an average value of 195 mg l(-1) CaCO3. Corresponding values for pH were 6.6-8.3 with an average of 7.5. Over half of the samples were estimated to be supersaturated with respect to calcite. It is suggested that the state of calcite saturation may be responsible for the high Pu Kd. As a consequence of the high particle reactivity, migration of Pu contamination, both within and away from the AWE Aldermaston site, is likely to be very restricted.

Application of a magnetic extraction technique to assess radionuclide-mineral association in Cumbrian shoreline sediments.

An assessment has been made of the association of (239+240)Pu, 241Am and 210Po (in secular equilibrium with 210Pb) with iron minerals using a magnetic extraction technique. Grab samples of beach sand from the Cumbrian (UK) coastline were subjected to successive extractions with an approximately 0.1 T ferrite magnet and an approximately 0.3 T rare-earth magnet procedure to separate magnetic iron oxide minerals. Radionuclide concentrations in the magnetic extracts were enhanced (by approximately 4-6-fold) relative to the residue. Those in the approximately 0.1 T magnet extracts were broadly similar to those in the antiferromagnetic material extracted by the approximately 0.3 T magnet, despite the very large differences in magnetic property values between the two fractions (one to two orders of magnitude). The percentage of magnetic material in terms of mass was small and therefore, the majority of these radionuclides (on average 88%) were associated with the residue. Removal of stable Fe was incomplete. Given that the radionuclides may also bind to paramagnetic (nonmagnetic) Fe minerals, the data were extrapolated by normalising the results to quantitative Fe removal. This yielded average values of 37%, 45% and 46% for (239+240)Pu, 241Am and 210Po(210Pb), respectively, as upper limits for the fraction associated with magnetic + nonmagnetic Fe minerals. There are significant uncertainties inherent in quantifying data from this extraction technique. Nevertheless, it seems reasonable to conclude that radionuclide association with Fe minerals is unlikely to have a significant impact upon the physical dispersion of sediment contaminated by Sellafield discharges in the Irish Sea. However, it may be an important factor in governing Pu redox and redissolution behaviour.

Modelling 99Tc concentrations in Fucus vesiculosus from the north-east Irish Sea.

In 1994 there were substantial increases in the quantity of 99Tc discharged into the north-east Irish Sea from BNFL Sellafield (UK), concomitant with improvements in waste treatment procedures. As a consequence, the concentration of 99Tc observed in seawater and biota samples, taken from the Irish Sea coastline, increased significantly. Elevated concentrations were also reported in Dutch, Danish, Norwegian, Swedish and Arctic waters in subsequent years. In the present study a simple numerical model was developed and applied to time-series data of 99Tc concentrations in the brown seaweed Fucus vesiculosus, collected from three UK sites in the vicinity of Sellafield (St. Bees, Heysham, Port William). The model considered site-specific scaling effects, lag times, previous discharge history and potential seasonal variation in uptake. In general, there was a good fit between predicted and observed concentrations, but the degree of uncertainty varied inversely with the frequency of sampling. We did not observe a significant seasonal variation. The modelled lag times to the three sites were consistent with transport times based on observations of the water column distribution of 99Tc. The model was applied to a variety of discharge scenarios, reflecting current discussion on the future management of 99Tc releases. Concentrations in Fucus reached asymptotic values in 3-10 years, depending on the scenario and sampling site under consideration.

Accumulation of technetium-99 in the Irish Sea?

An assessment has been carried out to determine the impact of continued (99)Tc discharges into the Irish Sea from the nuclear fuels reprocessing plant at Sellafield. Samples of surface and bottom seawater and sediment have been collected from the Irish Sea and analysed for (99)Tc. The information has been used, together with supporting data, to determine the effect of summer stratification upon the seawater concentrations and to evaluate whether sediments provide a sink for (99)Tc. Hydrographic data provide clear evidence of thermal stratification of waters above the muddy sediment in the western Irish Sea. Surface water contained higher (99)Tc concentrations than bottom water, and concentrations were inversely related to water salinity. This inverse relationship was not observed in the eastern Irish Sea close to Sellafield. (99)Tc activities in surficial sediments were greatest (>20 Bq/kg) at sites closest to the Cumbrian coastline. Activity, from equivalent sampling sites, remained similar between surveys carried out in 1995 and 1998. The muted response of the seabed sediments, to fluctuations in the Sellafield discharges, compared with the water column is to be expected given that they reflect the integrated radionuclide discharge history.