Distribution of Technetium-99 in sub-tidal sediments of the Irish Sea

Abstract

To date, relatively little attention has been given to the accumulation of 99Tc discharged from Sellafield in the subtidal sediments of the Irish Sea. The potential implications for secondary seafood contamination from contaminated sediment has driven the UK Food Standards Agency to commission further research into this pathway. The work reported here reviews existing data and provides new measurements of 99Tc specific activity in surface and sub-surface sediments of the Irish Sea, together with environmental K d values. The results are used to assess the spatial and temporal evolution of 99Tc in the seabed after 8 years of enhanced Sellafield discharges (between 1994 and 2002), of the aforementioned radionuclide. The information is discussed with reference to other studies, in an attempt to infer the processes controlling 99Tc uptake and release from seabed sediments. The average environmental Kd value for 99Tc in the Irish Sea (1.9×103) was more than an order of magnitude greater than the presently recommended value of 102 [IAEA, 2004. Sediment distribution coefficients and concentration factors for biota in the marine environment. Technical Report Series No. 422, IAEA, Vienna]. Comparison with results from laboratory studies indicates that the observed distribution may represent metastable binding rather than thermodynamic equilibrium. Activities in surface sediments decreased with increasing distance from Sellafield but were also dependent upon the nature of the underlying substrate, being greater on muddy material. Preliminary measurements of grain-size distribution indicated that the observed variation in activities was probably not due to surface area effects. There is an emerging body of evidence from other studies that indicate the differences were most likely due to variations in redox regimes between the different substrates. Vertical profiles were significantly irregular, probably due to the effects of variable sediment mixing processes. Comparison of profiles, close to the Sellafield pipeline, with a core taken over 20 years earlier (pre-EARP) indicated that the increase in the cumulative Sellafield discharge and redissolution from surficial sediment were required to explain the temporal variation. Since the surveys reported here were completed, substantial progress has been made in reducing 99Tc discharges from Sellafield. Assuming that the rate and extent of 99Tc remobilisation follows a similar pattern to that previously observed for caesium (137Cs), then the half-time for redissolution of 99Tc bound to sedimentary material in the Irish Sea is likely to be of the order of several tens of years. It is probable that small but nevertheless measurable 99Tc contamination of local seafood will persist for several decades, due to this secondary source. Crown Copyright © 2006 Published by Elsevier Ltd. All rights reserved