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.