Understanding Radioactive 'Hot' Particle Evolution in the Environment

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Whilst radioactivity has always been present in the environment, industrial and military use of nuclear materials over the past 70 years has led to numerous deliberate and accidental releases of radioactive materials. The impact of these materials on humans and wider ecosystems is controlled by the behaviour of the radionuclides in the environment. In turn, radionuclide behaviour and resultant bioavailability is dictated by their concentration and chemical form.Radioactive 'hot' particles are often an important part of releases to the environment and thus they are commonly found at nuclear sites (e.g. Sellafield) or in areas impacted by deliberate releases (e.g. Ravenglass and Eskmeals, UK) or accidents (e.g. Chernobyl and Fukushima). After release, particle-bound radionuclides have been shown to behave very differently in the environment when compared with homogeneously dispersed contamination. However, there is a distinct lack of knowledge about the composition of, and chemical form of radionuclides in hot particles, or of the processes that control their longer-term stability, fate and impact, particularly at the molecular scale. This leaves significant gaps in our conceptual models of radionuclide environmental behaviour, making it difficult to facilitate robust, long-term predictions of radionuclide transport and fate. Ultimately, the impact of these uncertainties is profound: a lack of confidence in our ability to predict radionuclide behaviour in the environment impacts on the public perception of priority issues, for example, the geological disposal of nuclear waste and the implementation of new nuclear build. As a result, better quantification and understanding of the short- to long-term behaviour and potential impacts of hot particles in the environment is crucial.Reflecting the above, we will use a range of laboratory experiments and field samples combined with state-of-the-art characterisation tools, to develop a clear understanding of hot particle evolution in the environment over timescales ranging from months to decades. The majority of our experimental work will focus on uranium-rich hot particles due to their prevalence in the environment, and we will alter these under a range of environmental conditions in flowing columns, for periods of > 1 year. Throughout, we will monitor changes in solution chemistry; further, we will use a range of synchrotron, mass spectrometry, and electron microscopy techniques to assess changes over time in particle structure, chemistry, and isotopic composition, as well as characterising the formation of any secondary phases. Complementary to our column experiments, and in an effort to understand longer timescale reactions (years to decades) and assess processes across a wider range of particle types, we will use the same techniques to characterise particles from contaminated field samples (e.g. from the Sellafield area and Eskmeals firing range).The information from this work will lead to a much-improved conceptual model of radionuclide behaviour when hot particles are present in the environment. Further, by working with a range of key stakeholders (e.g. EA, DSTL), we can use this knowledge to predict radiological risk at contaminated sites better and inform land management / monitoring practices.