Browsing by Subject "Plutonium"

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  • Ray, Daisy; Leary, Peter; Livens, Francis; Gray, Neil; Morris, Katherine; Law, Kathleen A.; Fuller, Adam J.; Abrahamsen-Mills, Liam; Howe, John; Tierney, Kieran; Muir, Graham; Law, Gareth T.W. (2020)
    Understanding anthropogenic radionuclide biogeochemistry and mobility in natural systems is key to improving the management of radioactively contaminated environments and radioactive wastes. Here, we describe the contemporary depth distribution and phase partitioning of 137Cs, Pu, and 241Am in two sediment cores taken from the Irish Sea (Site 1: the Irish Sea Mudpatch; Site 2: the Esk Estuary). Both sites are located ~10 km from the Sellafield nuclear site. Low-level aqueous radioactive waste has been discharged from the Sellafield site into the Irish Sea for >50 y. We compare the depth distribution of the radionuclides at each site to trends in sediment and porewater redox chemistry, using trace element abundance, microbial ecology, and sequential extractions, to better understand the relative importance of sediment biogeochemistry vs. physical controls on radionuclide distribution/post-depositional mobility in the sediments. We highlight that the distribution of 137Cs, Pu, and 241Am at both sites is largely controlled by physical mixing of the sediments, physical transport processes, and sediment accumulation. Interestingly, at the Esk Estuary, microbially-mediated redox processes (considered for Pu) do not appear to offer significant controls on Pu distribution, even over decadal timescales. We also highlight that the Irish Sea Mudpatch likely still acts as a source of historical pollution to other areas in the Irish Sea, despite ever decreasing levels of waste output from the Sellafield site.
  • Salminen-Paatero, Susanna; Vira, Julius; Paatero, Jussi (2020)
    The activity concentrations of Pu-238,Pu-239,Pu-240 and Am-241 (for determining its mother nuclide, Pu-241) as well as activity ratios of Pu-238/Pu239+240, Pu-241/Pu239+240 and Pu239+240/Cs-137 and the mass ratio of Pu-240/Pu-239 were determined from air filter samples collected in Rovaniemi (Finnish Lapland) in 1965 to 2011. The origin of plutonium in surface air was assessed based on these data from long time series. The most important Pu sources in the surface air of Rovaniemi were atmospheric nuclear-weapon testing in the 1950s and 1960s, later nuclear tests in 1973-1980 and the SNAP-9A satellite accident in 1964, whereas the influence from the 1986 Chernobyl accident was only minor. Contrary to the alpha-emitting Pu isotopes, Pu-241 from the Fukushima accident in 2011 was detected in Rovaniemi. Dispersion modeling results with the SILAM (System for Integrated modeLling of Atmospheric composition) model indicate that Pu contamination in northern Finland due to hypothetical reactor accidents would be negligible in the case of a floating reactor in the Shtokman natural gas field and relatively low in the case of an intended nuclear power plant in western Finland.
  • Eriksson, Mats; Ämmälä, Kirsi; Levy, Isabelle; Gastaud, Janine; Lehto, Jukka; Scholten, Jan (2019)
    To analyze plutonium (Pu) in open ocean waters can be challenging due to the low seawater concentrations. In this study we compared two techniques for Pu determination, one in-situ MnO2 cartridge system and the more commonly used MnO2 precipitation technique. During the pre-pilot GEOTRACES cruise ANT XXX-1 (2005) we tested MnO2 cartridges for the pre-concentration of Pu from seawater at 19 sampling stations on a transect in the southeastern Atlantic Ocean between Vigo (Spain) and Cape Town (South Africa). Our in-situ sampling setup consisted of one particle cartridge followed by three MnO2 cartridges in a series. Through the system we pumped between 956 and 2700 I of surface seawater with a flow rate between 1.6 and 5.21/min. We found that the adsorption efficiency of a single MnO2 cartridge to adsorb Pu was rather constant and on average a 58 +/- 7%. The adsorption efficiency was also found to be independent of seawater: temperature in the range of 18.3-29.2 degrees C, salinity range 34.2-37.1 parts per thousand, and conductivity in the range of 46.8-58.4 mS/cm. In parallel with the in-situ sampling, discrete surface water samples between 259 and 281 I were taken and Pu was pre-concentrated using the MnO2 precipitation method. We find a good agreement between the Pu concentrations determined with the two different techniques. The in-situ pre-concentration technique requires more radiochemical work in the laboratory but has the advantage that large seawater volumes can be sampled without the necessity for radiochemical processing on-board the ship. The much larger volumes sampled with the in-situ technique compared with the precipitation technique, enables accurate determination of Pu-isotopic ratios with a low relative standard deviation. We have shown in this study that in-situ MnO2 cartridge technique can be used in a reliable way for the determination of dissolved Pu seawater concentration in open ocean waters.
  • Smith, Kurt F.; Morris, Katherine; Law, Gareth T. W.; Winstanley, Ellen H.; Livens, Francis R.; Weatherill, Joshua S.; Abrahamsen-Mills, Liam G.; Bryan, Nicholas D.; Mosselmans, J. Frederick W.; Cibin, Giannantonio; Parry, Stephen; Blackham, Richard; Law, Kathleen A.; Shaw, Samuel (2019)
    Understanding interactions between iron (oxyhydr)oxide nanoparticles and plutonium is essential to underpin technology to treat radioactive effluents, in cleanup of land contaminated with radionuclides, and to ensure the safe disposal of radioactive wastes. These interactions include a range of adsorption, precipitation, and incorporation processes. Here, we explore the mechanisms of plutonium sequestration during ferrihydrite precipitation from an acidic solution. The initial 1 M HNO3 solution with Fe(III)((aq)) and Pu-242(IV)((aq)) underwent controlled hydrolysis via the addition of NaOH to pH 9. The majority of Fe(III)((aq)) and Pu(IV)((aq)) was removed from solution between pH 2 and 3 during ferrihydrite formation. Analysis of Pu-ferrihydrite by extended X-ray absorption fine structure (EXAFS) spectroscopy showed that Pu(IV) formed an inner-sphere tetradentate complex on the ferrihydrite surface, with minor amounts of PuO2 present. Best fits to the EXAFS data collected from Pu-ferrihydrite samples aged for 2 and 6 months showed no statistically significant change in the Pu(IV)-Fe oxyhydroxide surface complex despite the ferrihydrite undergoing extensive recrystallization to hematite. This suggests the Pu remains strongly sorbed to the iron (oxyhydr)oxide surface and could be retained over extended time periods.
  • Paatero, Jussi; Salminen-Paatero, Susanna (2020)
    Following the atmospheric nuclear tests in the '50s and early '60s radioecological research on the (sub)arctic food chain lichen-reindeer/caribou-man was initiated in Finland among other northern countries. The enrichment of radionuclides in this food chain can lead to exceptionally high body burdens among the indigenous Sami and Inuit populations consuming large quantities of the meat and edible organs of reindeer and caribou. In Finland, first fission and activation products and natural radionuclides were studied but in the early 1970s' the investigations concerning transuranium elements were started. These studies have continued to the present as also the effects of the Chernobyl accident on the existence of neptunium, plutonium, americium and curium isotopes in the environment of northern Finland have been investigated. In addition to radioactivity measure-ments detailed dietary surveys were performed among the reindeer herders and other Sami persons to assess the human intake of radionuclides by ingestion. The main aim of this literature review is to summarize the obtained data concerning transuranium elements in the food chain lichen-reindeer-man in northern Finland but also some supporting data is included.