Reaching environmental levels of 244Pu by accelerator mass spectrometry at the Centro Nacional de Aceleradores.

244Pu (T1/2 = 81 My) is the longest-lived, most minor, and the most understudied Pu isotope. The anthropogenic production of 244Pu is linked to nuclear detonations. Reported 244Pu/239Pu atom ratios in environmental samples range from below 10-6 to above 10-3. This work discusses the performance of the 1 MV Accelerator Mass Spectrometry system at the Centro Nacional de Aceleradores (CNA, Seville, Spain) to analyse 244Pu at environmental levels. The presence of 232Th traces in the Pu sample limits the sensitivity of the technique through the formation of the diatomic trication (232Th12C)3+, of mass 244 u, which must be suppressed by adjusting the stripper gas pressure. A244Pu background of 0.0075 fg (2 × 104 at) is demonstrated for samples that have undergone a chemical treatment. The reliability of the technique is proved through the analysis of three reference sediments provided by the International Atomic Energy Agency (IAEA-412, IAEA-465, IAEA-385). 244Pu results are complemented with 239Pu, 240Pu, 241Pu and 236U and their relative isotopic abundances are discussed.

Fate of anthropogenic radionuclides (90Sr, 137Cs, 238Pu, 239Pu, 240Pu, 241Am) in seawater in the northern Benguela upwelling system off Namibia.

A baseline study on anthropogenic radioactivity in the Namibian marine ecosystem, which is part of the northern Benguela upwelling system, known as one of the most productive ocean areas in the world, has been performed. A scientific cruise carried out in 2014 covering inshore and offshore areas, exhibiting different oceanographic features, has provided a basis for better understanding the distributions, ratios and inventories of six anthropogenic radionuclides (90Sr, 137Cs, 238Pu, 239Pu, 240Pu and 241Am) in seawater. Although 3H was also measured, due to extremely low levels, its behaviour was not studied. The main source of 90Sr, 137Cs, 239Pu, 240Pu and 241Am in the samples analysed was proven to be global fallout, a finding further confirmed by 240Pu/239Pu and 90Sr/137Cs ratios. Furthermore, the 238Pu SNAP-9A satellite accident signal was confirmed once again through the determination of the 238Pu/239+240Pu activity ratio. Inshore and offshore samples showed different patterns due to the unique oceanographic features of this upwelling system. The levels of anthropogenic radionuclides, comprehensively assessed for the first time in this region, are comparable with the few existing data and filled a critical gap for the Southern Atlantic Ocean.

Insights into the Pu isotopic composition (239Pu, 240Pu, and 241Pu) and 236U in marshland samples from Madagascar.

This work provides new insights into the presence of 239Pu, 240Pu, 241Pu, and 236U in the Southern Hemisphere through the study of peat bog cores from marshlands in Madagascar (19°S). 210Pb, 238Pu and 239+240Pu activities were characterized by alpha spectrometry in previous studies. Here, Pu from alpha-spectrometry discs corresponding to 10 peat-bog cores (85 samples) was reassessed for the aim of completing its isotopic composition (239Pu, 240Pu, and 241Pu) by Accelerator Mass Spectrometry. In addition, 236U was studied in a single core exhibiting unusually low 240Pu/239Pu ratios. Integrated 240Pu/239Pu atom ratios in the single cores ranged above and below the (0-30°S) fallout average ratio, 0.173 ± 0.027, from 0.126 ± 0.003 to 0.206 ± 0.002, without a regional pattern, thereby demonstrating the heterogeneous distribution of the 239Pu and 240Pu signal. However, such a variability was not observed for 241Pu/239Pu, ranging from (6 ± 1) · 10-4 to (11 ± 1) · 10-4 and consistently below the (0-30°S) fallout ratio of (9.7 ± 0.3) · 10-4 (2012). The integrated 236U/239Pu atom ratio in the studied core, 0.147 ± 0.005, was also significantly lower than the values reported for the global fallout in the Northern Hemisphere, in the 0.20-0.23 range. Our results point out to stratospheric fallout as the main source of both 236U and 241Pu at the studied site, whereas 239Pu and 240Pu signals show the influence of tropospheric fallout from the low-yield tests conducted in Australia (1952-1958) by United Kingdom and in French Polynesia (1966-1975) by France despite the long relative distances (i.e. about 15,000 and 8500 km). It was also demonstrated that a representative number of samples is necessary in order to assess Pu contamination and its various origins in a specific region in the Southern Hemisphere due to the heterogeneous distribution, and results based on single sample analysis should be interpreted with caution.

Impact of Saharan dust events on radionuclides in the atmosphere, seawater, and sediments of the northwest Mediterranean Sea.

In February 2004, anthropogenic radionuclides (137Cs, 236U, 239Pu and 240Pu), transported from the Sahara Desert, were observed in the Monaco air, and later in water and sediment samples collected at the DYFAMED site in the northwest (NW) Mediterranean Sea. While 236U and 137Cs in Saharan dust particles showed a high solubility in seawater, Pu isotopes were particle reactive in the water column and in the sediment. The impact of the Saharan deposition was found at 0-1.0 cm of the sediment core for 236U and 137Cs, and between 1.0 and 1.5 cm for Pu isotopes. The excess of 236U was observed more in the water column than in the sediment, whereas the 239+240Pu total inventories were comparable in the water column and the sediment. This single-day particle event represented 72% of annual atmospheric deposition in Monaco. At the DYFAMED site, it accounted for 10% (137Cs) and 15% (239+240Pu) activities of sinking particles during the period of the highest mass flux collected at the 200 and 1000 m water depths, and for a significant proportion of the total annual atmospheric input to the NW Mediterranean Sea (28-37% for 137Cs and 34-45% for 239+240Pu). Contributions to the total 137Cs and 239+240Pu sediment inventories were estimated to be 14% and 8%, respectively. The Saharan dust deposition phenomenon (atmospheric input, water column and sediment) offered a unique case to study origin and accumulation rates of radionuclides in the NW Mediterranean Sea.

Excess of (236)U in the northwest Mediterranean Sea.

In this work, we present first (236)U results in the northwestern Mediterranean. (236)U is studied in a seawater column sampled at DYFAMED (Dynamics of Atmospheric Fluxes in the Mediterranean Sea) station (Ligurian Sea, 43°25'N, 07°52'E). The obtained (236)U/(238)U atom ratios in the dissolved phase, ranging from about 2×10(-9) at 100m depth to about 1.5×10(-9) at 2350m depth, indicate that anthropogenic (236)U dominates the whole seawater column. The corresponding deep-water column inventory (12.6ng/m(2) or 32.1×10(12) atoms/m(2)) exceeds by a factor of 2.5 the expected one for global fallout at similar latitudes (5ng/m(2) or 13×10(12) atoms/m(2)), evidencing the influence of local or regional (236)U sources in the western Mediterranean basin. On the other hand, the input of (236)U associated to Saharan dust outbreaks is evaluated. An additional (236)U annual deposition of about 0.2pg/m(2) based on the study of atmospheric particles collected in Monaco during different Saharan dust intrusions is estimated. The obtained results in the corresponding suspended solids collected at DYFAMED station indicate that about 64% of that (236)U stays in solution in seawater. Overall, this source accounts for about 0.1% of the (236)U inventory excess observed at DYFAMED station. The influence of the so-called Chernobyl fallout and the radioactive effluents produced by the different nuclear installations allocated to the Mediterranean basin, might explain the inventory gap, however, further studies are necessary to come to a conclusion about its origin.