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A simple and fast radiochemical procedure for the sequential extraction of U, Np and Pu from small-volume seawater samples (<10 L) is presented. The method has been developed and optimized for the final determination of 236U, 237Np, 239Pu and 240Pu by Accelerator Mass Spectrometry (AMS). It is based on the use of 242Pu as tracer for both Np and Pu isotopes. Samples are pre-concentrated by Fe(OH) 2 co-precipitation. TEVA® and UTEVA® resins are used in a very simplified way for the final purification of the Pu+Np and U fractions, respectively. The radiochemical yields of the three elements have been investigated in detail by alpha spectrometry (AS) and gamma spectrometry (GS). The obtained results indicate high and robust chemical yields for the three elements and similar ones for Pu and Np. Furthermore, the use of 242Pu as tracer for 237Np is validated by analyzing a reference seawater sample (IAEA-443) by radiometric techniques. We demonstrated that, if chemicals are properly chosen, processed blank levels can be kept at the same level of the extremely low detection limits that can be achieved by AMS (105–106 atoms/sample). The procedure is finally applied for the study by AMS of a reference seawater sample from the Mediterranean Sea (IAEA-418). fx1 • Sequential extraction of U, Np and Pu from low-volume seawater samples (<10 L). • Specifically designed for the study of 236U, 237Np and 239,240Pu by AMS. • The method is based on the use of 242Pu as tracer for both 237Np and Pu isotopes. • Validated an applied for the study of IAEA-418 (Mediterranean Sea) by AMS. • Processed blanks levels minimized for the analysis of low-level samples. [ABSTRACT FROM AUTHOR]

In this work we present and evaluate a radiochemical procedure optimised for the analysis of 236 U and 239,240 Pu in seawater samples by Accelerator Mass Spectrometry (AMS). The method is based on Fe(OH) 3 co-precipitation of actinides and uses TEVA® and UTEVA® extraction chromatography resins in a simplified way for the final U and Pu purification. In order to improve the performance of the method, the radiochemical yields are analysed in 1 to 10 L seawater volumes using alpha spectrometry (AS) and Inductively Coupled Plasma Mass Spectrometry (ICP-MS). Robust 80% plutonium recoveries are obtained; however, it is found that Fe(III) concentration in the precipitation solution and sample volume are the two critical and correlated parameters influencing the initial uranium extraction through Fe(OH) 3 co-precipitation. Therefore, we propose an expression that optimises the sample volume and Fe(III) amounts according to both the 236 U and 239,240 Pu concentrations in the samples and the performance parameters of the AMS facility. The method is validated for the current setup of the 1 MV AMS system (CNA, Sevilla, Spain), where He gas is used as a stripper, by analysing a set of intercomparison seawater samples, together with the Laboratory of Ion Beam Physics (ETH, Zürich, Switzerland). [ABSTRACT FROM AUTHOR]

The performance of the 1 MV AMS system at the CNA (Centro Nacional de Aceleradores, Seville, Spain) for 236 U and 239,240 Pu measurements has been extensively investigated. A very promising 236 U/ 238 U abundance sensitivity of about 3 × 10 −11 has been recently achieved, and background figures for 239 Pu of about 10 6 atoms were reported in the past. These promising results lead to the use of conventional low energy AMS systems for the analysis of 236 U and 239 Pu and its further application in environmental studies. First 236 U results obtained on our AMS system for marine samples (sediments and water) are presented here. Results of two new IAEA reference materials (IAEA-410 and IAEA-412, marine sediments from Pacific Ocean) are reported. The obtained 236 U/ 239 Pu atom ratios, of 0.12 and 0.022, respectively, show a dependency with the contamination source (i.e. local fallout from the US tests performed at the Bikini Atoll and general fallout). The results obtained for a third IAEA reference material (IAEA-381, seawater from the Irish Sea), are also presented. In the following, the uranium and plutonium isotopic compositions obtained on a set of 5 intercomparison seawater samples from the Arctic Ocean provided by the ETH Zürich are discussed. By comparing them with the obtained results on the 600 kV AMS facility Tandy at the ETH Zürich, we demonstrate the solidity of the CNA technique for 236 U/ 238 U determinations at, at least, 7 × 10 −10 level. Finally, these results are discussed in their environmental context. [ABSTRACT FROM AUTHOR]

The aim of this study was to assess the potential of combining the conservatively behaving anthropogenic radionuclides 236U and 237Np to gain information on the origin of water masses tagged with liquid effluents from Nuclear Reprocessing Plants. This work includes samples collected from three full-depth water columns in two areas: i) the Arctic Ocean, where Atlantic waters carry the signal of Sellafield (United Kingdom) and La Hague (France) nuclear reprocessing facilities; and ii) the western Mediterranean Sea, directly impacted by Marcoule reprocessing plant (France). This work is complemented by the study of the particle-reactive Pu isotopes as an additional fingerprint of the source region. In the Canada Basin, Atlantic waters showed the highest concentrations and 237Np/236U ratios in agreement with the estimated values for North Atlantic waters entering the Arctic Ocean and tagged with the signal of European Nuclear Reprocessing Plants. These results may reflect the impact of the documented releases for the 1990s. In the Mediterranean Sea, an excess of 236U presumably caused by Marcoule is reflected in the lower 237Np/236U ratios compared to the Global Fallout signal in all the studied samples. On the contrary, the 239,240Pu profiles were mainly governed by the Global Fallout. The impact of Marcoule as a local source is further corroborated when comparing the temporal evolution of these ratios between 2001 and 2013. The lowest 237Np/236U ratios observed in 2001 at the surface reflect a previous local input that is no longer observed in 2013 as it had been homogenized through the whole water column. This work presents the use of 237Np as a new ocean tracer. A more accurate characterization of the main sources is still needed to optimize the use of 236U-237Np as a new tool to understand transient oceanographic processes. Unlabelled Image • 236U, 237Np and 239,240Pu investigated in three full-depth water columns by AMS. • Study of two regions impacted by nuclear reprocessing facilities. • Different 237Np/236U ratios in the Arctic Ocean and the Mediterranean Sea. • 240Pu/239Pu: values close to global fallout in both sampling regions. • 237Np 236U dual tracer is investigated as fingerprint to constrain sources. [ABSTRACT FROM AUTHOR]

• 236U and 237Np were studied in Benguela Upwelling System of the South Hemisphere. • Seawater samples collected and analyzed using AMS. • 237Np/236U global fallout ratio in seawater was 1.77 ± 0.20. • 236U and 237Np concentrations at the 106 atoms kg−1 level. • Different 237Np behavior compared to 236U is observed at inshore stations. The Benguela Upwelling System (BUS), off the south-western African coast, is one of the four major eastern boundary upwelling ecosystems in the oceans. However, this area has been overlooked in the field of environmental radioactivity. In this work, 236U and 237Np were collected off the coast of Namibia within the northern BUS. Surface seawater exhibited similar 236U and 237Np concentrations, ranging from 3.9·106 to 5.6·106 atoms kg−1 and from 4.6·106 to 8.5·106 atoms kg−1, respectively. The observed inventories in a water column from the continental margin, of (2.10 ± 0.11)·1012 atoms m−2 for 236U and (3.48 ± 0.13)·1012 atoms m−2 for 237Np, were in agreement with the global fallout (GF) source term in the Southern Hemisphere that was the main source of actinides to the region. A pattern was observed in the surface samples, with 237Np concentrations that decreased by 25–30% when moving from inshore to offshore stations, but such an effect could not be clearly discerned in the case of 236U within the data uncertainties. An explanation based on the larger particle reactivity of GF 237Np compared to GF 236U was proposed. Such an effect would have been important at the studied site due to the enhance presence of particles in the continental shelf triggered by the upwelling phenomenon. A value of 1.77 ± 0.20 was obtained for the 237Np/236U atom ratio for the GF source term in the marine environment. [ABSTRACT FROM AUTHOR]