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Soil samples collected from locations in Kosovo where depleted uranium (DU) ammunition was expended during the 1999 Balkan conflict were analysed for uranium and plutonium isotopes content (234U, 235U, 236U, 238U, 238Pu, (239 + 240)Pu). The analyses were conducted using gamma spectrometry (235U, 238U), alpha spectrometry (238Pu, (239 + 240)Pu), inductively coupled plasma-mass spectrometry (ICP-MS) (234U, 235U, 236U, 238U) and accelerator mass spectrometry (AMS) (236U)). The results indicated that whenever the U concentration exceeded the normal environmental values (approximately 2 to 3 mg/kg) the increase was due to DU contamination. 236U was also present in the released DU at a constant ratio of 236U (mg/kg)/238U (mg/kg) = 2.6 x 10(-5), indicating that the DU used in the ammunition was from a batch that had been irradiated and then reprocessed. The plutonium concentration in the soil (undisturbed) was about 1 Bq/kg and, on the basis of the measured 238Pu/(239 + 240)Pu, could be entirely attributed to the fallout of the nuclear weapon tests of the 1960s (no appreciable contribution from DU).

Accelerator Mass Spectrometry (AMS) is the analytical technique of choice for the detection of long-lived radionuclides which cannot be practically analysed with decay counting or conventional mass spectrometry. AMS allows an isotopic sensitivity as low as one part in 10(15) for 14C (5.73 ka), 10Be (1.6 Ma), 26Al (720 ka), 36Cl (301 ka), 41Ca (104 ka), 129I (16 Ma) and other long-lived radionuclides occurring in nature at ultra-trace levels. These radionuclides can be used as tracers and chronometers in many disciplines: geology, archaeology, astrophysics, biomedicine and materials science. Low-level decay counting techniques have been developed in the last 40-50 years to detect the concentration of cosmogenic, radiogenic and anthropogenic radionuclides in a variety of specimens. Radioactivity measurements for long-lived radionuclides are made difficult by low counting rates and in some cases the need for complicated radiochemistry procedures and efficient detectors of soft beta-particles and low energy x-rays. The sensitivity of AMS is unaffected by the half-life of the isotope being measured, since the atoms not the radiations that result from their decay, are counted directly. Hence, the efficiency of AMS in the detection of long-lived radionuclides is 10(6)-10(9) times higher than decay counting and the size of the sample required for analysis is reduced accordingly. For example, 14C is being analysed in samples containing as little as 20 microg carbon. There is also a world-wide effort to use AMS for the analysis of rare nuclides of heavy mass, such as actinides, with important applications in safeguards and nuclear waste disposal. Finally, AMS microprobes are being developed for the in-situ analysis of stable isotopes in geological samples, semiconductors and other materials. Unfortunately, the use of AMS is limited by the expensive accelerator technology required, but there are several attempts to develop compact AMS spectrometers at low (< or = 0.5 MV) terminal voltages. Recent advances in AMS will be reviewed with highlights from the scientific programs at Lucas Heights and other AMS centres.

This work provided a novel analytical procedure for rapid and precise uranium isotopic determination in marine sediment and seawater, using a new type of extraction resin, TK200 resin, in combination with microwave digestion (for marine sediments), Fe(OH) 3 co-precipitation (for seawater), and single collector sector field-inductively coupled plasma mass spectrometry (SF ICP-MS) measurement. The removal ability of TK200 extraction chromatography for the interfering elements (IEs) Hg, Pb, Th, Pt, Tl, and the matrix rare earth elements (REEs) was carefully investigated. High decontamination factors (DFs) were obtained for IEs and REEs. Accurate quantification of uranium isotope ratios was accomplished based on a "double-cycle" ICP-MS measurement method. The analytical method was optimized and validated with isotopic standards (IRMM-187), matrix-containing certified reference marine sediments (IAEA-384, IAEA-385, and IAEA-412), and seawater reference material (IAEA-443). A stable chemical recovery of ~ 90% was obtained for both types of marine environmental samples, and the method showed great efficiency with a total analytical time of less than 6 h. The proposed procedure was validated following ISO/IEC 17025 guidelines. The important factors affecting the isotope ratio results (instrument background, procedural blank, memory effects, peak tailing, mass discrimination, dead time, and hydride interferences) were considered in the estimation of combined uncertainties. This work provides an alternative way for the determination of trace uranium isotope ratios and can be applied in the emergency monitoring of nuclear accidents and marine environmental analysis., (© 2023. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)

The Aare river system in Switzerland, with two nuclear power plants on the banks of the river, and its intermediate lakes and reservoirs, provides a unique opportunity to analyze the contribution of different sources to the radioactive contamination. Sediment cores were collected from two lakes and a reservoir, all connected by the river Aare. In order to study the influence of the Chernobyl accident, one sediment core was collected from a lake in the southern part of Switzerland. The sediment cores were sliced and analyzed with gamma ray spectrometry. Plutonium, americium, and uranium were extracted radiochemically, and their concentrations were measured with a sector field ICP-MS. The uranium isotope ratios were further measured with a multi collector ICP-MS. The maximum 137 Cs activity from the Chernobyl accident and the Pu and 137 Cs activities associated to the 1963 global fallout maximum were well identified in sediments from all three lakes. High-resolution records of plutonium isotopes in the zone of the sediments corresponding to the period of maximum fallout from the atmospheric nuclear weapon testing showed distinct fingerprints, depending on the different test activities. Pu isotope ratios could be used to detect non-global fallout plutonium. The ratio 241 Am/ 241 Pu was used to determine the age of the plutonium. Despite of very low 241 Pu and 241 Am concentrations, the calculated plutonium production dates seemed to be reasonable for the sediment layers corresponding to the NWT tests. The calculated production date of the plutonium in the upper most 15 cm of the sediment core seemed to be younger. The reason for this could be additional non-global fallout plutonium. For the lake sediments, natural ratios for 235 U/ 238 U and enriched or depleted ratios for 234 U/ 238 U were measured, depending on the lake. A small increase of the 236 U/ 238 U ratio could be recognized for the NWT zone in all three lakes and, for Lake Lugano, a further distinct increase in the Chernobyl layer., (© 2022. The Author(s).)

The activity concentrations of natural and artificial radionuclides ( 40 K, 232 Th, 226 Ra, 238 U, 137 Cs) and concentrations of six heavy metals of interest (Cd, Cr, Cu, Ni, Pb and Zn) were investigated in 18 soil samples through soil depths (0-10, 10-20, 20-30, 30-40.40-50, 50-60 cm) at the three selected sites in the Hadžići. Since at this area ammunition with depleted uranium had been used during the NATO strikes in 1995, this study was conducted with the aim to assess the radiological and environmental health hazards. Radioactivity was determined by gamma spectrometry using HPGe and LEGE detectors and content of heavy metals by using a flame atomic absorption spectrometry. The correlation with distribution of the radionuclides and their activity concentrations through depths was found only at the site 1 for 40 K, 232 Th and 226 Ra, where minimum/maximum activity concentrations for 40 K were 814.42 Bq/kg/1039.48 Bq/kg, for 232 Th 53.98 Bq/kg/74.12 Bq/kg and for 226 Ra 50.32 Bq/kg/65.73 Bq/kg. Vertical distribution of 137 Cs along 3 site profiles was used for distinction of cultivated and uncultivated soil. Using the activity ratio of 238 U/ 226 Ra and 235 U/ 238 U, the presence of depleted uranium (DU) was established at the site 3. Obtained I geo values for determined heavy metals showed that all of three sites were unpolluted to moderately polluted. Pb content in all three sites showed correlation with concentration decreasing with increasing soil depth., (© 2022. The Author(s), under exclusive licence to Springer Nature Switzerland AG.)

Isotopic ratios of radioactive releases into the environment are useful signatures for contamination source assessment. Uranium is known to behave conservatively in sea water so that a ratio of uranium trace isotopes may serve as a superior oceanographic tracer. Here we present data on the atomic [Formula: see text]U/[Formula: see text]U ratio analyzed in representative environmental samples finding ratios of (0.1-3.7)[Formula: see text]10[Formula: see text]. The ratios detected in compartments of the environment affected by releases of nuclear power production or by weapons fallout differ by one order of magnitude. Significant amounts of [Formula: see text]U were only released in nuclear weapons fallout, either produced by fast neutron reactions or directly by [Formula: see text]U-fueled devices. This makes the [Formula: see text]U/[Formula: see text]U ratio a promising new fingerprint for radioactive emissions. Our findings indicate a higher release of [Formula: see text]U by nuclear weapons tests before the maximum of global fallout in 1963, setting constraints on the design of the nuclear weapons employed.

Abstract: The objective of this study was to evaluate the effect of depleted uranium (DU) on the rat immune system. Three-wk-old, specific pathogen-free Sprague-Dawley rats that received dietary DU for 4 mo were divided into four groups (30 rats per group) according to exposure dose: 0 (control group), 1.3 (DU1.3 group), 13 (DU13 group), and 130 mg U kg-1 (DU130 group). After 4 mo of exposure, the splenic tissues of the rats presented elevated uranium content in accordance with increasing dosage. The rats in the DU130 group exhibited immunological damage characterized by pathomorphological changes of immune organs and significantly lower thymic and splenic relative weight, whereas the influences of DU on the immune system were slight in the other groups. In addition, higher uranium exposure also resulted in reduced numbers of peripheral lymphocytes, lower lymphocyte proliferation, and reduced paw swelling. The authors concluded that the influences of DU on the immune system were slight after ingestion of DU at lower doses but severe after exposure to DU at higher doses., Competing Interests: The authors declare no conflicts of interest., (Copyright © 2013 by the Health Physics Society.)