Sources and distributions of Cs, Pu, Pu radionuclides in the north-western Barents Sea

Sediment deposits are the ultimate sink for anthropogenic radionuclides entering the marine environment. The major sources of anthropogenic radionuclides to the Barents Sea are fallout from nuclear weapons tests, long range transport from other seas, and river and non-point freshwater supplies. In this study we investigated activity concentrations, ratios, and inventories of the anthropogenic radionuclides, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu in dated sediment cores collected along a north-south transect in the northwestern Barents Sea. The data were used to evaluate the influence of different sources on the derived spatial and temporal patterns of anthropogenic radionuclides in seafloor sediment deposits. Activity concentrations of ¹³⁷Cs ranged from <0.1 Bq/kg to 10.5 Bq/kg while ^239,240Pu ranged from <0.01 Bq/kg to 2.74 Bq/kg and ²³⁸Pu activity concentrations ranged from <0.01 Bq/kg to 0.22 Bq/kg. Total inventories of ¹³⁷Cs ranged from 29.5 ± 1.5 Bq/m² to 152.7 ± 5.6 Bq/m² and for ^239,240Pu inventories (6 sediment layers only) ranged from 9.5 ± 0.3 Bq/m² to 29.7 ± 0.4 Bq/m². Source contributions varied among stations and between the investigated radionuclides. The ²³⁸Pu/^239,240Pu ratios up to 0.18 indicate discharges from nuclear fuel reprocessing plants as a main contributor of plutonium. Based on ²³⁸Pu/^239,240Pu ratio, it was calculated that up to 19-27% of plutonium is supplied from sources other than atmospheric global fallout. Taking into account Atlantic current flow trajectories and that both activity concentrations and inventories of plutonium negatively correlate with latitude, Sellafield is a major source for the Barents Sea. Concentrations and inventories of ¹³⁷Cs correlate positively with latitude and negatively with distance from the Svalbard archipelago. The ¹³⁷Cs concentrations are highest in an area of intensive melting of sea ice formed along the Siberian coast. Thus, sea ice and supplies from Svalbard may be important source of ¹³⁷Cs to the Barents Sea seafloor.     

Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry

Plutonium in Polish forest soils and the Bór za Lasem peat bog is resolved between Chernobyl and global fallout contributions via inductively coupled plasma mass spectrometric measurements of 240Pu/230Pu and 241Pu/239Pu atom ratios in previously prepared NdF3 alpha spectrometric sources. Compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/230Pu and 241Pu/239Pu co-vary and range from 0.186 to 0.348 and 0.0029 to 0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407 x [240Pu/239Pu] - 0.0413; r2 = 0.9924). Two-component mixing models are developed to apportion 239+240Pu and 241Pu activities; various estimates of the percentage of Chernobyl-derived 239+240Pu activity in forest soils range from < 10% to > 90% for the sample set. The 240Pu/230Pu - 241Pu/239Pu atom ratio mixing line extrapolates to estimate 241Pu/239Pu and the 241Pu/239+240Pu activity ratio for the Chernobyl source term (0.123 +/- 0.0007; 83 +/- 5; 1 May 1986). Sample 241Pu activities, calculated using existing alpha spectrometric 239+240Pu activities, and the 240Pu/230Pu and 241Pu/239Pu atom ratios, agree relatively well with previous liquid scintillation spectrometry measurements. Chernobyl Pu is most evident in locations from northeastern Poland. The 241Pu activities and/or the 241Pu/239Pu atom ratios are more sensitive than 240Pu/239Pu or 238Pu/239+240Pu activity ratios at detecting small Chernobyl 239+240Pu inputs, found in southern Poland. The mass spectrometric data show that the 241Pu activity is 40-62% Chernobyl-derived in southern Poland, and 58-96% Chernobyl in northeastern Poland. The Bór za Lasem peat bog (49.42 degrees N, 19.75 degrees E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu.     

Geotrupine beetles (Coleoptera: Scarabaeoidea) as bio-monitors of man-made radioactivity

Adults of the geotrupine beetle Anoplotrupes stercorosus (Coleoptera, Geotrupidae), a common European forest insect species, were used in the role of bio-monitors for mainly man-made radionuclides in a forest environment. Activities of 137Cs, 40K, 238Pu, (239+240)Pu, 90Sr and 241Am were studied. Samples originated from four areas in Poland, two from the north-east and two from the south of the country. The north-eastern areas were previously recognized as the places where hot particle fallout from Chernobyl took place. Results confirmed the differences in the activities between north-eastern and southern locations. Significant correlations were found between activities of 40K and 137Cs, and between activities of plutonium and americium isotopes. An additional study of the concentration of radionuclides within the bodies of beetles showed a general pattern of distribution of radioisotopes in the insect body.     

Plutonium, 137Cs and 90Sr in selected invertebrates from some areas around Chernobyl nuclear power plant

Results are presented for ¹³⁷Cs, ⁹⁰Sr and plutonium activity concentrations in more than 20 samples of terrestrial invertebrates, including species of beetles, ants, spiders and millipedes, collected in the highly contaminated area of the Chernobyl exclusion zone. The majority of samples were collected in Belarus, with some also collected in the Ukraine. Three other samples were collected in an area of lower contamination. Results show that seven samples exceed an activity concentration of 100 kBq/kg (ash weight - a.w.) for ¹³⁷Cs. The maximum activity concentration for this isotope was 1.52 ± 0.08 MBq/kg (a.w.) determined in ants (Formica cynerea). Seven results for ⁹⁰Sr exceeded 100 kBq/kg (a.w.), mostly for millipedes. Relatively high plutonium activity concentrations were found in some ants and earth-boring dung beetles. Analyses of activity ratios showed differences in transfer of radionuclides between species. To reveal the correlation structure of the multivariate data set, the Partial Least-Squares method (PLS) was used. Results of the PLS model suggest that high radiocesium activity concentrations in animal bodies can be expected mainly for relatively small creatures living on the litter surface. In contrast, high strontium activity concentrations can be expected for creatures which conduct their lives within litter, having mixed trophic habits and a moderate lifespan. No clear conclusions could be made for plutonium.     

Sources and pathways of artificial radionuclides to soils at a High Arctic site

Activity concentrations, inventories and activity ratios of ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am in soil profiles were surveyed in the dry tundra and the adjoining proglacial zones of glaciers at a High Arctic site on Svalbard. Vertical profiles of radionuclide activities were determined in up to 14-cm-thick soil sequences. Additionally, soil properties (pH, organic matter, texture, mineral composition and sorption capacity) were analyzed. Results obtained in this study revealed a large range of activity concentrations and inventories of the fallout radionuclides from the undetectable to the uncommonly high levels (inventories of 30,900?±?940, 47?±?6, 886?±?80 and 296?±?19 Bq/m² for ¹³⁷Cs, ²³⁸Pu, ^239?+?240Pu and ²⁴¹Am, respectively) found in two profiles from the proglacial zone. Concentration of these initially airborne radionuclides in the proglacial zone soils is related to their accumulation in cryoconites that have a large ability to concentrate trace metals. The cryoconites develop on the surface of glaciers, and the material they accumulate is deposited on land surface after the glaciers retreat. The radionuclide inventories in the tundra soils, which effectively retain radionuclides due to high organic matter contents, were comparable to the global fallout deposition for this region of the world. The ²³⁸Pu/^239?+?240Pu activity ratios for tundra soils suggested global fallout as the dominant source of Pu. The ²³⁸Pu/^239?+?240Pu and ^239?+?240Pu/¹³⁷Cs activity ratios in the proglacial soils pointed to possible contributions of these radionuclides from other, unidentified sources.     

Traces of DU in samples of environmental bio-monitors (non-flowering plants, fungi) and soil from target sites of the Western Balkan region

This paper reports results of gamma and alpha spectrometric measurements for mosses, lichens, fungi and soil samples from areas in the Balkans targeted by depleted uranium (DU). Samples were collected in 2002 and 2003 in the vicinity of several villages, principally Han Pijesak (Bosnia and Herzegovina, hit by DU in 1995) and Bratoselce (South Serbia, hit by DU in 1999) and in lesser numbers from Gornja Stubla, Kosovo (which is identified as a high natural radon/thoron area) and Presevo close to the Kosovo border. In the course of gamma spectrometric measurements some results suggested samples with unusual high uranium contents which might be considered to be a signature for the presence of DU, although many samples had very high detection limits. Alpha spectrometric measurements directly proved the presence of DU for five samples, all from directly targeted places. These were samples of mosses, lichens and soil. For some samples homogeneity tests were applied which showed a rather even distribution of DU in these samples. No trace of DU was found in any sample from a dwelling.     

Human bones obtained from routine joint replacement surgery as a tool for studies of plutonium, americium and ⁹⁰Sr body-burden in general public

The paper presents a new sampling method for studying in-body radioactive contamination by bone-seeking radionuclides such as ⁹⁰Sr, ^239+240Pu, ²³⁸Pu, ²⁴¹Am and selected gamma-emitters, in human bones. The presented results were obtained for samples retrieved from routine surgeries, namely knee or hip joints replacements with implants, performed on individuals from Southern Poland. This allowed to collect representative sets of general public samples. The applied analytical radiochemical procedure for bone matrix is described in details. Due to low concentrations of ²³⁸Pu the ratio of Pu isotopes which might be used for Pu source identification is obtained only as upper limits other then global fallout (for example Chernobyl) origin of Pu. Calculated concentrations of radioisotopes are comparable to the existing data from post-mortem studies on human bones retrieved from autopsy or exhumations. Human bones removed during knee or hip joint surgery provide a simple and ethical way for obtaining samples for plutonium, americium and ⁹⁰Sr in-body contamination studies in general public.     

Cs and K in fruiting bodies of different fungal species collected in a single forest in southern Poland

Fruiting bodies of fungi belonging to more than 70 species were collected within a few thousand square meter area of one forest during 2006 and 2007. The soil profile was collected to check the cumulative deposition of ¹³⁷Cs, which was relatively high, equal to 64 ± 2 kBq/m² (calculated for October 2006). The majority of this activity was in the first 6 cm. Fruitbodies were analyzed for radiocesium and ⁴⁰K by means of gamma-spectrometry. The highest ¹³⁷Cs activity was 54.1 ± 0.7 kBq/kg (dry weight) for a sample of Lactarius helvus collected in 2006. The results for 2006 were higher than those for 2007. In a few cases the traces of short-lived (T_1/2 = 2.06 a) ¹³⁴Cs were still found in samples. The importance of mycorrhizal fungi for radiocesium accumulation is confirmed. The differences in activity among the species are discussed in relation to observations and predictions from previous studies, where the change in relative accumulation between fruiting bodies of different species was at least partially explained by the differences in the depth of the mycelium localization in a litter/soil system. It is concluded that in some cases, such as Boletus edulis and Xerocomus badius, this prediction is fulfilled and therefore this explanation confirmed.