Exploration of the potential application of plutonium isotopes in source identification of sandstorm in the atmosphere of Beijing

Plutonium (Pu) is an anthropogenic radionuclide which mainly derived from atmospheric nuclear tests in the environment. In this study, the Pu isotopes (²³⁹Pu and ²⁴⁰Pu) in aerosol samples collected during the sandstorm and non-sandstorm period were measured by accelerator mass spectrometry (AMS) and the behavior of Pu was studied. The activity concentrations of ²³⁹Pu and ²⁴⁰Pu in the aerosol samples of Beijing were ranged from 0.62 nBq/m³ to 99.6 nBq/m³ for ²³⁹Pu and 3.51 nBq/m³ to 60.23 nBq/m³ for ²⁴⁰Pu, respectively. ²³⁹Pu and ²⁴⁰Pu concentrations exhibited a remarkable seasonal variation trend, with the higher results showed in spring, and the relatively lower concentrations in winter. The observed higher concentration of ²³⁹Pu and ²⁴⁰Pu detected in sandstorm samples further indicated Pu was closely related to the occurrence of sandstorms. The global fallout characteristics of ²⁴⁰Pu/²³⁹Pu atom ratios (average 0.20, ranging from 0.16 to 0.27) in aerosol samples indicating that global fallout was the major source of Pu in the atmosphere. Using aluminum (Al) as an indicator of soil resuspension, significant positive correlation between ²³⁹Pu and Al (r² = 0.934), ²⁴⁰Pu and Al (r² = 0.525) revealed that soil resuspension was a primary source of atmospheric Pu in Beijing. These results implied that the combination of ²³⁹Pu, ²⁴⁰Pu and Al could be used as the potential tracer of sandstorm.     

Isotopic composition of plutonium immissions in Austria after the Chernobyl accident

Alpha-spectrometric Pu determinations in aerosol samples collected after the Chernobyl accident in Austria show a²³⁸Pu/²³⁹ (240)Pu ratio in the range of 0.33–0.76 with a most reliable value of 0.47. From²⁴¹Am measurements in old Pu preparations and air filter analyses also²⁴¹Pu activities have been calculated. The ratio²⁴¹Pu/^{239 (240)}Pu during the main contamination period is 74.6±5.7, when maximum²⁴¹Pu concentrations in air achieved 4.5–6.0 mBq/m³.     

Gamma-emitters 90Sr, 238,239+240Pu and 241Am in bones and liver of eagles from Poland

Summary The present study focused on analyzing samples of bones, livers and kidneys of European white-tailed eagles (Halia?tus albicilla) and lesser-spotted eagle (Aquila pomarina). Bone samples were collected for both species, from 7 and 2 individuals, respectively, whereas liver and kidney samples for white-tailed eagle species only, 2 and 1 individuals, respectively. The samples were analyzed for the presence of gamma-emitters and then for ⁹⁰Sr, ²³⁸Pu, ^239+240Pu and ²⁴¹Am. The applied radiochemical method is presented. Activity concentration in ashen bones (600 °C) for ⁹⁰Sr ranged from 4.6±1.2 to 31.0±2.5 Bq/kg, for ^239+240Pu from <1.7 to 21±4 mBq/kg, for ²³⁸Pu from <2.7 to 6.5±1.3 mBq/kg and for ²⁴¹Am from <1.2 to 6.5±4.4 mBq/kg. Relatively high ^239+240Pu activity concentration of 78±9 mBq/kg (for fresh weight) was recorded in a single kidney sample. The liver samples showed activities of magnitude at least one order lower. No clear correlations were found between the activities of different radionuclides.     

Radioactivity of plutonium isotopes, <Superscript>137</Superscript>Cs and their ratio in sediment,seawater and biota from the east coast of Peninsular Malaysia

This study with sampling expeditions of marine sediment, seawater and biota were performed at 30 stations within Malaysian Exclusive Economic Zone (EEZ). A total of >400 samples were collected to determine the activity concentration of anthropogenic radionuclides (^239+240Pu, ¹³⁷Cs) and their activity ratio (^239+240Pu/¹³⁷Cs) in sediments, seawater and biota. The purpose of this study was to determine the concentration levels for these radionuclides and to evaluate any occurrence of radioactive contamination. Sediment cores were obtained using multicorer device, while water samples via co-precipitation techniques and biota was purchased from local fishermen. The activity concentrations of ^239+240Pu in sediment, seawater and biota were ranged 0.21–0.45 Bq/kg dry wt., 2.33–7.95 mBq/m³ and <0.008 Bq/kg fresh wt., respectively. Meanwhile, the values of ¹³⁷Cs were ranged <1.00–2.71 Bq/kg dry wt. in sediment, 3.40–5.89 Bq/m³ in seawater and <0.05–0.41 Bq/kg fresh wt. in biota, respectively. Activity ratios of ^239+240Pu to ¹³⁷Cs obtained seem to confirm that these artificial radioactivities were mainly due to global nuclear fallout.     

Behavior and distribution of <Superscript>239+240</Superscript>Pu and <Superscript>241</Superscript>Am in the east coast of Peninsular Malaysia marine environment

The present distributions of ^239+240Pu, ²⁴¹Am and activity ratio of ²⁴¹Am/^239+240Pu in surface seawater of the Peninsular Malaysia east coast were studied. The surface seawater samples were collected at 30 identified stations during the expedition conducted in 2008. ^239+240Pu activity concentrations in surface seawater of the studied area were in the range of 2.33 ± 0.20–7.95 ± 0.68 mBq/m³, meanwhile ²⁴¹Am activity concentrations ranged from MDA to 1.90 ± 0.23 mBq/m³. The calculated activity ratios of ²⁴¹Am/^239+240Pu were varied and disperse distributed with the ranged of 0.12–0.53. The relationships between anthropogenic radionuclide and oceanographic parameters such as turbidity and salinity were examined. The linearly relationships between ^239+240Pu and oceanographic parameters are important for better understanding of its transport processes and behavior in the east coast of Peninsular Malaysia marine environment. Thus, the differ of distribution of ^239+240Pu, ²⁴¹Am and ²⁴¹Am/^239+240Pu in the studied area mainly due to high affinity of ^239+240Pu to associate with sinking particles, mobility nature of ²⁴¹Am, degree of particle reactive of both anthropogenic radionuclides, scavenging and removal process; and others.     

Plutonium Isotopes in Sediments from the Sudanese Coast of the Red Sea

This paper presents the activity concentrations of Pu isotopes in surface marine sediments collected from the Sudanese coast of the Red Sea. The following concentration ranges were determined: ²³⁸Pu, 4.7–28.6 mBq/kg; ^239+240Pu, 53–343 mBq/kg dry weight. The average activity ratios of ²³⁸Pu/^239+240Pu (0.075±0.045 mBqk/kg) and ^239+240Pu/¹³⁷Cs (0.026±0.025 mBq/kg) are appropriately comparable to the literature values that are characteristic of the global fallout from the atmospheric nuclear weapon tests. However, ^239+240Pu/¹³⁷Cs ratio in sediments collected from the biologically rich fringing reef is an order of magnitude higher compared to other sampling locations.     

Vertical profiles of 239+240Pu in seawater from the East China Sea

Seawater samples were collected from the East China Sea continental shelf and analyzed for ^239+240Pu activities. The vertical profiles of ^239+240Pu had a similarity for all three stations in the East China Sea. ^239+240Pu concentrations were low in the surface layer (3-4 mBq/m³) and increased gradually with depth to become high in the near-bottom layer (7-10 mBq/m³). ^239+240Pu concentrations in seawater and the concentrations of suspended particles showed almost the same vertical profiles in the East China Sea continental shelf. The maximum value of ^239+240Pu found in the near-bottom layer may be due to the contribution of Pu-rich suspended particles.     

238Pu, 239+240Pu, 241Am, 90Sr and 137Cs in mountain soil samples from the Tatra National Park (Poland)

Activity concentrations and inventory for ²³⁸Pu, ^239+240Pu, ²⁴¹Am, ⁹⁰Sr, and ¹³⁷Cs in soil from Tatra Mountains of Poland are presented. Soil samples were collected using 10 cm diameter cores down to 10 cm and sliced into 3 slices. Details of the applied procedure are described with the quality assurance program. The maximum activity concentrations found for various samples were: 1782±13 Bq/kg, 17.4±0.9 Bq/kg, 3.4±0.3 Bq/kg and 84±7 Bq/kg for ¹³⁷Cs, ^239+240Pu, ²⁴¹Am and ⁹⁰Sr, respectively. The maximum cumulated deposition of ^239+240Pu is 201±8 Bq/m². The origin of radionuclides is discussed, based mostly on the observed isotopic ratio of Pu. Significant correlations were found between ^239+240Pu, ²⁴¹Am and ¹³⁷Cs. The effective vertical migration rate seems to be in the order of: ⁹⁰Sr≫Pu>Am>Cs.     

240Pu/239Pu atom ratios in the bottom sediments of the NW Pacific Ocean

^239+240Pu concentrations and ²⁴⁰Pu/²³⁹Pu atom ratios in bottom sediments of the Yellow Sea, Korea Strait, East Sea (Sea of Japan), Sea of Okhotsk, and Northwest Pacific Ocean were determined. In coastal sediments near the Korean Peninsula, ^239+240Pu concentrations varied from 0.02 to 1.72 Bq^.kg^-1, and their ²⁴⁰Pu/²³⁹Pu atom ratios from 0.15 to 0.24, with an average of 0.20±0.03. ²⁴⁰Pu/²³⁹Pu atom ratios of bottom sediments in the deep NW Pacific Ocean and its marginal seas (East, Okhotsk seas) were in the range of 0.15-0.23. A little elevated ²⁴⁰Pu/²³⁹Pu atom ratios in the bottom layer sediment may be due to Pu released into the environment during the pre-moratorium period, having high ²⁴⁰Pu/²³⁹Pu atom ratios and low ²³⁸Pu/^239+240Pu activity ratios.     

Simultaneous analysis of 137Cs, 90Sr, 238Pu and 239+240Pu in Brazilian seawater

Methodologies for simultaneous analysis of ¹³⁷Cs, ⁹⁰Sr, ²³⁸Pu and ^239+240Pu were developed and applied to seawater samples. ¹³⁷Cs levels in Brazilian coastal seawater ranged from 0.12 to 4.7 Bq·m^-3, for ⁹⁰Sr from 2.0 to 8.6 Bq·m^-3, for ^239+240Pu from 0.8 to 4.5 mBq·m^-3 and for ²³⁸Pu it was of 1.9 mBq·m^-3. The artificial radioactivity levels in Brazilian seawater are typical values due to fallout deposition.     

Identification of the contamination source of plutonium in environmental samples with isotopic ratios determined by inductively coupled plasma mass spectrometry and alpha-spectrometry

Concentrations of^239+249Pu in environmental samples were detemined by ICP-MS and spectrometry, showing consistent results, which suggests an applicability of ICP-MS to²³⁹Pu and²⁴⁰Pu measurement. The activity ratios of²³⁸Pu/^239+240Pu and²⁴⁰Pu/²³⁹Pu were significantly different in samples from the general environment and near Sellafield reprocessing plants, indicating the usefulness of these ratios for identification of the Pu contamination source.     

Activities of Pu radionuclides and 241Am in soil samples from an alpine pasture in Romania

Activity concentrations of Pu radioisotopes and ²⁴¹Am were determined in the organic and mineral layers of four soil sections collected in 1996, providing for the first time information on the levels of these radionuclides in soil samples from Romania. The investigated site was an alpine pasture located in the Charpathian Mountains, in an area found as one of the most affected in Romania after the Chernobyl accident. In the examined soil sections radioactive inventories were estimated to be 500 Bq/m² for ²⁴¹Pu, 115 Bq/m² for ^239+240Pu, 8 Bq/m² for ²³⁸Pu and 50 Bq/m² for ²⁴¹Am. On the basis of activity ratios in the soil profile, the source of the radioactive release is discussed.     

Inflow of polonium, uranium and plutonium radionuclides in Odra River catchment area assessment by environmetric expertise

The study deals with the application of cluster analysis (CA) and non-parametric tests (Shapiro–Wilk, Kruskal–Wallis, Dunn, U Mann–Whitney) to classify and interpret of a monitoring data set for Odra River water quality assessment based on concentration values of radiochemical parameters. The data set represents results for 3 alpha emitters (²¹⁰Po, ²³⁸U and ^239+240Pu) measured in surface water samples collected at 13 different sampling locations (5 in major Odra stream while 8 in Odra tributaries) within four seasons: winter, spring, summer and autumn, in the framework of 1 year-term quality monitoring research. The correlation analysis of polonium, uranium and plutonium data indicates that significant values of Spearman’s correlation coefficient appears between ²¹⁰Po and ^239+240Pu (r = 0.55 in autumn and 0.77 in winter as well as 0.49 in all year), while statistical significant correlation between uranium and plutonium as well as uranium and polonium were not found. In the Odra drainage basin, the biggest differences were observed in the case of ²³⁸U. The hypothesis about possible geographic and seasonal differences between concentration of ²¹⁰Po, ²³⁸U and ^239+240Pu in the Odra River catchment area was verified by cluster analysis (CA). Finally, to asses if there are statistically significant differences in mean concentration value of ²¹⁰Po, ²³⁸U and ^239+240Pu for Vistula and Odra Rivers drainage basins were obtained by used of the non-parametric tests. Comparing to Vistula catchment area, statistically different concentration of ²¹⁰Po and ^239+240Pu in all year was observed for river samples collected on Odra drainage basin.     

Plutonium in lungs and livers of persons from Chernobyl fallout affected areas in Byelorussia

^239+240Pu and-when possible-also the ratio²³⁸Pu/^239+240Pu was determined in the lungs and livers of 15 residents from Chernobyl-fallout contaminated areas in Byelorussia. In several cases various sections of the lungs were analyzed separately. With the exception of one person the activity concentrations of^239+240Pu, were always within the range expected from the global fallout of weapon tests in the sixties and did not indicate any contribution of Chernobyl-derived plutonium.     

Concentrations of239,240Pu and238Pu in the surface air of Prague in 1993, 1994 and 1995

The activity concentration of^239,240Pu and²³⁸Pu in the surface air of Prague in the years 1993, 1994 and 1995 have been determined. The content of^239,240Pu in air in different monitoring periods of the years studied ranged from <0.5 to 5.5 nBq.m^–3. The source of^239,240Pu in air is the resuspension of fallout plutonium from the opsoil layer.     

239+240Pu and137Cs concentrations in salmon (Oncorhynchus keta) collected on the Pacific coast of Japan

Salmon (Oncorhynchus keta) samples were collected on the Pacific coast of Japan and analyzed for their^239+240Pu and¹³⁷Cs concentrations in six places, i.e., muscle, viscera, gill, gonad, skin and spine. The^239+240Pu concentrations in muscle ranged from 0.07 to 0.14 mBq/kg (wet) and had the lowest value among the six regions. The mean^239+240Pu concentrations in viscera, gonad and spine were more than 1 mBq/kg (wet_ while those in muscle and skin were one order of magnitude lower. The largest amounts of^239+240Pu were accumulated in gonad. The^239+240Pu/¹³⁷Cs activity ratios in all positions were lower than that of the global fallout ratio of 0.022, suggesting that¹³⁷Cs could be accumulated with greater ease than^239+240Pu in all positions and ratios of uptake differed remarkably from position to position. The total accumulations of^239+240Pu and¹³⁷Cs in salmon were 1.32 and 328 mBq/individual, respectively.     

Large volume preconcentration and purification for determining the240Pu/<Superscript>239</Superscript>Pu isotopic ratio and <Superscript>238</Superscript>Pu/<Superscript>239+240</Superscript>Pu alpha-activity ratio in seawater

Summary The present paper describes a new analytical method for determining the ²⁴⁰Pu/²³⁹Pu isotopic ratio and ²³⁸Pu/^239+240Pu α -activity ratio in seawater, both of which are important parameters for determining Pu sources in the ocean. Plutonium isotopes were preconcentrated from a large volume of seawater (4700-10800 liter) by solid phase extraction using MnO₂-impregnated fibers and eluted into 3M HCl. After the elution, the Pu species of all oxidation states were converted to Pu(IV) using NaNO₂, purified by solvent extraction using thenoyltrifluoroacetone (TTA)-benzene, and concentrated in 5 ml of 0.2M HNO₂. The ²⁴⁰Pu/²³⁹Pu and ²³⁸Pu/^239+240Pu ratios in the 5-ml final solution were determined by inductively coupled plasma-mass spectrometry (ICP-MS) and α-spectrometry, respectively. A pg level of Pu, which was a sufficiently large amount for the determination, was obtained by the solid phase extraction. Through the redox conversion and solvent extraction, the Pu species, such as Pu(III), Pu(IV) and Pu(VI), were collected at a high recovery of 96±2% (n=3) despite the presence of large amounts of Mn, and interfering ²³⁸U (3.3 μg^. l^-1in seawater) was effectively removed with a decontamination factor of 1.7·10⁷. The accuracy of the method for the ²⁴⁰Pu/²³⁹Pu ratio was verified using reference materials of seawater and a terrestrial soil sample. The present technique was applied to the determination of the ²⁴⁰Pu/²³⁹Pu and ²³⁸Pu/^239+240Pu ratios in coastal and oceanic water.     

ICP-MS analysis of plutonium activities and <Superscript>240</Superscript>Pu/<Superscript>239</Superscript>Pu ratio in alpha spectrometry planchet deposits

Plutonium isotopes were measured by alpha-spectrometry and ICP-MS in sediment samples from two European lakes: Blelham Tarn in U.K. and Stechlin lake in Germany. The ICP-MS measurements were made after alpha-spectrometry counting of the planchets. The planchets were prepared by traditional electrodeposition method after radiochemical extraction, separation and purification of the Pu fraction. A short radiochemical separation using plutonium selective resin, between the two spectrometry measures, is presented. The results show that these two complementary methods are in good agreement, the plutonium activity concentrations are the same. Alpha-spectrometry allows the ²³⁸Pu determination and ICP-MS individual measurement of ²³⁹Pu and ²⁴⁰Pu. ²³⁸Pu/^239+240Pu and ²⁴⁰Pu/²³⁹Pu ratios are calculated to determine the plutonium contamination source. With the results of these two techniques, it could be demonstrate that the plutonium is of global fallout origin.     

241Pu in the biggest Polish rivers

In the paper the results of ²⁴¹Pu activity concentration determination in the biggest Polish rivers are presented. The analysis of more than 100 river water samples showed the Vistula and the Odra as well as three Pomeranian Rivers are important sources of ²⁴¹Pu in the southern Baltic Sea. There were differences in ²⁴¹Pu activities depending on season and sampling site and the plutonium contamination came mainly from the global atmospheric fallout as well as the Chernobyl accident, which is confirmed by plutonium activity ratios of ²⁴¹Pu/^239+240Pu and ²³⁸Pu/^239+240Pu.     

Simultaneous determination of plutonium and americium in soils by extraction chromatography

A radiochemical method is described for the determination of²³⁸Pu,^239(240)Pu and²⁴¹Am in a single soil sample. Plutonium is separated from a HNO₃ leaching solution by a Microthene-TNOA column; amcricium is coprecipitated by oxalic acid, decontaminated from polonium by a TNOA-column in HCl medium, separated from the rare earth elements by a Microthene-HDEHP column, eluted with a 0.07M DTPA+1M lactic acid solution and finally purified by a PMBP-TOPO extraction. The method supplies a good decontamination of Am and Pu from natural alpha emitters; starting from 50 g soil, the average yields were 75.1±13.4% for plutonium and 57.7±10.8% for Am.^239(240)Pu,²³⁸Pu and²⁴¹Am concentrations (mBq/kg) in three different kinds of soil were the following: 255, 10.4, 81.3 (uncultivated soils); 236, 11.6, 76.7 (cultivated soils); 46, 1.9, 19.8 (river sediment). The average ratios²³⁸Pu to^239(240)Pu and²⁴¹Am to^239(240)Pu were 0.044 and 0.350, respectively.