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.     

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.     

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.     

239+240Pu concentrations of sediments and seawater in the coastal sea of Korea

Summary The ^239+240Pu content of the marine sediments and seawater of the costal sea of Korea was measured. In marine sediments the ^239+240Pu concentrations were in the range of 0.11-1.91 Bq/kg dry weight and in the coastal sea of Korea the ratio of ^239+240Pu/¹³⁷Cs was 0.27. The correlations between ^239+240Pu and ¹³⁷Cs concentrations and the content of organic matter (C, O, H, N, S) as well as the grain size of marine sediment were investigated by regression analysis. The distribution coefficient of ^239+240Pu was 1.22^. 10⁵. The ^239+240Pu concentration in seawater increased with seawater depth. However, the ¹³⁷Cs concentration in seawater did not change considerably with depth.     

Development of a bipolar electrolysis system for tritium accumulation in HTO

Due to the different ²⁴⁰Pu/²³⁹Pu atom ratios from different sources of Pu in the environment, Pu isotopes have been widely used for source identification of radionuclides in sediments. In this work, using sector-field ICP-MS, we investigated Pu inventory and its isotopic composition in a lacustrine sediment core collected in Chenghai Lake, SW China. The ²⁴⁰Pu/²³⁹Pu atom ratios in this sediment core ranged from 0.166 to 0.271 with a mean of 0.195±0.021, which was slightly higher than that of global fallout. The ^239+240Pu/¹³⁷Cs activity ratios ranged from 0.0155 to 0.0411, with a mean of 0.0215, and the ^239+240Pu inventory was 35.4 MBq/km²; both ^239+240Pu/¹³⁷Cs activity ratio and Pu inventory were close to those values of global fallout at 20–30 °N. Three peaks were observed for both ¹³⁷Cs and ^239+240Pu activities in the examined sediment core; they most probably indicated the maximum deposition of global fallout between 1963 and 1964, the fallout from a series of Chinese nuclear tests during the 1970s, and the deposition of resuspended Pu-bearing particles from the Chernobyl accident. Therefore, the vertical profile of Pu isotopes should provide useful time markers for rapid dating of recent sediments. These authors contributed equally to this work.     

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.     

Geographical distribution of plutonium derived from the atomic bomb in the eastern area of Nagasaki

In order to know the distribution of plutonium derived from the Nagasaki atomic bomb, soil samples were measured to determine the ²⁴⁰Pu/²³⁹Pu isotope ratio of and concentrations of ^239+240Pu and ¹³⁷Cs. The ^239+240Pu concentrations in soils, except for Nishiyama area, were close to the average concentration of soil collected in Japan. In soils collected at the Nishiyama area and at the eastern area of Nagasaki Prefecture and at part of northern area in Kumamoto Prefecture, the ²⁴⁰Pu/²³⁹Pu ratios were lower than the global fallout values. This suggests that plutonium from the atomic bomb was deposited in the eastern area from the hypocenter reaching up to 100 km eastwards.     

Vertical Profiles, Inventories, and Activity Ratios of 239+240Pu and 137Cs in Sediments from Sagami Bay, Western Northwest Pacific Margin

Marine sediment cores were taken from Sagami Bay of the western Northwest Pacific and analyzed for ^239+240Pu and ¹³⁷Cs activities. A significant correlation was observed between ^239+240Pu and ¹³⁷Cs activities in sediment cores, i.e., their vertical profiles. The measured activities which were used to obtain the inventories of ^239+240Pu and ¹³⁷Cs in the sediment column, showed large variations, ranging from 36 to 474 MBq/km² for ^239+240Pu and 49 to 652 MBq/km² for ¹³⁷Cs. ^239+240Pu inventories in the sediment from one region in the Bay, Sagami Nada were 5–10 times greater than those predicted from atmospheric global fallout 42 MBq/km² at the same latitude. On the other hand, ¹³⁷Cs inventories, with a mean value of 297±168 MBq/km², were much less than predicted, 2040 MBq/km². The activity ratios of ^239+240Pu/¹³⁷Cs obtained, with a mean of 0.65±0.17, were significantly greater than the ratio predicted from fallout, 0.021. Furthermore, there was a clear relationship between both ^239+240Pu and ¹³⁷Cs inventories and the water content, indicating that higher inventories may be attributed principally to concentration in, and scavenging by, fine-grained particles.     

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.     

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.     

The isotopic composition of plutonium in the National Institute of Standards and Technology Standard Reference Material 4351, human lung

The Standard Reference Material 4351 from the National Institute of Standards and Technology is acknowledged to be inhomogeneous. The value of a single analysis for²³⁹Pu+²⁴⁰Pu could lie within a wide range, but the accuracy of the analysis can be corroborated by comparing the corresponding²³⁸Pu/²³⁹Pu+²⁴⁰Pu or²⁴⁰Pu/239Pu values with the relationships between these ratios and the total plutonium concentration.     

Plutonium characteristics in sediments of Hiroshima Bay in the Seto Inland Sea in Japan

Sediment core samples were collected from Hiroshima Bay in the Seto Inland Sea, western Northwest Pacific Ocean, and their ^239+240Pu activities and ²⁴⁰Pu/²³⁹Pu atom ratios were determined by sector field ICP-MS. The activities of ^239+240Pu ranged from 0.556 ± 0.025 to 0.745 ± 0.023 mBq/g. The atom ratios of ²⁴⁰Pu/²³⁹Pu were almost constant within the whole depth; the average value was 0.227 ± 0.014. This atom ratio was significantly higher than the mean global fallout ratio of 0.18, proving the presence of close-in fallout Pu that originated from the Pacific Proving Ground (PPG). The water masses exchanges between the Kuroshio Current and the Seto Inland Sea brought the PPG source Pu to this area, then Pu was extensively scavenged into sediment particles supplied by the rivers around the bay. The relative contributions of the global fallout Pu and the PPG close-in fallout Pu were evaluated by the two end-member mixing model. The contribution of the PPG close-in fallout was 38?C41% of the total Pu in sediment. The remaining 59?C62% was attributed to direct global fallout and the land-origin Pu transported by the rivers around the Hiroshima Bay.     

Study on the rate of plutonium vertical migration in various soil types of Lublin region (Eastern Poland)

Soil contamination level with ^239+240Pu of Lublin region was determined using the alpha spectrometric method. Results were compared with similar data from the study performed 15 year earlier. Decrease in total ^239+240Pu concentration and reducing quantity of Chernobyl fraction (up to almost negligible value of 1 %) has been observed in upper soil layer. Determination of ^239+240Pu concentration in soil profile layers allows calculating a vertical migration velocity of plutonium applying a compartment migration model. It was found that ^239+240Pu migration rate varies depending on soil type from 0.29 cm year^?1 in Podsols to 0.58 cm year^?1 in Fluvisols with mean value of 0.5 cm year^?1.     

Determination of Pu isotopes in sediment cores in the Sea of Okhotsk and the NW Pacific by sector field ICP-MS

Summary Studies on the environmental behavior of plutonium in the marine environment require an analytical method with high sensitivity and capability to provide the isotopic composition of Pu in marine samples. In this work, as part of our on-going project on Pu environmental behavior in the Pacific Ocean, a sector field ICP-MS method combined with an off-line anion-exchange chromatography system was optimized for the determination of Pu and its atomic ratio of ²⁴⁰Pu/²³⁹Pu in sediment core samples. Using a conical concentric nebulizer and 150-second counting time, we were able to lower the detection limit of Pu down to 0.35 fg. The mass discrimination effect was evaluated using a mixed Pu isotope standard solution with certified a ²⁴⁰Pu/²³⁹Pu isotope ratio (NBS-947). The overall performance of the analytical method was validated by the determination of Pu and its isotope composition in an ocean sediment reference material (IAEA-368). Both the ^239+240Pu activity and ²⁴⁰Pu/²³⁹Pu atomic ratio were found to be in good agreement with the certified and/or literature values. As an important application, we employed the analytical method to investigate the vertical profiles of ^239+240Pu activity and ²⁴⁰Pu/²³⁹Pu atomic ratio in sediment cores in the Sea of Okhotsk and the NW Pacific. It was found that the Bikini close-in fallout Pu could be transported as far as the Sea of Okhotsk. The results provided evidence to support our hypothesis on the oceanic current transportation of Bikini close-in fallout Pu in the NW Pacific and its marginal seas.     

Calculation of artificial radionuclides in the ocean by an ocean general circulation model

The concentrations of three artificial radionuclides (⁹⁰Sr, ¹³⁷Cs and ^239+240Pu) introduced into seawaters from global fallout were simulated from 1957 to 1994 by using an ocean general circulation model. The distributions of the calculated ¹³⁷Cs and ⁹⁰Sr concentrations were in good agreement with the observed concentrations. The vertical distribution of the calculated ^239+240Pu concentration in the South Pacific also agreed with the observed data. However, the calculated ^239+240Pu concentrations in the North Pacific water columns were significantly underestimated in comparison with the observed data, which strongly suggests the presence of additional sources of plutonium input to the North Pacific.     

Plutonium concentration and <Superscript>240</Superscript>Pu/<Superscript>239</Superscript>Pu isotopic ratio in the surface soils from the Jiuquan region in northwestern China

Surface soil samples collected in the Jiuquan region in the downwind area of the Chinese nuclear test site (CNTs) were analyzed for Pu isotopes. The ^239+240Pu activities ranged from 0.025 ± 0.009 to 0.89 ± 0.16 mBq g^?1, varying significantly with different sampling sites. The Dunhuang city that is located in the southwestern part of the Jiuquan region received the heaviest Pu deposition (^239+240Pu activities, 0.23–0.89 mBq g^?1). Most of the ²⁴⁰Pu/²³⁹Pu isotopic ratios were similar with that of the global fallout. However, the low values (0.080–0.147) observed in three sampling sites further supported the finding of Pu originated from CNTs in that region.     

Intertidal mangrove mudflat <Superscript>240+239</Superscript>Pu signatures,confirming a <Superscript>210</Superscript>Pb geochronology on the southeastern coast of Brazil

A sediment core was taken to determine if sediment accumulation rates could be conducted using ^240+239Pu signatures in the coastal mangrove mudflats of southeastern Brazil. The results from this study show that ^240+239Pu fallout activities are sufficient and well preserved in the coastal sediments of this region. Sediment accumulation rates determined from the ^240+239Pu signatures were 4.4 mm/year and 4.1 from ²¹⁰Pb (CIC) method. A sediment mixing coefficient rate was calculated using chlorophyll-a profile (9.5 cm²).     

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.     

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.     

Use of combined alpha-spectrometry and fission track analysis for the determination of240Pu/239Pu ratios in human tissue

Plutonium and other actinides were determined in human autopsy tissues of occupationally exposed workers who were registrants of the United States Transuranium and Uranium Registries (USTUR). In this study, Pu was purified and isolated from Am, U and Th, after drying and wet-ashing of the tissues, and the addition of²³⁸Pu as a radiotracer. After electrodeposition onto vanadium planchets the^239+240Pu activity was determined by alpha-spectrometry. A fission track method was developed to determine²³⁹Pu in the presence of²³⁸Pu and²⁴⁰Pu, using Lexan^TM polycarbonate detectors. Combining the two techniques allowed the determination of the²⁴⁰Pu/²³⁹Pu activity and atom ratios. Data from selected USTUR cases are presented.