137Cs, 40K, 90Sr, 238, 239+240Pu, 241Am and 243+244Cm in forest litter and their transfer to some species of insects and plants in boreal forests: Three case studies

Results for ¹³⁷Cs, ⁴⁰K, ⁹⁰Sr, ^238,239+240Pu, ²⁴¹Am and ^243+244Cm measurements in plant, insects and forest litter samples collected at three sites in Poland are presented. New results are compared with some existing data for locations examined during previous studies. Insect samples were introduced now for the first time. Relatively high activities of ⁹⁰Sr were noticed for spruce bark beetle (Ips typographus) and those for ¹³⁷Cs, plutonium and ²⁴¹Am for forest dung beetle (Anoplotrupes stercorosus). Faster than caused by physical decay decrease of radiocesium activity was noticed for the majority of plant and litter samples. The results for ^239+240Pu for litter were similar to previous results, but the activities of ²³⁸Pu were smaller. The activity ratio between ²⁴¹Am and ^239+240Pu was found lower than expected for known proportions between global and Chernobyl fallout. Thus a kind of dynamic behavior of Pu and Am in the forest ecosystem is concluded. Transfer factors and aggregation coefficients were estimated and discussed for both plants and insects as well as between insects and the part of plants (or litter) they feed on. Many of them were never presented before.The authors are thankful to the Polish State Committee for Scientific Research for financial support of this investigation, Grant No. PG04 07520.     

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.     

The Effect of Carbonate Soil on Transport and Dose Estimates for Long-Lived Radionuclides at a U.S. Pacific Test Site

The United States conducted a series of nuclear tests from 1946 to 1958 at Bikini, a coral atoll, in the Marshall Islands (MI). The aquatic and terrestrial environments of the atoll are still contaminated with several long-lived radionuclides that were generated during testing. The four major radionuclides found in terrestrial plants and soils are cesium-137, strontium-90, plutonium-239+240 and americium-241. Cesium-137 in the coral soils is more available for uptake by plants than ¹³⁷Cs associated with continental soils of North America or Europe. Soil-to-plant ¹³⁷Cs median concentration ratios (CR) (kBq·kg^-1 dry weight plant/kBq·kg^-1 dry weight soil) for tropical fruits and vegetables range between 0.8 and 36, much larger than the range of 0.005 to 0.5 reported for vegetation in temperate zones. Conversely, ⁹⁰Sr median CRs range from 0.006 to 1.0 at the atoll versus a range from 0.02 to 3.0 for continental silica-based soils. Thus, the relative uptake of ¹³⁷Cs and ⁹⁰Sr by plants in carbonate soils is reversed from that observed in silica-based soils. The CRs for ^239+240Pu and ²⁴¹Am are very similar to those observed in continental soils. Values range from 10^-6 to 10^-4 for both ^239+240Pu and ²⁴¹Am. No significant difference is observed between the two in coral soil. The uptake of ¹³⁷Cs by plants is enhanced because of the absence of mineral binding sites and the low concentration of potassium in the coral soil. Cesium-137 is bound to the organic fraction of the soil, whereas ⁹⁰Sr, ^239+240Pu and ²⁴¹Am are primarily bound to soil particles. Assessment of plant uptake for ¹³⁷Cs and ⁹⁰Sr into locally grown food crops was a major contributing factor in: (1) reliably predicting the radiological dose for returning residents and (2) developing a strategy to limit the availability and uptake of ¹³⁷Cs into locally grown food crops.     

90Sr, 137Cs, 238Pu, 239+240Pu and 241Am levels in terrestrial and marine ecosystems around the Italian base in Antarctica

During the last 14 years the Radioecology Laboratory of Parma University and the General Chemistry Institute of Urbino University collaborated on a radioecological programme having the aim to observe the evolution of antropogenic radioactivity in Antarctica in the period 1987-2001. The artificial radionuclides considered were ⁹⁰Sr, ¹³⁷Cs, ^239+240Pu,²³⁸Pu and ²⁴¹Am. The contamination seems to be higher in the continental environment rather than in the marine one. Mosses, algae and lichens showed the highest values for all radionuclides analyzed. The results prove that the Antarctic continent is interested by radioactive pollution. As far as ¹³⁷Cs is concerned, a progressive decrease was observed.     

Presence of 137Cs, Pu isotopes and 241Am in ligurian and Tyrrhenian Seas sediments

During the last ten years, the Italian Universities of Parma and Urbino collaborated on a special radioecological program having the aim to study the levels and the distribution of long-lived radionuclides in different marine and terrestrial matrixes. This paper summarizes the results concerning the concentrations of ^239+240Pu and ²³⁸Pu, ²⁴¹Am and ¹³⁷Cs in sediments collected in the Ligurian and South Tyrrhenian Seas (Rapallo Harbour, Vado Ligure Canyon, Eolie Islands). Superficial sediments and sediment cores were collected. For cores the vertical distribution was calculated and the sedimentation rate obtained. ¹³⁷Cs was determined directly by gamma-spectrometry, while ^239+240Pu, ²³⁸Pu and ²⁴¹Am were separated by extraction chromatography, electroplating and determined by alpha-spectrometry. This revised version was published online in August 2006 with corrections to the Cover Date.     

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.     

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, 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.     

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.     

239Pu, 240Pu, 241Pu, 241Am, 137Cs,and 210Pb in seafloor sediments in the western North Pacific Ocean and the Sea of Japan: distributions,sources and budgets

Journal of Radioanalytical and Nuclear Chemistry - Vertical distributions of 239Pu, 240Pu, 241Pu, 241Am, 137Cs, and 210Pb concentrations, and 240Pu/239Pu ratios were determined in seafloor...     

Simultaneous determination of238Pu,239+240Pu,241Pu,241Am,242Cm,244Cm,89Sr,and90Sr in vegetation samples,and application to Chernobyl-fallout contaminated grass

A radiochemical procedure is described for the simultaneous determination of²³⁸Pu,^239+240Pu,²⁴¹Pu,²⁴¹Am,²⁴²Cm,²⁴⁴Cm,⁸⁹Sr, and⁹⁰Sr in vegetation samples. The method was applied for the determination of these, radionuclides in grass, collected near Munich after the fallout from the reactor accident at Chernobyl, USSR. The specific activities observed were (in Bq kg^–1 dry weight):²³⁸Pu, 0.077;^239+240Pu, 0.15;²⁴¹Pu, 3.9;²⁴¹Am, 0.031;²⁴²Cm, 3.0;²⁴⁴Cm, 0.008;⁸⁹Sr, 2000;⁹⁰Sr, 99.     

Sequential separation and determination of plutonium, americium-241 and strontium-90 in soils and sediments

A sensitive and reliable metbod for the sequential separation and determination of plutonium,²⁴¹Am and⁹⁰Sr in soil samples was developed. Plutonium was separated by a Microthene-TNOA column. Then⁹⁰Y (for⁹⁰Sr determination) was separated from americium by a HDEHP column after elimination of large amounts of interfering stable or radioactive nuclides (iron,²¹⁰Bi and²¹⁰Po etc.) by an oxalate precipitation and a Microthene-TNOA column. Finally americium was purified by another HDEHP column and a PMBP-TOPO extraction. A special attention was paid to the decontamination of Pu and Am from²¹⁰Po and of⁹⁰Y from²¹⁰Bi; the relevant decontamination factors resulted greater than 10⁵, 10⁶ and 10⁴ respectively. The detection limits were 1.2 mBq/kg for Pu and 1.7 mBq/kg for²⁴¹Am and 0.32 Bq/kg for⁹⁰Sr. The procedure was checked by analyzing three certified samples supplied by IAEA. Some Italian soil samples were also analyzed giving average yields of 84.9±7.2% for Pu, 57.8±3.2%for Am and 96.7±1.6% for Y; the^239+240Pu,²³⁸Pu,²⁴¹Am and⁹⁰Sr contents (Bq/kg) ranged from 0.347 to 1.53, from 0.013 to 0.048, from 0.126 to 0.556 and from 2.89 to 11.6 respectively and the average ratios were 0.037±0.017 for²³⁸Pu/^239+240Pu, 0.357±0.040 for²⁴¹Am/^239+240Pu and 7.0±1.2 for⁹⁰Sr/^239+240Pu.     

Activity concentration of some anthropogenic radionuclides in the surface marine sediments near the Saudi coast of the Arabian (Persian) Gulf

Activity concentrations of some anthropogenic radionuclides (⁹⁰Sr, ¹³⁷Cs, ²³⁸Pu, ^239+240Pu and ²⁴¹Am) have been measured in the surface of marine sediments along the Saudi coast of the Arabian (Persian) Gulf. The samples were collected at different locations and water depths. The spatial distribution of the concentrations of the measured radionuclides showed a heterogeneous pattern and is independent of location or water depth. The obtained results are discussed and some conclusions are drawn.     

Plutonium, 90Sr and 241Am in human bones from southern and northeastern parts of Poland

The paper presents the results of our study on ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Am and ⁹⁰Sr concentration in human bones carried out on a set of 88 individual samples of central Europe origin. Bone tissue samples were retrieved under surgery while introducing hip joint implants. The conducted surgeries tend to cover either southern or northeastern parts of Poland. While for the southern samples only global fallout was expected to be seen, a mixed global and Chernobyl fallout were to be reflected in the others. Alpha spectrometry was applied to obtain activity concentration for ²³⁸Pu, ^239+240Pu, ²⁴¹Am, while liquid scintillation spectrometry for ⁹⁰Sr and mass spectrometry to receive ²⁴⁰Pu/²³⁹Pu mass ratio. Surprisingly enough, and to the contrary to our expectations we could not see any significant differences in either Pu activity or Pu mass ratio between the studied populations. In both populations Chernobyl fraction proved marginal. The results on ⁹⁰Sr and ²⁴¹Am confirm similarities between the two examined groups.     

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.     

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.     

Evaluation of 239+240Pu, 137Cs and natural 210Pb fallout in agricultural upland fields in Rokkasho, Japan

The background distributions of ^239+240Pu and ¹³⁷Cs fallout in agricultural soil were investigated in Rokkasho where Japan's first commercial nuclear fuel reprocessing plant is now being constructed. The mean inventories of ^239+240Pu and ¹³⁷Cs in three fields with non-yam-cultivation history were 116 Bq·m⁻² and 3.4 kBq·m⁻², respectively. The mean atomic ratio of ²⁴⁰Pu/²³⁹Pu for all studied fields was 0.18±0.04, and was similar to that of global fallout. The ^239+240Pu concentrations correlated very well with ¹³⁷Cs (r = 0.97) in spite of heavy disturbance of the soil, and the activity ratio of ^239+240Pu/¹³⁷Cs was 0.037±0.007, which is a typical value for global fallout. These results showed that the nuclides had similar behavior in agricultural upland fields in Rokkasho. Since ²¹⁰Pb is steadily deposited from the atmosphere to the land, this nuclide could be an index for the degree of disturbance of a field and of soil lost from the field. The ratio of excess ²¹⁰Pb inventory in the soil to the equivalent inventory of atmospheric ²¹⁰Pb deposition was 96%, and indicated that soil was not lost from the cultivated fields. This revised version was published online in July 2006 with corrections to the Cover Date.     

Radioanalytical approach to determine 238Pu, 239+240Pu, 241Pu and 241Am in soils

The simultaneous determination of multiple actinide isotopes in samples where total quantity is limited can sometimes present a unique challenge for radioanalytical chemists. In this study, re-determination of ²³⁸Pu, ^239+240Pu, and ²⁴¹Am for soils collected and analyzed approximately three decades ago was the goal, along with direct determination of ²⁴¹Pu. The soils had been collected in the early 1970’s from a shallow land burial site for radioactive wastes called the Subsurface Disposal Area (SDA) at the Idaho National Lab (INL), analyzed for ²³⁸Pu, ^239+240Pu, and ²⁴¹Am, and any remaining soils after analysis had been archived and stored. We designed an approach to reanalyze the ²³⁸Pu, ^239+240Pu, and ²⁴¹Am and determine for the first time ²⁴¹Pu using a combination of traditional and new radioanalytical methodologies. The methods used are described, along with estimates of the limits of detection for gamma-and alpha-spectrometry, and liquid scintillation counting. Comparison of our results to the earlier work documents the ingrowth of ²⁴¹Am from ²⁴¹Pu, and demonstrates that the total amount of ²⁴¹Am activity in these soil samples is greater than would be expected due to ingrowth from ²⁴¹Pu decay.     

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.     

Inventories of 239+240Pu, 137Cs, and excess 210Pb in sediment cores from brackish Lake Obuchi, Rokkasho Village, Japan

The aim of this study was to measure the distribution and inventories of ^239+240Pu, ¹³⁷Cs, and excess ²¹⁰Pb (²¹⁰Pb_excess) in sediment core samples from brackish Lake Obuchi, which is in the vicinity of nuclear fuel facilities in Rokkasho Village, Japan. The inventory of the ^239+240Pu activity in the sediment samples from the estuary of a freshwater river, the central point of the lake, and the deepest point in the lake were 0.18, 0.29, and 0.24 kBq·m^–2, respectively. The inventories of ¹³⁷Cs and ²¹⁰Pb_excess in sediments were 0.83–1.2 kBq·m^–2 and 25–30 kBq·m^–2, respectively. The mean ^239+240Pu/¹³⁷Cs and ²¹⁰Pb_excess/¹³⁷Cs activity ratios were 0.23 and 28, respectively. The^239+240Pu/¹³⁷Cs activity ratios were approximately 13–24 times the ratio expected from global fallout. The inventories of ^239+240Pu and ²¹⁰Pb in sediments were higher than the inventory expected from atmospheric fallout, but the ¹³⁷Cs inventory was significantly lower than expected.This revised version was published online in November 2005 with corrections to the Cover Date.