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.     

Determination of137Cs,90Sr and fallout Pu in the volcanic soil of Korea

The cumulative depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic ash soil of Korea were determined. The average accumulated depositions of¹³⁷Cs,⁹⁰Sr and fallout Pu in the volcanic soil were much higher than those in other forest sites of Korea. From depth profiles, it was found that¹³⁷Cs,⁹⁰Sr and^239,240Pu in the volcanic soil are more mobile than those in other forest sites of Korea, and that the downward movement of⁹⁰Sr is faster than¹³⁷Cs and^239,240Pu. A significant correlation was found between the concentration of¹³⁷Cs and those of⁹⁰Sr and^239,240Pu. The activity ratios of²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu in soils are close to those observed in the cumulative deposit from the global fallout of nuclear weapon testings.     

Artificial radioactive contamination of sediment samples along the Romanian sector of the Danube river and the Black Sea coast

The concentrations of¹³⁷Cs were determined by in 11 sediment samples, collected along the Romanian sector of the Danube river and the Black Sea coast during 1994 γ-ray spectrometry. The concentrations of⁹⁰Sr in the same sediment samples were determined by β-counting of the⁹⁰Y oxalate, precipitated after strontium separation using a strontium extraction chromatography column. The concentration distributions of¹³⁷Cs and⁹⁰Sr are compared with the²³⁸Pu and^239,240Pu concentration distributions in the same samples, reported in a previous paper. The accumulation potential of¹³⁷Cs,⁹⁰Sr and plutonium isotopes in the river and sea sediments analysed is discussed.     

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.     

Determination of fission-products and actinides in the Black Sea following the Cherynobyl accident

Radiochemical procedures are discussed for the isolation and determination of a suite of radionuclides in samples from the Black Sea following their input from the Chernobyl reactor accident. The samples analyzed include discrete water samples and both suspended and dissolved phases collected by in-situ chemisorption techniques. The radiochemical scheme permits the separation and analysis of¹³⁴Cs,¹³⁷Cs,⁹⁰Sr,¹⁴⁴Ce,¹⁴⁷Pm,¹⁰⁶Ru,²³⁹Pu,²⁴⁰Pu, and in some instances²⁴²Cm,²³⁸Pu, and²⁴¹Am. The detection techniques employed include various instrumental gamma spectrometric methods, low-level beta counting, alpha spectrometry, and mass spectrometry.The method's developments are described and data are presented on some representative samples from the Black Sea. The sensitivity of the analysis for the various nuclides and sample types is summarized and questions of radiochemical interferences are addressed.     

Geochemical studies on the Chernobyl radioactivity in environmental samples

Artificial radionuclides in deposition and airborne dust samples in 1986 were measured at Tsukuba and 11 stations in Japan. In May 1986, the Chernobyl radioactivity was observed in rain and air samples in Japan. The Chernobyl-derived Pu isotopes, which are characterized by higher²³⁸Pu/^239,240Pu (85) and²⁴¹Pu/²³⁸Pu (0.5) activity ratios than those of the nuclear test-derived Pu and⁹⁰Sr, were detected in deposition and airborne dust samples in Japan, as well as volatile radionuclides such as¹³¹I and¹³⁷Cs. However, the activities of Pu isotopes and⁹⁰Sr observed in Japan were about two and three orders of magnitude lower than those expected from the activity ratios in the total release at Chernobyl, which means that the residence time of Pu in the air was shorter than that of¹³⁷Cs. In order to understand the fractionation between the Chernobyl radionuclides we studied about individual wet and dry deposition. The results suggest that this cause is due to the difference of the particle size of radionuclide-bearing particles, which may be related to the release process of Chernobyl radionuclides.     

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.     

Deposition of90Sr and plutonium isotopes derived from the Chernobyl accident in Japan

To clarify environmental effects of the Chemobyl radionuclides, long-lived Chernobyl radioactivity (^239,240Pu,²³⁸Pu,²⁴¹Pu and⁹⁰Sr) in deposition samples in May 1986 was measured at 11 stations in Japan. Temporal variation of weekly deposition of⁹⁰Sr differed from that of volatile radionuclides such as¹³¹I and¹³⁷Cs, which may reflect the released process at Chernobyl. On the other hand, the geographical distributions of the monthly deposition of long-lived radionuclides were similar to those of volatile radionuclides, in which maximum deposits of⁹⁰Sr and plutonium were observed in Akita, a northwestern Japan Sea coast site of Honshu Island. Higher²⁴¹Pu deposition in most of the stations, as well as high²³⁸Pu/^239,240Pu activity ratios were observed. The²⁴¹Pu/²³⁸Pu activity ratios in deposition samples were nearly equal to that in the total release, which is clear evidence that Chernobyl-derived plutonium was transported to Japan in May 1986 together with volatile radionuclides although the contribution of Chernobyl Pu was about three orders of magnitude lower than¹³⁷Cs.     

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.     

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.     

Determination of90Sr and137Cs in mushrooms following the Chernobyl fallout

After the Chernobyl accident high concentrations of radionuclides were found in Sweden in mushrooms and the contents of⁹⁰Sr and¹³⁷Cs were measured. The level of⁹⁰Sr was generally low and, in proportion to¹³⁷Cs, 2–3 orders of magnitude lower than in the fallut. The contents of¹³⁷Cs varied among species and extreme local variations occurred. The ratio¹³⁴Cs/¹³⁷Cs diverged from other biological samples leading to the conclusion that old fallout was involved in the uptake.     

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.     

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.     

A separation procedure for the analysis of90Sr,154Eu, and the actinides237Np,239Pu,241Am and244Cm

A procedure for the analysis of⁹⁰Sr,¹⁵⁴Eu,²³⁷Np,²³⁹Pu,²⁴¹Am and^242−244Cm was developed. Separation was done with the separating agent, di-2(ethyl hexyl)-phosphoric acid (HDEHP), and results in fractions containing the different elements to be analysed.⁹⁰Sr analysis was done by analysing its daughter nuclide⁹⁰Y, detected through the Cherenkov radiation emitted by this high energy β⁻-emitter.¹⁵⁴Eu was detected using γ-spectrometry with a lower Compton background as a result of the removal of other fission products.²⁴¹Am could also be detected with γ-spectrometry or together with^242−244Cm with α-spectrometry. The long-lived radionuclides²³⁷Np and²³⁹Pu were detected using inductively coupled plasma mass spectrometry (ICP-MS).     

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.     

Selected radionuclides and heavy metals in skeletons of birds of prey from eastern Poland

Results of determination of ¹³⁷Cs, ⁹⁰Sr, ⁴⁰K, ^239+240Pu, and heavy metals: Mn, Zn, Pb, Cd, Ni, Cr, Co, and Cu in skeletons of 15 species of birds of prey from Eastern Poland were presented. The greatest amounts of ¹³⁷Cs and ⁹⁰Sr (70 Bq/kg and 33 Bq/kg, respectively) were found in rough-legged buzzards (Buteo lagopus), winter visitors, coming from former soviet nuclear test places. Concentrations of ^239+240Pu in raptors were negligible, only lesser-spotted eagles (Aquila pomarina) revealed slightly higher values. Median concentrations of ¹³⁷Cs and ⁹⁰Sr in raptors which feed predominantly on small mammals were higher in comparison to concentrations found in other ones preferring different trophy. The most noticeable was a very high lead concentration (reaching above 600 mg/kg) in birds which utilize un-retrieved hunting casualties as their prey.     

Studies of the vertical distribution of134Cs,137Cs,238Pu,239, 240Pu,241Pu,241Am and210Pb in ombrogenous mires at mid-latitudes

Six peat cores taken from three unmodified blanket and raised bogs in Ireland were sectioned and analyzed for a range of radionuclides including¹³⁴Cs,¹³⁷Cs,²³⁸Pu,²³⁹Pu,²⁴¹Am, and²¹⁰Pb.¹³⁴Cs and¹³⁷Cs were measured by high resolution gamma-spectrometry, while the transuranium nuclides were determined after chemical separation by alpha-spectrometry.²⁴¹Pu, present on the electroplated discs together with Pu(), was measured directly by low-level liquid scintillation counting. Core chronologies were established by measuring the unsupported²¹⁰Pb component using low energy photon spectrometry (LEPS). From the resulting profiles, relaxation depths and migration rates for the above mentioned radionuclides have been determined and differences in the values of these parameters interpreted.²³⁸Pu/^239,240Pu and²⁴¹Pu/^239,240Pu ratios have been examined carefully and are discussed in some detail. Finally, the contribution from Chernobyl to the total radiocaesium inventory in each core has been established using the¹³⁴Cs/¹³⁷Cs ratio observed in the initial fallout from Chernobyl.     

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.     

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.     

Pu isotopes and137Cs in the surrounding areas of the former Soviet Union's Semipalatinsk nuclear test site

Field missions were sent to Semipalatinsk City and several settlements near the former Semipalatinsk nuclear test site to investigate the current radioactive contamination levels of the land coming from long-lived radionuclides. The soil was sampled at about 20 sites, including some settlements such as Mostik, Dolon and Chagan, forest and pasture areas, along the roads from Semipalatinsk City to Kurchatov City and to Korosteli settlement in the direction of the Altai District. The radioactivities of¹³⁷Cs,²³⁸Pu and^239,240Pu as well as²⁴⁰Pu/²³⁹Pu atomic ratios in the soil were determined by non-destructive γ-ray spectrometry and radiochemical separation followed by α-ray spectrometry and/or ICP-MS, respectively. The results showed a distinction of¹³⁷Cs and^239,240Pu inventories in soil depending on the site where we visited. While the overall¹³⁷Cs levels were as same as or slightly lower than the domestic global fallout level (3·10³–7·10³ Bq/m²),^239,240Pu levels at some sites were several to a few ten times higher than the domestic level (40–120 Bq/m²). The atomic ratios of²⁴⁰Pu/²³⁹Pu in the soil were in the range of 0.024–0.125, which were significantly lower than the value of 0.18 commonly accepted for global fallout Pu.