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.     

Depth profiles of long lived radionuclides in Chernobyl soils sampled around 10 years after the accident

Depth profiles of the long-lived radionuclides, ¹³⁷Cs, ⁹⁰Sr, Pu isotopes and ²⁴¹Am were examined in undisturbed sandy, peaty and Podsol soils in the Chernobyl 30 km exclusion zone sampled around 10 years after the accident. Two Podsol soils, which have different radioactive deposition characteristics, have also been examined. Activity ratios of ^239,240Pu/¹³⁷Cs, ⁹⁰Sr/¹³⁷Cs, and ²⁴¹Am/¹³⁷Cs in the 0-1 cm layer of the two Podsol soils differed very much. Speciation of the radionuclides by sequential selective extraction was examined in the soils. Depth profiles of the soils have been analyzed according to the speciation results and soil characteristics.     

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.     

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.     

Preliminary estimates of cumulative caesium and plutonium deposition in the Irish terrestrial environment

A number of soil and peat cores, sampled throughout Ireland from November 1987 to March 1988, have been analyzed for fallout caesium and plutonium. Specifically,¹³⁴Cs and¹³⁷Cs levels were measured by high resolution gamma spectrometry while²³⁸Pu and^239,240Pu were determined after chemical extraction by alpha spectrometry. The inventories of these nuclides at the locations sampled have been calculated from the resulting profiles and, by extrapolation, preliminary estimates made of the cumulative deposition throughout Ireland. The relative contribution from weapons testing in the atmosphere and the Chernobyl accident to the total caesium inventory have been determined by the¹³⁴Cs/¹³⁷Cs isotopic ratio. As expected, no plutonium of Chernobyl origin was detected in surface layers. The cumulative²³⁸Pu/^239,240Pu ratio measured in Irish soils was found to be consistant with mid-latitude ratios reported by others.     

Study of 137Cs, 90Sr, 239,240Pu, 238Pu and 241Am behavior in the Chernobyl soil

The vertical distribution of ¹³⁷Cs, ⁹⁰Sr, ^239,240Pu, ²³⁸Pu and ²⁴¹Am was determined in soil samples collected from the Chernobyl exclusion zone in 1994. The results show very close distribution profiles for all radionuclides, with about 90% of the total activity of each nuclide lying between the surface and the fourth centimeter. Sequential extraction methods were used to determine the association of radionuclides in soil. The data on vertical distribution of radionuclide species were used to calculate their vertical migration parameters.     

Plutonium isotopes in the surface air in Japan: Effect of Chernobyl accident

Plutonium isotope concentrations in the surface air at Tsukuba, Japan are reported during the period from 1981 to the end of 1986. The^239,240Pu concentration in the surface air, which showed a marked seasonal variation with a spring maximum and fall minimum, decreased until the end of 1985 according to the stratospheric residence time of 1.15 years. In May 1986, elevated^239,240Pu concentrations with high²³⁸Pu/^239,240Pu activity ratios were observed. The serial trend of plutonium concentration in the surface air is similar to the concentrations of the Chernobyl-released radionuclides. These findings suggest that a significant part of the plutonium in the surface air in May 1986 was due to the Chernobyl fallout. The size distribution of plutonium bearing particles indicates that plutonium isotopes were mechanically released in the Chernobyl accident. The surface air concentration of plutonium from the Chernobyl accident was much lower than the concentrations of the volatile fission products, and increased the monthly mean^239,240Pu concentration by only 0.03 Bqm^–3.     

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.     

Contents of238Pu,239,240Pu and137Cs in sediments and shore depositions of the Vltava river in 1995–1996

The²³⁸Pu,^239,240Pu and¹³⁷Cs concentrations in sediments and shore deposition samples of the Vltava river were determined.^239,240Pu and¹³⁷Cs concentrations in sediment samples (five locations) ranged from 19.6 to 124.8 mBq·kg⁻¹ and from 1.8 to 28.2 Bq·kg⁻¹, respectively. The²³⁸Pu,^239,240Pu and¹³⁷Cs concentrations in shore deposition samples (four locations) ranged from 2 to 16.8, from 26.8 to 477.2 mBq·kg⁻¹, and from 1.6 to 86.3 Bq·kg⁻¹, respectively. The superficial activity of studied radionuclides in shore deposition areas was determined and radionuclide origin at studied locations was discussed.     

Regional distribution of Chernobyl-derived plutonium deposition in Finland

The Chernobyl nuclear power plant accident in April 1986 caused a widely spread plume of radionuclides containing, amongst other materials, plutonium isotopes. The regional deposition of these nuclides in Finland has been assessed, based on samples of lichen, peat, precipitation, surface soil and grass. Unlike the deposition of transuranium elements from the weapons tests in the 1950"s and the 1960"s, the deposition in Finland from the Chernobyl accident was very unevenly distributed. Even then, the Chernobyl-derived deposition of ^239,240Pu in the most contaminated regions of Finland was only around 10% of the global fallout from weapons tests. The total amount of ^239,240Pu deposited in Finland was 1^.10¹¹ Bq (»25 g), i.e., approximately half of a percent of the activity deposited in the 1950"s and the 1960"s. In addition to the alpha-emitting Pu isotopes, the Chernobyl plume also contained a significant amount of the beta-emitting ²⁴¹Pu, which is the precursor of the long-lived alpha-emitter ²⁴¹Am. The highest plutonium deposition values were found in a relatively narrow swath from the southwestern coast of Finland northeastwards across the country. This is related to the calculated route of the air parcel trajectory associated with the initial explosion of the Chernobyl reactor. The high deposition values found in the northeastern part of the plume route over Finland can be attributed to the simultaneous occurrence of precipitation. The relatively high plutonium deposition in the southwestern part of Finland occurred, however, without concurrent precipitation. This indicates that the plutonium was at least partly associated with relatively large particles having a substantial deposition velocity due to gravitational setting     

Study on the Horizontal Transport of Some Radionuclides in the Wieprz River Valley

A horizontal transport of radionuclides was studied by the analysis of the radioactivity of the surface soil samples from valleys of Wieprz river and its bottom sediments. Natural gamma-isotopes (⁴⁰K, ²³⁸U and ²³²Th series) antropogenic (¹³⁴Cs and ¹³⁷Cs) and alpha-isotopes ²³⁸Pu and ^239,240Pu were measured. The different kind of bed rock and terrain configuration, influenced the radionuclide transportation from the soil to river bottom sediments. Radioactivity of the sediment samples is definitely lower than the soils. Very strong adsorption of isotopes in soil hinders their horizontal migration. Calculated ²³⁸Pu/^239,240Pu ratio is characteristic for global fallout and about 90% of the ¹³⁷Cs comes from Chernobyl.     

239,240Pu,241Am and137Cs in soils from several areas in China

This paper gives the first data on^239,240Pu and²⁴¹Am in Chinese soils. Surface soil samples with a set of 0–5 cm and 5–20 cm depth were collected from Beijing, Taiyuan, Shijiazhuang and Jinang of China in 1990, and^239,240Pu,²⁴¹Am and¹³⁷Cs, including naturally occurring radionuclides, in these samples were measured to evaluate their present levels and distributions. From these results, the average accumulated depositions were estimated roughly to be 24±13 MBq/km² for^239,240Pu, 10±5 MBq/km² for²⁴¹Am and 1.2±0.7 GBq/km² for¹³⁷Cs. The activity ratios of^239,240Pu/¹³⁷Cs and²⁴¹Am/^239,240Pu ranged from 0.016 to 0.026 with a mean value of 0.020±0.004 and 0.35 to 0.49 with a mean value of 0.43±0.05, respectively.     

Plutonium and cesium isotopes in river waters in Japan

Concentrations of cesium isotopes and plutonium in river water samples in Japan, collected during the period from June 1985 to February 1987, have been measured. The total¹³⁷Cs concentrations in the Japanese river waters ranged from 0.063 to 1.89 mBq·l^–1. The portion of particulate¹³⁷Cs to total was observed to be less than 10 to 35%. The total^239,240Pu concentrations ranged from 0.56 to 1.93 Bq·l^–1. Particulate^239,240Pu occupied 13 to 95% of the total. After the Chernobyl fallout, elevated¹³⁷Cs concentrations were observed in the Japanese river waters as well as the detection of¹³⁴Cs, whereas there was no effect on the river plutonium from the Chernobyl fallout. The partition coefficients of¹³⁷Cs and plutonium between suspended particulate and dissolved phases in the Japanese rivers were determined: from 1.0·10⁴ to 3.2·10⁵ and from 4.1·10⁴ to 2.3·10⁶ for¹³⁷Cs and plutonium, respectively. The result suggests that these radionuclides, especially plutonium, are tightly associated with soil particles and/or suspended matter.     

Scaling model for prediction of radionuclide activity in contaminated soils using a regression triplet technique

A scaling model was built to calculate the activity of alpha emitting radionuclides in contaminated soil in the lysimeter field. Linear regression can be applied for the evaluation of radioactivity measurement data. Activities of the radionuclides ²⁴¹Am, ²³⁸Pu, ^239,240Pu and ⁹⁰Sr obtained by experiments from real contaminated soils of the experimental lysimeter placed in a nuclear power plant (NPP) in Slovakia were evaluated using linear regression models with the method of least squares. A suitable scaling model for monitoring the ²⁴¹Am, ²³⁸Pu, ^239,240Pu alpha radionuclide activity was built using the regression triplet analysis and regression diagnostics. A regular designed scaling model opens the possibilities of longtime activity monitoring of these radionuclides, thus decreasing the number of necessary radiochemical analyses. The Fisher-Snedecor test, however, confirmed that the regression model for ⁹⁰Sr activity monitoring by ²⁴¹Am, ^239,240Pu activity determination in contaminated soils can not be recommended.     

Plutonium isotopes in the surface air at Vinča-Belgrade site in May 1986

Surface air concentrations of plutonium isotopes at the Vinca-Belgrade site for the period May 1–15, 1986, are reported. The increase in²³⁸Pu/^239,240Pu ratios confirms that the source of plutonium in surface air was the Chernobyl accident.     

Natural and anthropogenic radionuclides in the rivers of Azerbaijan

In the frame of an International Atomic Energy Agency Technical Cooperation project, a radiological survey was performed in the Araks and Kura Rivers (Azerbaijan). Sediment samples, and where available, aquatic plants were collected along these two rivers and their inflow and tributary rivers. ¹³⁷Cs, ²³⁸U, ²³⁴U, ^239+240Pu, ²³⁸Pu, ⁹⁰Sr and ²⁴¹Am activity concentrations were measured. The radionuclide levels measured were relatively low, and in most cases below the detection limit, as compared with those from other areas of the world which have been directly affected by effluents from nuclear installations or influenced by the Chernobyl accident. The results indicated that the radionuclides are of natural origin or attributable to the atmospheric fallout from nuclear weapons tests or to the Chernobyl-derived deposition.     

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.     

Distribution of3H,137Cs and239,240Pu in the surface seawater around Korea

The concentrations of³H,¹³⁷Cs and^239,240Pu were determined in surface seawaters collected at 21 sampling stations around Korea from October of 1994 to May of 1995. The results were consistent with the past data observed in the North Pacific. The concentrations of³H and¹³⁷Cs did not show much difference no matter where the samples were taken. Due to the limited distribution of sampling points, no systematic change in³H and¹³⁷Cs levels with latitude was observed. On the other hand,^239,240Pu concentration in the East Sea (Japan Sea) was somewhat higher than that in the South and the Yellow Seas, although the data on^239,240Pu concentration were not enough to explain the reason. The activity ratios of^239,240Pu/¹³⁷Cs in surface seawater ranged from 0.13% to 0.44% with a mean of 0.25±0.08%. The activity ratios were lower than those of the global fall-out level, 1.1%. This result presumably arose from the different behavior of the two radionuclides in seawater.     

Concentration and vertical distribution of plutonium and americium in Italian mosses and lichens

The plutonium and americium concentration and vertical distribution in some Italian mosses and lichens have been determined. The^239,240Pu,²³⁸Pu and²⁴¹Am concentration ranges in tree trunk lichens 0.83–1.87, 0.052–0.154 and 0.180–0.770 Bq/kg, respectively. The corresponding values in tree mosses are higher and more scattered ranging from 0.321 to 4.96, from 0.029 to 0.171 and from 0.200 to 1.93 Bq/kg. The mean²³⁸Pu/^239,240Pu and²⁴¹Am/^239,240Pu ratios are 0.088±0.037 and 0.38±0.13 in lichens and 0.091±0.072 and 0.54±0.16 in tree mosses. The Pu and Am concentrations are relatively low in terrestrial mosses. The^239,240Pu,²³⁸Pu and²⁴¹Am vertical distributions in a terrestrial moss core (Neckera Crispa) collected near Urbino (central Italy) show an exponential decrease with the height. On the contrary the²⁴¹Am vertical distribution in another terrestrial moss core (Sphagnum Compactum) collected in the Alps (northern Italy) shows an interesting peak at 16 cm which corresponds to the deposition of fallout from the nuclear weapon tests in 1960's. The²⁴¹Am movement upward and downward in the moss core is also studied. The results show once again that both mosses and lichens are very effective accumulators of Pu and Am and that they can be used as good biological indicators of the radionuclide airbome pollution from nuclear facilities and nuclear weapon tests. They can play a very impotant role in cycling naturally or artificially enhanced radionuclides in the atmosphere over long time scales.     

Certified reference material for radionuclides in seawater IAEA-381 (Irish Sea Water)

A certified reference material (CRM) for radionuclides in seawater, IAEA-381 (Irish Sea Water), is described and the results of certification are presented. The material has been certified for nine radionuclides (⁴⁰K, ⁹⁰Sr, ¹³⁷Cs, ²³⁷Np, ²³⁸Pu, ²³⁹Pu,²⁴⁰Pu, ^239,240Pu and ²⁴¹Am). Information on massic activities with the corresponding 95% confidence intervals are given for eight radionuclides (³H, ¹²⁵Sb, ²³⁴U, ²³⁵U, ²³⁶U, ²³⁸U, ²⁴¹Pu and ²⁴⁴Cm). Less reported radionuclides include ⁶⁰Co, ⁹⁹Tc, and ²⁴²Pu. The CRM may be used for quality assurance/quality control of the analysis of radionuclides in environmental water samples, for the development and validation of analytical methods and for training purposes. The material is available from the IAEA in 5 kg units.