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.     

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.     

Observation of111Ag and110mAg in the Chernobyl fallout

Evidence for the presence of¹¹¹Ag in Chernobyl fallout at Monaco is given. This fission radionuclide has not been previously reported in Chernobyl fallout. Peak values were as high as 1.9 Bq m^–3. Arguments are presented that the observed^110mAg content in the fallout originated from volatilisation of silver neutron flux monitors in the reactor rather than production by other nuclear reactions.     

Pilot measurements of <Superscript>237</Superscript>Np in forest litter from Poland

Described are results and the procedure for a pilot study on ²³⁷Np content in forest litter samples from Poland in relation to their plutonium activity. Neptunium was determined by inductively coupled plasma mass spectrometry (ICP-MS) and Pu by alpha spectrometry. Two samples originated from a location with pure global fallout and two others from a place with about 65% of the plutonium from Chernobyl. Plutonium activities were determined twice: at Krakow and in Monaco. The two results were consistent and ^239 + 240Pu activities ranged from about 1 to about 7 Bq/kg dry weight (dw). The chemical recovery for Np was between 27 and 89%. Results for ²³⁷Np activity concentrations were between 0.099 ± 0.005 and 2.21 ± 0.076 mBq/kg dw. Observed activity ratios were lower than expected and could be explained by fractionation of Np against Pu in forest litter.     

Measurement of radiocesium in Irish peatland soils

Results are presented for soils taken from twelve peatland sites in Ireland. Two depth horizons, 0–5 and 5–15 cm, were sampled on each site and sampling was carried out in summer and autumn. Deposition of Chernobyl¹³⁷Cs varied between 0.4 and 4.6 kBq m^–2, which is at the lower end of values reported by other authors for Irish agricultural soils. The data showed that the relative percentages of activity and deposition remained internally consistent in each soil horizon for Chernobyl and weapons fallout sources on both sampling occasions: this provided evidence that sampling and analytical procedures were consistent. An apparent reversal in the relative importance of weapons fallout in soils was found when deposition data were compared to the same data presented in activity format, and this same reversal was found for both soil horizons. Different conclusions may erroneously be drawn from data depending on the parameter by which we make measurements. Presentation of results should be carefully considered and depends on the purpose for which a study is intended. A statistically significant change in bulk density of the deeper soil horizon was found between summer and autumn. Changes in bulk density important to bear in mind that in addition to analytical errors, sampling methods can only provide estimations which themselves have inherent sources of error.     

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.     

Fallout from Chernobyl in Bologna and its environs: Radioactivity in airborne,rain water and soil

The Chernobyl fallout was estimated in Emilia-Romagna, a Northeastern region of Italy. Nuclide composition of airborne and the time evolution of the radioactivity were investigated. The comparison of the activity ratio of¹⁰³Ru to¹³⁷Cs allows to conclude that Italy was not influenced by the first release. The trend of the total activity and¹³⁷Cs percentage in rain water was very similar to those of air particulates. A calculation model to estimate¹³⁷Cs deposition onto the ground has been developed and validated by comparison of the calculated and experimental values for soil samples. The activity range was 2–40 kBq ·m^–2.     

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.     

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     

Migration of plutonium isotopes in forest soil profiles in Lublin region (Eastern Poland)

The distribution of Pu isotopes in three profiles of forest soil in Lublin region was determined. The retention half-time and migration velocity of^239,240Pu originated from global and Chernobyl fallouts was calculated. The average rate of migration of the global fallout plutonium was 0.4 cm/year and that of the Chernobyl one 0.7 cm/year. Good correlation between Pu concentration and organic matter contents was found only in the case of podzolic soil profile. In two profiles a good negative correlation between Pu activity and exchangeable pH of the soil layer was determined.     

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.     

Simultaneous determination of plutonium and americium in biological and environmental samples

A radiochemical method is given to determine the specific activity of²³⁸Pu, and²⁴¹Am from the global fallout in environmental and biological samples. The radiochemical recovery was for human livers Pu: 60–70%, Am: 40–60%; Bran: Pu: 50–70%, Am: 30–40%; Soil: Pu: 50–80%, Am: 30–50%. The resolution of the alpha-spectrum was for soils 30–40 keV and for livers and brans 40–60 KeV. To facilitate the wet ashing of large amounts of bran (15 kg), which are necessary to determine the presently very small activity concentrations of the transuranic elements in these types of samples, a fermentation process was employed. The procedure was tested by using NBS standard reference material and subsequently applied for the determination of Pu and Am from the global fallout in livers, plant tissues (bran), and soils.     

On peculiarities of vertical distribution of 239,240Pu, 238Pu and 137Cs activity concentrations and their ratios in lake sediments and soils

Distributions of ^239,240Pu, ²³⁸Pu and ¹³⁷Cs activity concentrations in the cores of sediments in the shallow lake, flooded and upland forest soils taken in the vicinity of Vilnius city were analyzed. The radiochemical, α-spectrometric and mass spectrometric methods were used for the plutonium evaluation and γ-spectrometry was used for the radiocesium evaluation. The only peak of enhanced radionuclide activity concentrations was determined for the lake bottom sediments, whereas vertical profiles of the radionuclide activity concentrations in flooded and upland forest soil cores were distinguished by two peaks. The obtained values of the activity concentration ratio ²³⁸Pu/^239,240Pu and the isotopic ratio ²⁴⁰Pu/²³⁹Pu indicated that the global fallout was a source of plutonium in the investigated environment. Chernobyl-derived radiocesium was detected solely in the surface layers (2–11 cm) of the studied sample cores. The contribution of the Chernobyl deposits amounted to about 2.26, 6.11 and 20.9 % of the total radiocesium inventory in the bottom sediments, the upland soil and flooded soil, respectively.     

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.     

Fallout of transuranium elements following the Chernobyl accident

The deposition of transuranium elements in Sweden following the Chernobyl accident was investigated through the analysis of carpets of lichen-and moss-samples and also air-filters and precipitation. The impact of transuranium elements was small compared to that of radiocesium. The deposition of^239+240Pu was, as for other actinides, inhomogeneously distributed and ranged from 0.1% to 100% of the inventory in 1986 from nuclear detonation tests. The activity ratio of^239+240Pu/¹³⁷Cs was between 10^–3 and 10^–6 in comparison to 10^–2 for nuclear test fallout. The activity ratios of²⁴¹Pu,²⁴²Cm,²³⁸Pu,^243+244Am and^239+240Pu were about 86, 14, 0.47, 0.14, and 0.13 respectively, but large variations were observed. The results from Sweden were compared with those found in South Finland, Denmark and Southern Europe. The deposition over Scandinavia originated from the initial explosion at Chernobyl, which contained relatively higher amounts of actinide elements than the second emission, which occurred a few days later and was a result of actions taken to bring the fire under control.     

Leaching of glass components and surrogate nuclides from glassy waste forms for radioactive incineration ash

Three kinds of soil, collected in various places (in northwestern and southeastern Poland and near Chernobyl) were used as a subject of sequential extraction and plutonium distribution study. The modified method of Tessier was applied to separate readily available, carbonate, organic, Fe/Mn oxide and residual fractions. Plutonium isotope activity in soil as well as in particular separated fractions was determined by means of alpha spectrometry. The method of plutonium separation and purification for alpha-spectrometric measurements was modified according to the chemical properties of the extracted fraction. It was found that the major part (about 90%) of ^239,240Pu is bound to organic and Fe/Mn oxide fractions (in uncultivated soil samples of northwestern Poland and Chernobyl). In soil samples coming from river valley (southeastern Poland) almost equal amounts of plutonium are distributed between the available, organic and residual fractions.     

Origin and release date assessment of environmental plutonium by isotopic composition

The origin and release date of environmental plutonium have been assessed by the measurement of plutonium and americium isotopic composition. The applicability and sensitivity of different plutonium isotope ratios, ²⁴⁰Pu/²³⁹Pu and ²⁴¹Pu/²³⁹Pu measured by inductively coupled plasma sector field mass spectrometry and ²³⁸Pu/²³⁹Pu analysed by alpha spectrometry, have been evaluated for origin determination in several types of environmental samples. With use of mixing models the contribution of different sources (e.g. global fallout or Chernobyl) can be calculated. By the measurement of the ²⁴¹Am/²⁴¹Pu isotope ratio, the release date (i.e. formation of ²⁴¹Pu by irradiation) can be estimated in environmental samples, which is an important parameter to distinguish recent plutonium release from previous (e.g. Chernobyl) emissions.     

Determination of237Np in large volume samples of sea water by a radiochemical procedure

A radiochemical procedure followed by alpha spectrometry has been developed for the determination of²³⁷Np present at low activity concentrations in seawater. The analytical procedure is based on concentration of actinides from 1800 1 sea water samples by hydroxide precipitations. Neptunium is isolated by ion exchange, fluoride precipitation and extraction with TTA (thenoyltrifluoroacetone). As a radiochemical yield determinant²³⁹Np or²³⁵Np is used. Neptunium is electroplated onto stainless steel discs before alpha-spectrometry for about 10 days. The procedure allows for sequential separation of plutonium, americium, technetium and radiocaesium together with neptunium. The radiochemical yield for neptunium is only 20–50%, but the procedure has been applied with success on several samples contaminated with²³⁷Np at fallout or close to fallout levels.     

Determination of strontium-90 in various kinds of water after Chernobyl accident in Austria

As a consequence of the reactor-accident of Chernobyl on Tuesday 29 April 1986 the environmental radioactivity in Austria increased for above the level recorded before. Depending on the amount of precipitation the deposition of radioactive fallout showed great differences. Many water samples /rain water, lake water, swimming pool water, drinking water, underground water/ collected /during period of April 29 to May 30/ from Vienna, Lower Austria and Steiermark were analyzed for⁹⁰Sr. The following concentrations in /nCi 1^–1/ of⁹⁰Sr was found: 8.69±2.3 for rain water, 0.09±0.12 for lake water, 0.08–0.18 for swimming pool, 0.04–0.13 for drinking water, 0.07–0.2 for underground water. The⁹⁰Sr concentration was not higher than the maximal permissible /0.004–0.4 nCi 1^–1/ except for rain water.     

Procedures and findings of examination of air contamination by alpha-active plutonium aerosols: Primary and secondary products of Chernobyl accident

Atmospheric contamination pattern by Pu-radionuclides over a 30 km zone of the Chernobyl nuclear power plant in 1987–1988 has been examined. Aerosol samples were analyzed for isotopic composition by using gamma- and alpha-spectrometric, and radiochemcal methods. Preliminary analysis of isotopic and fractional composition of aerosols carried out earlier indicated that over the first few months after the Chernobyl accident the relative contribution of^238,239,240Pu to air contamination was lowered as compared with beta-active products. At present, however, alpha-active plutonium isotopes became the dominant radioactive contaminants of the atmosphere and the concentrations of^238,239,240Pu inhaled fractions turned out to be lower than the limiting permissible values based on the USSR radiation safety standards for radioactive contamination of the atmosphere for the limited part of population exposed to radionuclides. Neverheless, it is necessary to know even moderate levels of atmospheric contamination by Pu-radionuclides, since their long impacts on the personnel operating in the 30 km zone of the Chernobyl NPP and population residing in the adjavent regions have not been studied properly. So, the risks for population health of such impacts cannot be generally excluded from consideration.