Determination of239,240Pu and241Am in environmental samples

An accurate and reliable method has been developed and routinely carried out for the sequential determination of^239,240Pu and²⁴¹Am in environmental samples. After suitable pretreatment.^239,240Pu and²⁴¹Am are separated from other elements by means of the anion exchange resin method. Americium-241 is purified by coprecipitation with calcium oxalate and then ion exchanged in mixed media of the mineral acid-methanol. In the analysis,²⁴²Pu (or²³⁶Pu) and²⁴⁴Cm are used as chemical yield monitors. The recoveries of the yield monitors in the analyses of some kinds of environmental samples were 7080% for plutonium and 7686% for curium. The concentration of^239,240Pu in the coastal sea water were 7.022 Bq/l and that of²⁴¹Am was 1.26.3 Bq/l. The mean concentrations of^239,240Pu in the edible parts of the marine products ranged from 0.22 to 7.4 mBq/kg · fresh and those of²⁴¹Am ranged from 0.11 to 2.6 mBq/kg · fresh.     

Plutonium and americium in sediment samples along the Romanian sector of the Danube river and the Black Sea coast

The concentrations of²³⁸Pu,^239,240Pu and²⁴¹Am were determined in eight sediment samples, collected from the bed of the Romanian sector of the Danube river and the Black Sea coast during 1994 and 1995. Fusion with potassium carbonate was used to achieve complete dissolution of the samples. Tracers,²⁴²Pu and²⁴³Am, were added and the separation of plutonium from americium, uranium and thorium was performed by anion exchange. Americium was separated from uranium in two steps, using a conventional anion exchange resin and an extraction chromatographic resin for transuranics. After electrodeposition on stainless steel discs the nuclides were counted with -spectrometry with -PIPS detectors. The total plutonium concentrations obtained by this method were compared with the acid leachable plutonium concentrations reported for the same samples in a previous paper.     

Plutonium Activity Ratios in Plankton: New Evidence of Hold-Up Time in Irish Sea Sediments

The determination of activity ratios for radioisotopes of different half-lives can be used to estimate transit times from a point source to locations further away. For conservative elements, this time is approximately equivalent to the net hydrological transport. However, for non-conservative elements such as plutonium, the additional influence of biogeochemical processes decreases the net transport time. In this study, ²⁴¹Pu and ^239,240Pu concentrations in Irish Sea plankton samples, collected in May 1994, were determined and the ²⁴¹Pu/^239,240Pu ratios calculated. Plutonium-239,240 was measured using a standard method by ion exchange chromatography and alpha counting, and ²⁴¹Pu was determined by liquid scintillation counting using the disk-supported technique. The latter showed some methodological problems, which are briefly discussed. The ²⁴¹Pu/^239,240Pu ratios gave an estimate of the "transit time" from Sellafield to the different sampling points. In fact, this time represents the age of plutonium in plankton, i.e., the time lag between release from Sellafield and detection at the different sampling stations. The mean plutonium age was 17±2 years (n = 10) and 18.6±0.8 years (n = 13) in phytoplankton and zooplankton, respectively. The spatial distribution was reasonably homogeneous over the Irish Sea. The assimilation-elimination processes of plutonium in plankton are rather rapid. Therefore, it may be assumed that, in this time scale, the plutonium concentrations were in equilibrium with surrounding waters. Thus, it is concluded that plutonium was rather old because resuspension-sedimentation processes had occurred that delayed its transport within the Irish Sea. Therefore, the age of plutonium in plankton represented the hold-up time of plutonium in the sediments from the Irish Sea.     

Behaviour of239,240Pu and241Am in the Baltic Sea; Measurements and interpretation in 1980–1984

Concentrations of^239,240Pu and²⁴¹Am in filtered seawater, particulate fraction and sediment were measured. Methods for determination of these nuclides were critically chequed and a new rapid method for²⁴¹Am in sediment was developed. Due to seasonal variation a significant decrease of plutonium and americium concentrations in surface water takes place in summer. Americium is more efficiently associated with particulate matter than plutonium. From May 1980 to September 1984 soluble plutonium in the water was reduced to about half. The residence half-time of^239,240Pu in the water of Baltic Sea is of the order of 5 years. About similar concentrations of^239,240Pu and²⁴¹Am were found in particulates in water as in the surface layer of the sediment. The average K_d-values for plutonium and americium were 10⁵ and 10⁵–10⁶ ml/g, respectively.     

Host phase of239,240Pu and241Am in deep-sea sediment

Host phases of fallout^239,240Pu and²⁴¹Am were studied in the surface sediments obtained in 1994 from abyssal basins of relatively small area of the western North Pacific. An analytical procedure involving sequential chemical extraction was employed for partitioning the host phases of the nuclides in sediment into five fractions: (1) exchangeable (2) bound to carbonate, (3) bound to hydrous Fe-Mn oxides, (4) bound to organic matter and (5) residual. Decrease of total^239,240Pu concentration with decreasing association of^239,240Pu with organic matter, high²⁴¹Am/^239,240Pu activity ratio in carbonate phase and somewhat high proportion of oxidized^239,240Pu in leachable phases suggest a possibility of post-depositional diagenetic remobilization of Pu from sediment to water column.     

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.     

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     

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.     

Determination of plutonium and americium in moss and lichen samples

A simple, sensitive and selective method is described for the simultaneous determination of plutonium and americium in lichen and moss samples which can be used as the atmospheric radioactivity bioindicators. Plutonium is separated from a HCl leaching solution by a Microthene-TNOA column; americium is separated by a KL-HDEHP column and purified by PMBP-TOPO extraction. A special attention has been paid to the decontamination of plutonium and americium from²¹⁰Po. Ten lichen and 12 moss samples from tree trunks have been analyzed: starting from 2 g sample, the average yields and the detection limits were 70.2±12.5% and 28 mBq/kg for plutonium and 70.0±15.1% and 34 mBq/kg for americium. The concentrations (mBq/kg) ranged from 28 to 4960 for^239,240Pu, from 28 to 171 for²³⁸Pu and from 34 to 1930 for²⁴¹Am, respectively.     

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.     

Distribution and behaviour of99Tc,237Np,239,240Pu,and241Am in the coastal and estuarine sediments of the Irish Sea

Intertidal coastal and estuarine sediments from 24 sites in the Irish Sea have been analyzed for⁹⁹Tc,²³⁷Np,²³⁸Pu,^239,240Pu and²⁴¹Am. The²³⁷Np activity and²³⁹Pu/²⁴⁰Pu ratio were measured simultaneously by ICP-MS, and⁹⁹Tc was determined by HR-ICP-MS which is ten times more sensitive than Q-ICP-MS.The activities of⁹⁹Tc,²³⁷Np,^239,240Pu and²⁴¹Am were distributed over a wide range of 1.5–70.5, 0.01–13.3, 2.3–1589, 2.6–1894 Bq/kg, respectively. Activities of these radionuclides decreased exponentially with distance from the Sellafield source. The²⁴¹Am/^239,240Pu and²³⁷Np/^239,240Pu ratios were almost constant with distance from the Sellafield. This result suggests that the distribution and behavior of Np and Pu are controlled by complicated factors such as the influence of transport, the variation with time of Np/Pu ratio in the Sellafield discharges and sedimentary mixing processes in the Irish Sea.     

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 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.     

Determination of difficult-to-measure actinides in evaporator concentrate

Radiochemical separation of americium, neptunium and plutonium was tested on model solution of evaporator concentrate sample for isolation of each of them for alpha-spectrometry analysis. A good chemical separation of radionuclides of interest from the matrix and interfering radionuclides is required, once the relatively small difference in alpha-particle energy makes it difficult to spectrometrically separate the peaks. This paper describes use of the molecular recognition technology product AnaLig^®Pu-01 gel from IBC Advanced Technologies, Inc. to effectively and selectively pre-concentrate, separate and recover americium, neptunium and plutonium from model solution of evaporator concentrate samples from Nuclear Power Plant which belong to the most difficult matrices to analyse. The method is suitable for analysing highly contaminated samples of radioactive waste in a relatively short time. For counting the alpha activity of ²⁴¹Am, ^239,240Pu, ²³⁸Pu and ²³⁷Np ORTEC 576A alpha-spectrometer equipped with ULTRA^TM ion implanted silicon detectors (600 mm² active area) was used. The spectra were processed by using the Alpha-vision^TM 32-bit emulation software from the EG&G ORTEC company.     

A gamma-spectrometric method for the determination of plutonium isotope ratios

A gamma-spectrometric method using an intrinsic high resolution germanium detector has been developed for the determination of isotope ratios of plutonium from samples in solution form. The method is based on the assay of low energy gamma-rays of²³⁸Pu,²³⁹Pu,²⁴⁰Pu and²⁴¹Pu and does not require the use of branching intensities or the knowledge of detection efficiencies for different gamma rays. Since low energy gamma-rays are used, the effect of²⁴¹Am has also been studied. It is found that results are not affected up to 0.5 wt% of²⁴¹Am in plutonium samples. An accuracy of 3% is achievable in the determination of²⁴⁰Pu/²³⁹Pu and²⁴¹Pu/²³⁹Pu atom ratios as demonstrated by carrying out measurements on isotopic standards of plutonium.     

Procedures to define Pu isotopic ratios characterizing a contaminated area in Palomares (Spain)

Plutonium isotopic ratios have been calculated in soils contaminated by the Palomares accident which occurred in 1966 (Almería, Southeastem Spain). Contrasted techniques have been used to determine the radionuclide activities:²³⁸Pu and^238+240Pu were analysed by -spectrometry prior purification on anion-exchange resins, the ratio²³⁹Pu/²⁴⁰Pu was estimated by -spectra deconvolution and²⁴¹Pu was directly measured by liquid scintillation counting and indirectly through quantification of in-grown²⁴¹Am from aged plutonium discs. The mean activity ratios²³⁸Pu/²³⁹Pu,²³⁹Pu/²⁴⁰Pu,²⁴¹Pu/²³⁹Pu, backdated to 1966, were 0.027±0.002 (1), 4.5±0.2 (1) and 8.2±0.8 (1), respectively, characterizing the accident of Palomares as the source term of the measured plutonium.     

Concentration levels and behavior of transuranium nuclides in Japanese coastal marine environment

The concentration of^239,240Pu and²⁴¹Am in different samples collected from the coastal marine environment of Ibaraki Prefecture, Japan facing the Pacific Ocean have been studied. Seawater samples have been collected since 1975 and sea-biota since 1981. The mean concentration levels of^239,240Pu and²⁴¹Am were 0.51, 0.20 for anchovy, 0.22, 0.11 for flounder, 4.9, 0.77 for brown algae, 2.0, 2.4 for shellfish, and 0.022, 0.0028 for seawater (in mBq/kl), respectively. The chronological change of^239,240Pu in seawater was influence by fallout amounts. The activity ratio between the nuclides showed steady levels after two years from the end of atmospheric nuclear explosion tests. Activity levels and the ratios for each type of sample are briefly discussed.     

Plutonium in soils, bottom sediments and lichen near peaceful nuclear explosion sites in the Republic of Sakha (Yakutia)

During the 1974–1987 period 12 paceful nuclear explosions were conducted in the Republic of Sakha (Yakutia). For the first time^239,240Pu and²³⁸Pu concentrations were determined in samples of soils, bottom sediments and lichen taken at the Craton-3 and Crystal nuclear explosion sites. At the Craton-3^239,240Pu concentrations in the range 6.2 mBq/g to 5.9 Bq/g samples of soil and^239,240Pu concentrations up to 7.4 Bq/g in samples of lichen were observed.^239,240Pu concentration measurements in bottom sediments of a stream washing out the banking around the borehole of Craton-3 show that plutonium migrates in the direction of the Markha river. At the Crystal site local plutonium concentrations up to 35 Bq/g in soil and 1.8 Bq/g in lichen were observed.     

Fallout plutonium concentration in Japanese tissues: A new look at the old samples

Since 1962, we have been investigating the levels of^239,240Pu in human tissues. In the 1960s, the quantities of^239,240Pu found in the gonad and spleen were higher than those in liver and lung, as reported in our previous papers. This work was done to provide a reassessment of^239,240Pu distribution among several tissue samples from the 1960s and early 1970s, using current analytical techniques for plutonium. The autopsy tissues were collected from the Hospital of Niigata Prefectural Institute for Cancer Research in Northern Japan from 1968 to 1975. The subjects were at least 50 years old at the time of death. The accuracy and precision of^239,240Pu determinations were examined using NBS-SRM 4352 human liver samples. Our results are consistent with certified values.     

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.