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Transuranics in bone of deceased former residents of Rongelap Atoll, Marshall Islands.

Rongelap Atoll received intensive fallout from the 1 March 1954 Bravo thermonuclear test 105 miles upwind at Bikini. Fearful of their continued exposure to radiation, the residents of Rongelap Atoll went into voluntary exile in 1985. Transuranic soil concentrations on Rongelap Island are about 2-3 orders of magnitude greater than the average for the Northern hemisphere; the three dominating transuranics are 239,240Pu and 241Am. Only conflicting information has been available about the extent of transuranic uptake by the Rongelap community. As part of the Rongelap Resettlement Project, the community endorsed the exhumation of bones of deceased former atoll residents to provide an independent estimate of plutonium intake. This approach has the advantage of reducing the uncertainties associated with pathway modeling and the interpretation of urine data. Six graves (4 adults, 2 children) were selected for exhumation. Femora and tibiae were selected as well as humeri from the children's graves. The rest of the remains was left undisturbed. The results of the analysis of 239,240Pu and 241Am are presented. Assuming that the data can be considered as representative for the Rongelap population as a whole, the contamination with transuranics on Rongelap Atoll appears to result in radiation exposures in the order of 1% of the compliance limit of 100 mrem (1 mSv) effective dose equivalent per year.

Adult↗

Study of alpha-particle emission probabilities and energies in the decay of 240Pu.

In the frame of EUROMET Project No 325 "Analysis of Plutonium Alpha-Particle Spectra", the isotopic composition of a 238, 239, 240Pu mixture was measured by mass spectrometry and by high-resolution alpha-particle spectrometry. The latter revealed a discrepancy with published data of the alpha-particle emission probabilities (Palpha) and the energies (Ealpha) of the two major peaks of 240Pu. New values have been derived: Palpha1 = 0.7256 (6), Palpha2 = 0.2735 (7) and Ealpha1 = 5168.54 (14)keV, Ealpha2 = 5124.10 (15)keV, relative to reference peaks of 238Pu and 239Pu.

Alpha Particles↗

Accelerator mass spectrometry measurement of 240Pu/239Pu isotope ratios in Novaya Zemlya and Kara Sea sediments.

Generally low levels of plutonium in environmental samples, often combined with limited sample sizes, necessitate reliable low-level techniques for determination of Pu isotopes. Accelerator mass spectrometry (AMS) has proved to be a powerful method for measuring low-level Pu activity concentrations and Pu isotope ratios. Based on procedural blanks, detection limits for AMS were below 1 fg Pu (equivalent to ca. 2 microBq 139Pu), which can compete with both TIMS, high sensitivity ICP-MS, and certainly alpha-spectrometry, while showing less interference, memory and matrix effects as compared to routine ICP-MS techniques. In addition to low detection limits, the technique offers the advantage of giving information on Pu isotope ratios. Measurements of sediments collected from dumping sites at Novaya Zemlya showed deviation from global fallout 240Pu/239Pu ratios.

Environmental Monitoring↗

Retrospective estimation of the concentration of 241Pu in air sampled at a Belgrade site following the Chernobyl accident.

The surface air activity concentration of 241Pu for the period May 01-15, 1986, for a monitoring site in Vinca, Belgrade was retrospectively estimated. The results were obtained by re-measurement of plutonium fraction alpha-spectrometric sources, with 236Pu as a tracer, used almost 13 years earlier for the determination of (239,240)Pu concentration in surface air immediately after the Chernobyl accident. The estimated 241Pu concentration, based on the 241Am in-growth method for air samples, ranged from 240 to 7800 microBq/m3. The average activity ratio 241Pu/(239,240)Pu originating from the Chernobyl accident at Belgrade site was approximately 100 at the collection time.

Air Pollutants, Radioactive↗

A new digital autoradiographical method for identification of Pu particles using an imaging plate.

An autoradiographical method using an imaging plate (IP) was developed to identify rapidly the density of plutonium (Pu) particles on filter samples. Photostimulated luminescence (PSL) signals were obtained by exposing IPs to filter samples collecting Pu particles and naturally occurring radon decay products, respectively. Search and analysis of the alpha-induced PSL signals presented the time-dependent growth of PSL intensity from the Pu particles and the range of PSL intensities from radon decay products, making it possible to discriminate Pu particles from radon decay products using an empirical Pu-discrimination level, and then to quantify the Pu activities on a particle-by-particle basis. The method is useful for a fast screening of filter samples for Pu particles because it requires no special skills and tedious procedures during its use, gives a low discriminable activity for individual Pu particles with a relatively short exposure time, and allows us to measure a large number of filter samples at the same time.

Air Pollutants, Radioactive↗

40K, 137Cs, 90Sr, 238,239+240Pu and 241Am in mammals' skulls from owls' pellets and owl skeletons in Poland.

Skulls of small mammals belonging to two species of rodents and three species of insectivores collected in Eastern Poland were the subject of the present investigation. The skulls were separated from owl pellets. Activities of 40K, 137Cs, 90Sr, 238,239+240Pu and 241Am were determined by means of gamma spectrometry as well as liquid scintillation spectrometry or alpha spectrometry along with relevant radiochemical procedures. A detailed description of the procedures is provided. The research was supplied with the analysis of three skeletons of owls. No measurable difference between the skulls of rodents and insectivorous animals with regard to activity of any of the examined radionuclides was found. No accumulation effect in the owl skeletons was detected. Though measured activities of 137Cs and 40K for the skulls were of the same magnitude as those found previously for large wild herbivorous animals from typical locations in Poland, those for 90Sr were even lower than previously determined. A big difference was found for activities of plutonium and americium isotopes. Their mean activities were higher by an order of magnitude when compared to the examined previously values. The maximum 239+240Pu activity was equal to 97.5+/-7.7 mBq/kg, with 65% of it originating from global fallout. Relatively high content of transuranic elements found for rodents and insectivorous mammals seems to be unrelated to their feeding habits and should rather be attributed to the living conditions. It is suggested that small mammals, together with tiny soil particles present in mid-soil living tunnels, can inhale the transuranic elements.

Americium↗

Experimental values for 241Am and 239+240Pu Kd's in French agricultural soils.

Experiments resulted in determination of K(d) values for (241)Am and (239+240)Pu in 6 soils whose characteristics are representative of agricultural soils found around French nuclear power plant sites. These experiments were conducted in stirred batch reactors and the sorption isotherms were plotted. For americium, the experimental K(d) values varied from 60 to 4000 Lkg(-1) (d.w.) and correlated well with soil pH, K(d) increased with increasing pH. As regards plutonium, the experimental K(d) values varied between 300 and 9600 Lkg(-1) and decreased with increasing total sand content. The estimation of the total residence time determined by using a particular and experimentally refined value for K(d)-with a model similar to those currently used for impact assessments-illustrates the importance of establishing values that are better suited to specific soils than generic values. Lastly, depending on the type of evaluation envisioned, it might be important to look for a specific value of K(d)-and even modelling-more suited to the specificity of the scenario studied, by performing more complex, or even in situ, experiments.

Adsorption↗

A prognostic estimation of the area contaminated with alpha-emitting transuranium isotopes in Belarus following the Chernobyl accident.

As a result of the Chernobyl accident, some regions of Belarus have been contaminated with the plutonium isotopes (238,239,240,241)Pu. Considering the importance of the environmental impact of the alpha-emitting radionuclides we have carried out a prognostic estimation of the area contaminated with (238,239,240)Pu and (241)Am (the latter being a decay product of (241)Pu) in Belarus. The calculations were made using measurements of (238,239,240)Pu activity concentrations in soil samples from about 600 settlements in the affected region, together with the estimated activity ratio A((241)Am)/A((238,239,240)Pu). The area contaminated with alpha-emitting transuranium isotopes predicted for the year 2006 has been compared with that estimated for 1986. The results show that by 2006, the area of inhabited districts where contamination with (238,239,240)Pu and (241)Am exceeds the threshold level of 740 Bq/m(2), will be 3.7 times larger, reaching approximately 3.5 x10(3)km(2). Of this, almost 20% will have a contamination level of 1850--3700 Bq/m(2).

Americium↗

Distribution and inventories of fallout radionuclides (239+240Pu, 137Cs) and 210Pb to study the filling velocity of salt marshes in Doñana National Park (Spain).

Within an extensive multinational and multidisciplinary project carried out in Doñana National Park (Spain) to investigate its preservation and regeneration, the filling velocity of the salt marshes has been evaluated through the calculation of their average sediment accumulation rates. (239+240)Pu and (137)Cs from weapons testing fallout and total (210)Pb distribution profiles and inventories have been determined in some of the most characteristic zones of the park, namely, the ponds (or "lucios") and the waterjets (or "caños"). Plutonium inventories range from 16 to 101 Bq m(-2), (137)Cs values fluctuate between 514 and 3,758 Bq m(-2) and unsupported (210)Pb values comprise between 124 and 9398 Bq m(-2). Average sedimentation rates range from 3 to 5 mm y(-1) (1952-2002). These data are higher than those obtained by carbon dating for the period 6,500 AD-present, estimated as 1.5-2 mm y(-1), suggesting an increase in the accumulation of sediments and the alteration of the park's hydrodynamics caused by the re-channeling of the major rivers feeding the salt marshes.

Cesium Radioisotopes↗

Distribution of 137Cs, 238Pu and 239+240 Pu in sediments of the southeastern Brazilian shelf-SW Atlantic margin.

In this work levels of 137Cs, 238Pu and 239+240 Pu as well as activity ratios of anthrophogenic radionuclides in sediment samples from the southeastern Brazilian shelf are presented. Instrumental gamma spectrometry was used to determine 137Cs and alpha spectrometry to determine 238Pu and 239+240 Pu after a radiochemical procedure. The levels ranged from 0.30 to 1.79 Bq kg(-1) for 137Cs, from 15 to 150 mBq kg(-1) for 238Pu and, from 18 to 117 mBq kg(-1) for 239+240 Pu. There was a bathymetric differentiation in the radionuclides distribution. 137Cs values were generally higher in the samples collected at water depths of less than 100 m. On the other hand, plutonium isotopes exhibit higher values at greater depths. The mean ratio of 239+240 Pu/137Cs obtained was 0.112+/-0.072 which is in agreement with the value reported for the Atlantic from atmospheric fallout of nuclear explosions in the past. The 238Pu/230+240 Pu ratios varied widely (from 0.339 to 2.088) and showed the influence of the SNAP-9A accident in the 238Pu levels for this area. The main goal of this work was to present unpublished anthropogenic radionuclide levels and activity ratios related to the contamination of the southeastern Brazilian shelf.

Atlantic Ocean↗

Reconstructing historical radionuclide concentrations along the east coast of Ireland using a compartmental model.

A mathematical model is presented that simulates the annually averaged transport of radionuclides, originating from the BNFL reprocessing plant at Sellafield, throughout the Irish Sea. The model, CUMBRIA77, represents the processes of radionuclide transport and dispersion in the marine environment and allows predictions of radionuclide concentration in various environmental media, including biota, to be made throughout the whole of the Irish Sea. In this paper we describe the use of the model to reconstruct the historical activity concentrations of 137Cs and 239+240Pu in a variety of environmental media in the western Irish Sea and along the Irish east coast back to 1950. This reconstruction exercise is of interest because only limited measurements of 137Cs and 239+240Pu activity are available prior to the 1980s. The predictions were compared to the available measured data to validate their accuracy. The results of the reconstruction indicate that activity concentrations of 137Cs in the western Irish Sea follow a similar, though slightly delayed and smoothed, profile to the discharges from the Sellafield site, with concentrations at the time of peak discharge (the mid-1970s) being around an order of magnitude higher than those measured in the 1980s and 1990s. By contrast, the concentrations of 239+240Pu at the time of peak discharges were similar to those presently measured. These differences reflect the distinct marine chemistries of the two nuclides, in particular the higher propensity of plutonium to bind to sediments leading to extended transport times. Despite these differences in behaviour the doses to Irish seafood consumers from 137Cs remain significantly higher than those from 239+240Pu.

Animals↗

Measurement of 240Pu/239Pu isotopic ratios in soils from the Marshall Islands using ICP-MS.

Nuclear weapons tests conducted by the United States in the Marshall Islands produced significant quantities of regional or tropospheric fallout contamination. Here we report on some preliminary inductively coupled plasma-mass spectrometry (ICP-MS) measurements of plutonium isolated from seven composite soil samples collected from Bikini, Enewetak and Rongelap Atolls in the northern Marshall Islands. These data show that 240Pu/239Pu isotopic signatures in surface soils from the Marshall Island vary significantly and could potentially be used to help quantify the range and extent of fallout deposition (and associated impacts) from specific weapons tests. 137Cs and 60Co were also determined on the same set of soil samples for comparative purposes.

Environmental Monitoring↗

Availability of toxic trace metals to the conceptus.

Energy production releases numerous toxic metals into the environment. Among those metals which have been shown to be toxic to the conceptus are cadmium, lead, mercury, plutonium and vanadium. This paper reviews the results from the authors' studies of pregnant rats exposed to these metals by parenteral administration, inhalation or gastric intubation. In addition, direct measurements were made of maternal blood flow and clearance of metals across the guinea pig placenta to serve as conceptual examples of factors which regulate the effects of the metals on the fetus. Discussion includes the influence of route of maternal exposure and subsequent absorption, gestational age at exposure, metal behavior in the maternal bloodstream, movement of metals across the placenta, and distribution of metals in the products of conception.

Animals↗

Hot particles of the Yenisei River flood plain, Russia.

Some high-activity hot particles (HP) were found in the flood plain of the Yenisei River, near the Krasnoyarsk Mining-and-Chemical Combine (MCC), and their radionuclide compositions were determined. The ratios of plutonium and caesium isotopes in the particles are indicative of their reactor origin. The 137Cs activity of the particles amounts to 29,200 kBq/particle, which is higher than the corresponding activities of the fuel particles that formed as a result of the accident at the Chernobyl NPP. All the particles have been divided into two major groups according to the 137Cs/34Cs ratio: in the first group, the 137Cs/134Cs ratio is more than or equal to 3000, and in the second the 137Cs/134Cs ratio is less than or equal to 1000. The particles of the first and the second groups were preliminarily estimated to be formed 30 and 20 years ago, which suggests that there must have been at least two accidents at the MCC reactors, with part of the fuel released into the Yenisei River.

Cesium↗

Distributions of Pu, Am and Cs in margin sediments from the western Mediterranean (Spanish coast).

Continental margins are important areas to be considered when studying the distributions and depositions of pollutants, both conventional and radioactive. Coastal sediments accumulate most of those contaminants which can be introduced following atmospheric and/or fluvial pathways. Moreover, their residence times within the water column are usually shortened due to their affinity to associate with the downward falling particulate matter, more abundant at shallower depths. In this paper the distribution profiles and inventories of plutonium, americium and cesium are detailed, providing useful information about recent sedimentation phenomena such as sediment mixing, slumping processes and bioturbation. Unsupported 210Pb data are used as reliable indicators of enhanced/reduced deposition events. Also, the calculated inventories have enabled the estimation of the radiological contribution of the Spanish Mediterranean margin to the total radioactivity deposited onto the Mediterranean sea floor.

Air Pollutants, Radioactive↗

An assessment of the reported leakage of anthropogenic radionuclides from the underground nuclear test sites at Amchitka Island, Alaska, USA to the surface environment.

Three underground nuclear tests representing approximately 15-16% of the total effective energy released during the United States underground nuclear testing program from 1951 to 1992 were conducted at Amchitka Island, Alaska. In 1996, Greenpeace reported that leakage of radionuclides, 241Am and 239+240Pu, from these underground tests to the terrestrial and freshwater environments had been detected. In response to this report, a federal, state, tribal and non-governmental team conducted a terrestrial and freshwater radiological sampling program in 1997. Additional radiological sampling was conducted in 1998. An assessment of the reported leakage to the freshwater environment was evaluated by assessing 3H values in surface waters and 240Pu/239Pu ratios in various sample media. Tritium values ranged from 0.41 Bq/l +/- 0.11 two sigma to 0.74 Bq/1 +/- 0.126 two sigma at the surface water sites sampled, including the reported leakage sites. Only at the Long Shot test site, where leakage of radioactive gases to the near-surface occurred in 1965. were higher 3H levels of 5.8 Bq/1 +/- 0.19 two sigma still observed in 1997, in mud pit #3. The mean 240Pu/239Pu for all of the Amchitka samples was 0.1991 +/- 0.0149 one standard deviation, with values ranging from 0.1824 +/- 1.43% one sigma to 0.2431 +/- 6.56% one sigma. The measured 3H levels and 240Pu/239Pu ratios in freshwater moss and sediments at Amchitka provide no evidence of leakage occurring at the sites reported by Buske and Miller (1998 Nuclear-Weapons-Free America and Alaska Community Action on Toxics, Anchorage, Ak, p.38) and Miller and Buske (1996 Nuclear Flashback: The Return to Anchitka, p.35). It was noted that the marine sample; 240Pu/239Pu ratios are statistically different than the global fallout ratios presented by Krey et al. (1976) and Kelley, Bond, and Beasley (1999). The additional non-fallout component 240Pu/239Pu ratio, assuming a single unique source, necessary to modify the global fallout 240Pu/239Pu ratio to that measured in the marine samples is on the order of 0.65 (Hameedi, Efurd, Harmon, Valette-Silver, & Robertson, 1999; Kelley et al., 1999). While this potentially suggests another plutonium source, such as high burn-up nuclear reactor fuel, rather than underground nuclear tests, the uncertainties in analyses and environmental processes need to be fully assessed before any conclusion can be reached. Further work is needed to evaluate these findings and to support any radiological assessment of the marine environment surrounding Amchitka. Based on geohydrological testing and modeling, leakage from the Amchitka Underground Nuclear Tests is projected to occur to the marine environment (Claassen, 1978; Fenske, 1972; Wheatcraft, 1995).

Alaska↗

Indirect monitoring of internal exposure in the decommissioning of a nuclear power plant in Spain.

The experimental procedure used for the indirect measurement of internal exposure of workers involved in the first step of the decontamination of a nuclear power plant which is being decommissioned is presented. The establishment of decontamination and decommissioning programs is currently in progress at the nuclear power plant and monitoring procedures to assess workers' exposure have also been implemented. Due to the presence of transuranics, the monitoring program includes the analysis of excreta samples. An analytical method for the determination of plutonium (Pu) and americum (Am) in urine samples was developed. The radiochemical separation is based on the coprecipitation of transuranics and sequential isolation of Pu and Am by anion exchange and extraction chromatography. Finally, electrodeposited sources are prepared and counted by alpha-spectrometry.

Americium↗

New purification protocol for actinide measurement in excreta based on calixarene chemistry.

The determination of actinides concentration level in excreta, mainly urine is currently carried out to monitor people potentially exposed to alpha emitters. To measure actinides in such samples, specific analytical protocols have been set up. The chemical purification uses different chromatographic columns to selectively separate the actinides and each fraction, after electroplating, is measured by alpha spectrometry. To reach 1 mBq l(-1) of U, Pu or Am using these protocols, 6 days equally distributed between the chemical purification and the measurement are necessary. The protocol proposed here is based on a single extractant, the 1,3,5-trimethoxy-2,4,6-tricarboxy-p-tert-butylcalix[6]arene, used to selectively separate U, Pu and Am from the urinary matrix prior to be measured. Using this analytical protocol, U and Pu are quantitatively and selectively recovered in two different acidic backextraction solutions whereas Am is quantitatively and selectively recovered in the organic phase. Furthermore, the purification stage is considerably shortened. The uranium and plutonium amounts are measured in aqueous phases using alpha spectrometry or inductively coupled plasma-mass spectrometry, whereas Am is measured in the organic phase using alpha liquid scintillation (photon/electron-rejecting alpha liquid scintillation).

Actinoid Series Elements↗