Ecological considerations of the behavior of plutonium in the environment.
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There are a number of factors which must be considered in establishing whether or not the inadvertent intrusion of a sizable amount of plutonium-bearing material into a natural water system may have a significant impact on the health of those individuals who use that system as a drinking water resource. These factors include the chemical form(s) and solubility of plutonium in natural waters, its behavior in relation to natural processes (geochemical and biological), its fate in water treatment systems, and its uptake by man from drinking water. From the results obtained in our investigations of the behavior in natural water systems, it appears that (1) the chemical forms of plutonium dissolved in natural waters are Pu(IV) and Pu(V), (2) the soluble plutonium in many waters is bound to the organic constituents which probably enhances plutonium solubility, (3) the natural process responsible for the removal of plutonium from water is adsorption onto sediments, and (4) in water treatment systems, soluble plutonium is oxidized to the VI state and this form is not removed. From our investigations of gastrointestinal absorption, it appears that the value for f1, the fraction transferred from the gut to blood, is surely greater than 1 X 10(-3) and may be as high as 2 X 10(-1). Consideration of these and other factors indicates that, in the event of an accident, the concentration of plutonium could, in certain small natural water systems, approach and perhaps even exceed, the MPC for plutonium. However, the impact on the health of the affected population would not be inordinately high.
Estimates of both individual and collective doses received by the United States population following the Chernobyl accident have been made by using the data obtained from the U.S. Environmental Protection Agency's Environmental Radiation Ambient Monitoring System. Radionuclides associated with the debris first were measured in precipitation and surface air particulates at Portland, OR and Olympia, WA on 5 May 1986. Iodine-131 was the most consistently measured nuclide in all media, although several Cs and Ru isotopes also were observed. Strontium and any actinides notably were absent from the samples at the lower level of detection. The highest calculated individual-organ dose due to intake during May and June 1986 was 0.52 mSv to the infant thyroid in the state of Washington. This was predominantly (98%) from the ingestion of milk. The maximum U.S. collective dose equivalent to any organ was calculated to be 3,300 person-Sv to the thyroid. Risk estimates project three excess lung cancer deaths and an additional four deaths due to cancers of thyroid, breast and leukemia in the U.S. population over the next 45 y from exposure during the May-June 1986 interval. The only long-lived radionuclide measured in milk samples following the accident was 137Cs. We estimate 20 excess fatalities from the ingestion of 137Cs in milk during all subsequent years, with six of these due to lung cancer and the majority of the remainder distributed approximately equally among cancers of the thyroid, breast, liver and leukemia. A total of 100 excess fatalities from all dietary components was estimated. Because of the uncertainty of risk estimates from data such as those available for this study, all calculated values carry a range of uncertainty from a minimum of one-half the calculated value to a maximum of two times the calculated value. The estimated excess fatalities given above may be compared with corresponding projected cancer mortality from all other causes: 41,000 fatalities from thyroid cancer and 3,800,000 fatalities from lung cancer are estimated to occur within the U.S. population during the next 45 y.
When applying the standard method of in-situ gamma spectrometry to determine deposited radionuclide activities, an assumption is needed regarding the depth distribution of radionuclides in the ground. The method can be improved by assessing, from information contained in the spectrum, the attenuation of the radiation by the soil and vegetation. By comparing the count rates of the x ray and the gamma-ray lines of its daughter nuclide 137mBa, the 137Cs activity per area can be determined. The range of applicability of the method is discussed by means of an uncertainty analysis, and the method is applied to post-Chernobyl measurements. A comparison with the results of the standard method of in-situ spectrometry demonstrates the progress achieved by the proposed method. Nevertheless, the method still has some shortcomings for the peak analysis that could be improved by better detector resolution or better computer software.
The objectives of this study were to compare four common techniques used to estimate soil mass loadings on plant surfaces and to assess the need to account for particle-size distributions of both the soil tracer and contaminant of concern within the soil. Soil loadings (g soil kg-1 dried plant) from split samples collected in a pasture near Chernobyl were estimated using soil tracers of plutonium analyzed via alpha spectroscopy (mean +/- standard error; 1.0 +/- 0.2), titanium analyzed with an inductive coupled plasma spectrometer; (3.6 +/- 0.6), and neutron activation analysis for scandium (8.1 +/- 1.6), as well as simply washing the soil off the vegetation (34.1 +/- 5.6) Differences were significant at p < 0.001. We also found that soil loading estimates from any one technique varied by a factor of 10 depending on the soil particle size used in the calculations. This was because soil loadings decreased when smaller-sized soil fractions dominated the resuspension process. However, the percent of the plant's total contamination attributable to soil loading increased with smaller soil particles. Smaller soil particles apparently contribute less to the mass of soil loading (g soil kg-1 dry plant), but more to the total plant contamination (Bq) because of the higher concentration of contaminant found in the smaller-sized soil fractions. Differences in mass loading estimates due to the technique chosen (a factor of 10), or due to differences in elemental concentration as a result of the soil particle size used in the calculation (also a factor of 10), were greater than the natural variability observed in the field (2.5).
The Chernobyl Nuclear Power Plant accident in 1986 caused radionuclide contamination in most countries in Eastern and Western Europe. A prime example is Belarus where 23% of the total land area received chronic levels; about 1.5 x 10(6) ha of forested lands were contaminated with 40--190 kBq m-2 and 2.5 x 10(4) ha received greater than 1,480 kBq m-2 of 137Cs and other long-lived radionuclides such as 90Sr and 239,240Pu. Since the radiological dose to the forest ecosystem will tend to accumulate over long time periods (decades to centuries), we need to determine what countermeasures can be taken to limit this dose so that the affected regions can, once again, safely provide habitat and natural forest products. To address some of these problems, our initial objective is to formulate a generic model, FORESTPATH, which describes the major kinetic processes and pathways of radionuclide movement in forests and natural ecosystems and which can be used to predict future radionuclide concentrations. The model calculates the time-dependent radionuclide concentrations in different compartments of the forest ecosystem based on the information available on residence half-times in two forest types: coniferous and deciduous. The results show that the model reproduces well the radionuclide cycling pattern found in the literature for deciduous and coniferous forests. Variability analysis was used to access the relative importance of specific parameter values in the generic model performance. The FORESTPASTH model can be easily adjusted for site-specific applications.
After the Chernobyl event, a large area of land was contaminated following the deposition of radionuclides. This area became a continuing source of radionuclides to natural waters and aquatic ecosystems. In 1986, an experimental plot was constructed in a contaminated area near the Chernobyl Nuclear Power Plant to study the washoff of radionuclides by surface runoff. Concentrations of 137Cs and 90Sr were measured in the top 10 cm of the soil prior to the experiments. During two separate experiments, intense artificial rainfall was applied to the plot. A washoff scenario was then prepared with site-specific information on initial soil contamination, duration and quantities of rainfall and runoff, physicochemical properties of the topsoil, and some climatological data. Modelers were asked to predict (a) the vertical distributions of the initial concentrations of 137Cs and 90Sr in various chemical forms in the topsoil, (b) concentrations of these radionuclides in various chemical forms in the runoff water during each experiment, and (c) the total amounts of these radionuclides that were washed off during each experiment. Stochastically generated local rainfall data were used in a water budget model to generate annual average runoff and infiltration rates. A vertical, one-dimensional, multiphase, multispecies transport model was then developed to simulate the movement of contaminants in the topsoil during the 160-d period between the Chernobyl event and the experiments as well as the washouts of contaminants by runoff during the experiments and during the 24-h period thereafter. The model provided very good predictions of the vertical distributions of total contaminant concentrations in the top 10 cm of the soil; however, the concentrations in individual chemical forms were not predicted as accurately. Initially, the model overpredicted the washout of contaminants for the two experiments and the 24-h period thereafter. Fraction of runoff that flows as interflow and average sediment loading in the runoff were identified as parameters responsible for the overprediction. Calibration of the interflow fraction and adjustment of the average sediment loading in runoff to a level representative of Eastern Europe considerably improved these predictions. The complete modeling approach and comparisons of model predictions with measurements and with predictions from other modelers are presented.
Radiocesium contamination from the Chernobyl accident of fruits and leaves from various fruit trees was systematically studied from 1990 to 1995 on two agricultural experimentation farms in Northern Greece. The results are discussed in the framework of a previously published model describing the long-term radiocesium contamination mechanism of deciduous fruit trees after a nuclear accident. The results of the present work qualitatively verify the model predictions.
Beer has been brewed from barley contaminated with 137Cs as a consequence of the Chernobyl accident. The 137Cs activity has been measured in all intermediate steps and in the by-products of the production process. About 35% of the 137Cs in barley were recovered in beer. Processing factors defined as the concentration ratio of processed and raw products were determined to be 0.61, 3.3, 0.1 and 0.11 for malt, malt germs, spent grains and beer, respectively.
Radiocesium dynamics in a Quercus conferta Kit ecosystem in Northern Greece have been extensively studied over the years 1993-1995. Radiocesium distribution in the different parts of the ecosystem was measured. A total 137Cs inventory of 243+/-66 MBq ha(-1) due to the Chernobyl accident was measured in all parts of the ecosystem. Almost 90% of this inventory is still in the upper layers of the soil and the forest floor. In particular 13.4% is in the forest floor, 52.6% in the Ah horizon, and 23.4% in the upper 5 cm of the soil. Only 2.2% of this inventory is in the above ground biomass. The mean total 137Cs deposited on the forest floor from the above ground biomass is 0.18 MBq ha(-1) y(-1). Cesium leaching from the forest floor is negligible. The radiocesium distribution in soil is fixed and in equilibrium, at least since 1993. Most of radiocesium is not available for migration. Cesium migration in soil was modeled by a) an "equivalent diffusion" model with different initial conditions and b) a "compartment" model derived from a diffusion-advection model. A compartment model for the contamination of living biomass is proposed. The total absorbed dose rate in air as well as the contribution due to 137Cs from the Chernobyl accident was determined inside the forest, by in-situ gamma spectrometry.
The prevalence of thyroid nodules and thyroid cancer was studied in the indigenous population residing on Ebeye Island, Kwajalein Atoll, in the Republic of the Marshall Islands. This island, centrally located in the nation, is home to about 25% of the nation's population, many who have migrated there from other atolls. The objective of the study was to obtain thyroid disease rate statistics on as much of the population as possible that was alive during the years of nuclear testing and to test the hypothesis that described a linearly decreasing prevalence of palpable nodules with increasing distance from the Bikini test site. 1,322 Marshallese born before 1965 were given a thyroid examination using neck palpation, fine needle aspiration biopsy, and high resolution ultrasound imaging. Approximately 40% of the total population living on this island who are at risk from exposure to radioactive fallout during the years 1946-1958 were screened. Of that group, 815 were alive at the time of the BRAVO test on 1 March 1954. Two hundred sixty-six people with thyroid nodules were found (32.6%): 132 were palpable nodules (16.2%), and 134 were nodules that could be diagnosed with ultrasound only (15.7%). Prevalence of palpable nodules was particularly high in men and women older than 60 y, in men who were 6 to 15 y of age at the time of the BRAVO test, and in women 1 to 10 y of age at the time of the BRAVO test. In 22 people, the clinical diagnosis was most likely cancer though histopathological evidence was only available from 11 operated cases. Of the 11 operated cases, 10 were cancer. Cancer prevalence was particularly high in those women born between 1944 and 1953 (7/220 = 3.2%), i.e., who were children during the early years of nuclear testing. The Ebeye data showed a marginally significant correlation between palpable nodule prevalence among women and distance to Bikini (r = -0.44, p = 0.06). This report summarizes the clinical findings of the thyroid examinations, the age distributions for nodular disease and cancer, and examines the relationship between prevalence of nodules and present day levels of 137Cs in the environment of each atoll.
The residual radiocesium concentration, nearly 10 y after the Chernobyl accident, is measured at different sites on the Belgian territory by means of in-situ gamma-spectrometry. A possible link between the rainfall at the beginning of May 1986 and the actual cesium concentration is investigated. The radiological impact of this contamination, even in the most affected regions in the Ardennes, is very small (<6 microSv y(-1)).
A small number of animal thyroids from Bad Hall, Austria; Ulm, Germany; and Steinkjer, Norway had 131I (half-life 8.06 d) measured between 21 and 72 d following the nuclear accident at Chernobyl on 26 April 1986. Nine years later 129I (half-life 1.57 x 10(7) y) fission product and natural 127I were measured in the same thyroids. The mass ratios, 129I/131I were calculated to the date of the Chernobyl accident and they ranged between 13 and 71. These ratios are compared to the expected ratios within an operating nuclear reactor during 2 y of operation, where the 129I/131I(-1) ratio never exceeded 30. The observed ratio of 129I to natural 127I in thyroids ranged from 5 to 200 times the ratio before the accident, except that the Norwegian thyroids had 129I/127I ratios which were less than the ratios of pre-Chernobyl thyroids from Ulm. These studies show the 129I and 131I from the Chernobyl accident were accumulated with natural 127I in animal thyroids but the isotope ratios, calculated to the release date, had wide ranges. The 131I radioactive exposure might be estimated from a fission product mixture by measuring 129I in thyroids long after the exposure to 131I, but the results would probably show a wide range of possibilities. The determining variables should be evaluated. We know of no previous data regarding both 131I and 129I in thyroid glands during the first 3 mo after the Chernobyl accident.
This review examines the epidemiologic and experimental studies into the possible role ionizing radiation might play in Down Syndrome (trisomy 21). It is prompted by a report of a temporal cluster of cases of this chromosomal disorder observed in West Berlin exactly 9 mo after the radioactive cloud from Chernobyl passed. In approximately 90% of cases, Down Syndrome is due to the nondisjunction of chromosome 21, most often in the oocyte, which may be exposed to ionizing radiation during two separate periods: before the completion of the first meiosis or around the time of ovulation. Most epidemiologic studies into trisomies and exposure to ionizing radiation examine only the first period; the Chernobyl cluster is related to the second. Analysis of these epidemiologic results indicates that the possibility that ionizing radiation might be a risk factor in Down Syndrome cannot be excluded. The experimental results, although sometimes contradictory, demonstrate that irradiation may induce nondisjunction in oogenesis and spermatogenesis; they cannot, however, be easily extrapolated to humans. The weaknesses of epidemiologic studies into the risk factors for Down Syndrome at birth (especially the failure to take into account the trisomy cases leading to spontaneous abortion) are discussed. We envisage the utility and feasibility of new studies, in particular among women exposed to prolonged or repeated artificially-produced ionizing radiation.
The absorbed gamma dose rate in air 1 m above soil due to natural gamma emitters and 137Cs from the Chernobyl accident was determined inside a Quercus conferta Kit ecosystem in Northern Greece by combination of Monte Carlo simulations with the MCNP code and in-situ gamma spectrometry measurements. The total absorbed gamma dose rate in air is about 64 nGy h(-1), where 40% of this value is due to 137Cs and 60% to natural gamma emitters. The Monte Carlo simulations indicated that the gamma absorbed dose rate in air due to 137Cs is mainly due (70%) to unscattered radiation and to a lesser extent (30%) to the scattered radiation. The results obtained with the Monte Carlo simulations for the unscattered radiation were in very good agreement with the experimental values deduced by in-situ gamma spectrometry measurements. From the combination of the Monte Carlo simulations and in-situ gamma spectrometry measurements a conversion factor C = 1 nGy h(-1)/kBq m(-2) was deduced for 137Cs. This factor must be used with caution and only for forest sites similar to the one used for this work.
The Chernobyl accident in April 1986 resulted in widespread contamination of the environment with radioactive materials, including (131)I and other radioiodines. This environmental contamination led to substantial radiation doses in the thyroids of many inhabitants of the Republic of Belarus. The reconstruction of thyroid doses received by Belarussians is based primarily on exposure rates measured against the neck of more than 200,000 people in the more contaminated territories; these measurements were carried out within a few weeks after the accident and before the decay of (131)I to negligible levels. Preliminary estimates of thyroid dose have been divided into 3 classes: Class 1 ("measured" doses), Class 2 (doses "derived by affinity"), and Class 3 ("empirically-derived" doses). Class 1 doses are estimated directly from the measured thyroidal (131)I content of the person considered, plus information on lifestyle and dietary habits. Such estimates are available for about 130,000 individuals from the contaminated areas of the Gomel and Mogilev Oblasts and from the city of Minsk. Maximum individual doses are estimated to range up to about 60 Gy. For every village with a sufficient number of residents with Class 1 doses, individual thyroid dose distributions are determined for several age groups and levels of milk consumption. These data are used to derive Class 2 thyroid dose estimates for unmeasured inhabitants of these villages. For any village where the number of residents with Class 1 thyroid doses is small or equal to zero, individual thyroid doses of Class 3 are derived from the relationship obtained between the mean adult thyroid dose and the deposition density of (131)I or 137Cs in villages with Class 2 thyroid doses presenting characteristics similar to those of the village considered. In order to improve the reliability of the Class 3 thyroid doses, an extensive program of measurement of (129)I in soils is envisaged.