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Estimates of (239+240)Pu inventories in Gdańsk Bay and Gdańsk basin.

This paper presents and discusses the results of (239+240)Pu determinations in different components of Gdańsk bay and Gdańsk basin ecosystem, as well as estimated sources and inventories of plutonium in these basins. The total plutonium (239+240)Pu activities deposited in Gdańsk bay and Gdańsk basin sediments are 1.18 TBq and 3.77 TBq, respectively. Two rivers, the Vistula and Neman rivers, and atmospheric fallout were distinguished as the main sources of plutonium in these basins. In seawater (with suspended matter included) there is about 2.33 GBq (239+240)Pu (0.2% of total activity) in Gdańsk bay and 9.92 GBq (239+240)Pu (0.3% of total activity) in Gdańsk basin. In both cases, 56% of (239+240)Pu is associated with suspended matter. Organisms contain 3.81 MBq in Gdańsk bay and 7.45 MBq (239+240)Pu in Gdańsk basin. From this value in Gdańsk bay 82.1% of plutonium is associated with zoobenthos, 13.6% with phytobenthos, 1.6% with phytoplankton, 1.5% with zooplankton and 1.2% with fish. In Gdańsk basin, 83.2% is associated with zoobenthos, 7.5% with phytobenthos, 3.6% with phytoplankton, 3.2% with zooplankton and 2.5% with fish.

Animals↗

Risks to the public from historical releases of radionuclides and chemicals at the Rocky Flats Environmental Technology Site.

This paper summarizes the methods and results of estimating risks of cancer incidence resulting from plutonium, carbon tetrachloride, and beryllium releases from operations at the Rocky Flats Environmental Technology Site, near Denver, Colorado, from 1953 through 1989. The key findings show that people who lived near the facility were exposed to plutonium mainly through inhalation during routine operations, from a major fire in 1957, and from plutonium resuspended from contaminated soil from an outdoor drum storage area, called the 903 Area. Results were presented for five exposure scenarios that were location-independent. Individuals described by the laborer scenario received the highest risk of all scenarios considered. Upper bound (95th percentile) incremental lifetime cancer incidence risks for the laborer scenario were in about the 10(-4) range (1 chance in 10,000) for developing cancer from Rocky Flats plutonium releases during a lifetime. At the 5th percentile level, the maximum cancer risk was about 10(-7) (1 chance in 10 million) for developing cancer during a lifetime. Estimated cancer risks at the 95th percentile level are within the range of for acceptable risks established by the US Environmental Protection Agency of 10(-6) to 10(-4). Carbon tetrachloride was found to be the chemical that presented the highest risk to the public. The 5th and 95th percentile risk values for exposure to carbon tetrachloride were 9.2x10(-7) and 2.5x10(-5), respectively.

Adolescent↗

The induction by 239Pu of myeloid leukaemia and osteosarcoma in female CBA mice.

Plutonium-239 was injected into 12-week-old female CBA/H mice in the range 1.85-18.5 kBq kg-1 either as a single injection or as 16 injections spaced at 3.5 day intervals over eight weeks. There was a highly significant increase in the yield of fully developed osteosarcomas with increased amounts of 239Pu for both modes of injection. Osteosarcomas too small to be diagnosed radiographically were also seen in many bones and small but significant yields of myeloid leukaemia were seen in animals given plutonium. Although more myeloid leukaemia was seen in the mice given plutonium in divided amounts than in those given the plutonium in a single injection it could not be shown that multiple injection significantly affected the yield of either late effect.

Animals↗

Long-term effects of low-level 239Pu contamination on murine bone-marrow stem cells and their progeny.

The effects of long-term internal contamination with 13.3 kBq kg-1 239Pu injected intravenously were studied in 10-week-old ICR (SPF) female mice. Radiosensitivity of spleen colony-forming units (CFU-S) and 125IUdR incorporating into proliferating cells of vertebral bone marrow and spleens were determined in plutonium-treated and control animals one year after nuclide injection. The CFU-S in 239Pu-treated mice were more sensitive to X-rays (D0 = 0.52 +/- 0.01 Gy) than in controls (D0 = 0.84 +/- 0.02 Gy). 125IUdR incorporation into bone marrow and spleen cells was reduced after plutonium contamination. At one year following plutonium injection, the occurrence of chromosome aberrations was evaluated in metaphase figures of femoral bone marrow cells. The frequency of aberrations increased early after plutonium treatment, at later intervals it tended to decrease but not below the control level. While the relative numbers of vertebral marrow CFU-S decreased significantly, but only to 86 per cent of normal, cellularity of vertebral bone marrow, peripheral blood counts and survival of 239Pu-treated mice did not differ from the control data.

Alpha Particles↗

Analysis of symmetrical translocations for retrospective biodosimetry in radiation workers of the Mayak nuclear-industrial complex (Southern Urals) using FISH-chromosome painting.

PURPOSE: Frequencies of symmetrical translocations were determined by fluorescence in situ hybridization (FISH) for retrospective biodosimetry in workers occupationally exposed to external gamma-rays and internal plutonium at the Mayak nuclear-industrial complex (Southern Urals, Russia). MATERIALS AND METHODS: Chromosome analyses were carried out on peripheral lymphocytes from 75 Mayak workers who had received their main exposures between 1948 and 1963. Cumulative external gamma-ray doses between 0.02 and 9.91 Sv and plutonium burdens ranging between 0.26 and 18.5 kBq are reported. As controls, 33 unexposed persons from non-contaminated areas of the Southern Urals were used. Whole-chromosome painting probes for chromosomes 1, 4 and 12 were used simultaneously with a pancentromeric probe. RESULTS: Compared with the control group, a significantly elevated translocation frequency was found for the total study group and for either of two subsets with (48 subjects) and without (27 subjects) plutonium incorporation. The dicentric frequency was not significantly different from the control level. In the pooled data set, translocation frequencies showed a significant dependence on cumulative external gamma-ray doses. Plutonium uptake had no substantial influence. Individual dose estimates for 21 cases exhibiting at least five translocations ranged between 0.5 and 1.8 Gy, which is substantially lower than the workers' registered personal doses. CONCLUSION: At 35-40 years after protracted exposure to low-dose rate external gamma-rays, the postulated lifetime stability of translocations cannot be confirmed. Apparently, the natural loss of translocation-bearing peripheral lymphocytes cannot be fully compensated so that a temporal decline even of transmissible aberrations takes place. As a consequence, individual retrospective biodosimetry estimates cannot be obtained reliably from the remaining fraction of translocations.

Aged↗

Fallout 239/240Pu and 238Pu in human tissues from the Federal Republic of Germany.

To determine the present level of plutonium in human tissues of people in the F.R.G., due solely to fallout from weapons testing, 30 sets of tissues and bones from Munich residents were obtained at autopsy. Each set of tissues consisted of the entire lung, the entire liver, 300 g vertebrae, 300 g ribs and the lymph nodes. All subjects were males, born before 1940. Wet ashing, followed by solvent extraction, electrodeposition, and alpha-spectrometry were used to isolate and quantitate the plutonium isotopes present. The median concentrations of 239/240Pu (in fCi/kg wet weight) observed were: livers (530), vertebrae (92), ribs (73), lymph nodes (58) and lungs (28). The ratio of 238Pu/239/240Pu (in %) was livers 3.5, lungs 5.6, ribs 4.0 and vertebrae 3.2. Age trends for the plutonium concentration in livers, lungs, vertebrae and ribs were not observable. Possible correlations between the plutonium concentrations in livers, lungs and bones are discussed. The results are in many respects similar to observations in the U.S.A. and Southern Finland.

Adult↗

Measured 234,238U and fallout 239,240Pu in human bone ash from Nepal and Australia: skeletal alpha dose.

Human bone samples from Nepal and Australia were analyzed for isotopic uranium and fallout plutonium. The Nepalese samples were obtained for a 3-yr period (1976-78) while the Australian samples are representative of a single year (1977). The surface air plutonium concentrations for the latitude bands of these countries were either measured and/or estimated from 1954 through 1978. With the plutonium air concentrations and age-dependent breathing rates as input data, the measured human bone results were compared with skeletal estimates derived from the ICRP Task Group Inhalation Model, and the agreement was found to be reasonably good. The measured isotopic uranium concentrations in these samples provide a benchmark against which to assess fallout plutonium based upon a comparison of the skeletal alpha radiation dose from a natural actinide to these populations.

Adolescent↗

Long-term 238Pu and 239Pu retention and organ distribution in mice at low doses.

The 238Pu and 239Pu distribution in femur, liver, kidneys and testes and the retention function in the skeleton and liver have been studied in about 50 (C57 BL X C3H) F1 male mice. Groups of about 5-10 male mice were sacrificed from 10 to 800 days postinjection to cover their entire life span. All animals were injected intravenously with monomeric solutions of plutonium (1% trisodium citrate at pH 6.5) at doses of the order 7-15 kBq/kg body weight. The low levels of plutonium have been measured by direct counting in the entire animals and by radiochemical methods in the various tissues and organs. Significant differences between 238Pu and 239Pu were not observed at the injected doses used. The following proportions of the injected doses are retained in mice at the end of their life span: 12% in the skeleton, 0.7% in the liver, 0.1% in kidneys and 0.06% in gonads. Furthermore, the data have shown that (1) the long-term component of the plutonium skeleton retention in mice has a biological half-time that is much longer than their average life span; and (2) the long-term component of the plutonium liver retention in mice has a biological half-time of about 350 days.

Animals↗

In-line Kevlar filters for microfiltration of transuranic-containing liquid streams.

The Department of Energy Rocky Flats Plant has numerous ongoing efforts to minimize the generation of residue and waste and to improve safety and health. Spent polypropylene liquid filters held for plutonium recovery, known as "residue," or as transuranic mixed waste contribute to storage capacity problems and create radiation safety and health considerations. An in-line process-liquid filter made of Kevlar polymer fiber has been evaluated for its potential to: (1) minimize filter residue, (2) recover economically viable quantities of plutonium, (3) minimize liquid storage tank and process-stream radioactivity, and (4) reduce potential personnel radiation exposure associated with these sources. Kevlar filters were rated to less than or equal to 1 mu nominal filtration and are capable of reducing undissolved plutonium particles to more than 10 times below the economic discard limit, however produced high back-pressures and are not yet acid resistant. Kevlar filters performed independent of loaded particles serving as a sieve. Polypropylene filters removed molybdenum particles at efficiencies equal to Kevlar filters only after loading molybdenum during recirculation events. Kevlars' high-efficiency microfiltration of process-liquid streams for the removal of actinides has the potential to reduce personnel radiation exposure by a factor of 6 or greater, while simultaneously achieving a reduction in the generation of filter residue and waste by a factor of 7. Insoluble plutonium may be recoverable from Kevlar filters by incineration.

Pilot Projects↗

Past radionuclide releases from routine operations at Rocky Flats.

The Colorado Department of Public Health and Environment sponsored a study to reconstruct contaminant doses to the public from operations at the Rocky Flats nuclear weapons facility. This analysis of routine releases of plutonium and uranium, the principal radioactive materials used at the plant, was part of the Colorado Department of Public Health and Environment study. Historical radionuclide monitoring and data handling practices are characterized and uncertainties are quantified. Estimates of the annual release of plutonium and uranium are provided for the period from 1953 to 1989. Off-site airborne concentrations and deposition of plutonium and uranium associated with the releases are estimated, along with the highest doses for off-site populations. The predicted effective doses from the routine release of plutonium and uranium from Rocky Flats for a person residing near the plant boundary between 1953 and 1989 are very small.

Air Pollutants, Radioactive↗

Assessment of need for transport tubes when continuously monitoring for radioactive aerosols.

Aerosol transport tubes are often used to draw aerosol from desirable sampling locations to nearby air sampling equipment that cannot be placed at that location. In many plutonium laboratories at Los Alamos National Laboratory, aerosol transport tubes are used to transport aerosol from the front of room ventilation exhaust registers to continuous air monitors (CAMs) that are mounted on nearby walls. Transport tubes are used because past guidance suggests that extraction of aerosol samples from exhaust locations provides the most sensitive and reliable detection under conditions where the rooms have unpredictable release locations and significant spatial variability in aerosol concentrations after releases, and where CAMs cannot be located in front of exhaust registers without blocking worker walkways. Despite designs to minimize particle loss in tubes, aerosol transport model predictions suggest losses occur lowering the sensitivity of CAMs to accidentally released plutonium aerosol. The goal of this study was to test the hypotheses that the reliability, speed, and sensitivity of aerosol detection would be equal whether the sample was extracted from the front of the exhaust register or from the wall location of CAMs. Polydisperse oil aerosols were released from multiple locations in two plutonium laboratories to simulate plutonium aerosol releases. Networked laser particle counters (LPCs) were positioned to simultaneously measure time-resolved aerosol concentrations at each exhaust register (representative of sampling with transport tubes) and at each wall-mounted CAM location (representative of sampling without transport tubes). Results showed no significant differences in detection reliability, speed, or sensitivity for LPCs positioned at exhaust locations when compared to LPCs positioned at the CAM wall location. Therefore, elimination of transport tubes would likely improve CAM performance.

Aerosols↗

Effects of gadolinium on the retention and translocation of 239Pu-hydroxide.

The effect of gadolinium on the lung retention, excretion, and translocation of plutonium was studied in rats instilled intratracheally with plutonium hydroxide with and without gadolinium. Three types of plutonium hydroxide were prepared: pure 239Pu-hydroxide colloid, that containing a high concentration of gadolinium, and that containing a low concentration of gadolinium. The lung retention of 239Pu was higher and the fecal excretion was lower in the rats administered 239Pu-hydroxide containing a high concentration of gadolinium than those administered pure 239Pu-hydroxide colloid. The translocation of 239Pu from lung to other organs including the liver, spleen, femur, and kidney was not affected by gadolinium. The cytological examination of bronchoalveolar lavage cells showed that the administration of 239Pu-hydroxide containing a high concentration of gadolinium induced the inflammatory reactions in the lung. The delayed alveolar clearance of plutonium in the rats administered 239Pu-hydroxide colloid containing a high concentration of gadolinium may be attributable to the change in physicochemical characteristics of colloid and the inflammation induced in the lung by gadolinium.

Animals↗

Long-term behavior of 239Pu, 241Am and 233U in different bones of one-year-old rats: macrodistribution and macrodosimetry.

Female and male rats of the Sprague-Dawley strain, aged about 13 months, were injected intravenously with monomeric 239Pu-(30.7 kBq/kg), 241Am-(54.8 kBq/kg) or 233U-citrate (56.6 kBq/kg) and killed between 7 and 540 days after injection. In both sexes the wet skeletal weight was proportional to body weight; however, the skeletal weight of female rats remained constant, whereas the skeletal weight, and body weight, of male rats increased as a function of age. The initial skeletal deposition decreased in the order 239Pu greater than 241Am greater than 233U and for americium and uranium was greater in male rats. The 'half-time' of retention of plutonium and americium was considerably greater than 1 year but the corresponding values for uranium were 140 (females) and 80 (males) days. The relative concentration of the radionuclides in the skeleton varied between 0.2 and 2.0, the variation was greatest for plutonium and lowest for americium and decreased with increasing time after injection. For calculation of the nuclide content of the whole skeleton the most suitable reference bone was found to be the humerus in the case of uranium, and the femur and humerus for plutonium and americium. The cumulative mean skeletal absorbed radiation dose 1 year after injection decreased in the order 239Pu greater than 241 Am greater than 233U; for plutonium it was equal for both sexes, whereas for americium and uranium it was 1.5 times higher in male than in females rats. In the individual bones the cumulative dose was greatest in the vertebral column, except the tail, and lowest in the paws.

Americium↗

[The applicability of the concept of morpho-physiologic metabolic factors to the modification of the distribution of 239Pu deposited in the respiratory organs].

At the stage of intensive resorption of plutonium from lungs to blood the competitive per os administration of an iron preparation increased plutonium excretion from blood. As a result, soft tissues were enriched with plutonium at an early stage of metabolism. However, at the end of the experiment (30 days) the radionuclide content of soft tissues dropped to control values. Simultaneously, the share of plutonium deposited in bone tissue decreased considerably and that of the radionuclide eliminated from the body increased throughout the entire period of observation.

Administration, Oral↗

Pu(VI) hydrolysis: further evidence for a dimeric plutonyl hydroxide and contrasts with U(VI) chemistry.

A significant fraction of plutonium that is soluble in environmental waters and other aqueous solutions can be present as complexes of plutonyl, PuO2(2+). Few thermodynamic data are available for this ion, representing a problematic gap in plutonium chemistry and in the forecasting of radionuclide behavior under contamination and nuclear repository conditions. To address this need and more accurately determine the stoichiometry and stability of the basic hydrolytic products, we completed complimentary potentiometric and spectrophotometric studies of plutonium(VI) hydrolysis over the concentration range of 10(-2) to 10(-5) M Pu(VI). Dinuclear hydroxide species (PuO2)2(OH)2(2+) and (PuO2)2(OH)4(0)(aq) with hydrolysis constants log beta(2,2) = -7.79 +/- 0.20 and log beta(4,2) = -19.3 +/- 0.5 are indicated in all experiments of millimolar Pu(VI), 0.10 M NaNO3 solutions at 25 degrees C. At lower Pu(VI) concentrations, at and below 10(-4) M, the monomeric species PuO2OH+ and PuO2(OH)2(0)(aq) form with hydrolysis constants of log beta(1,1) = -5.76 +/- 0.07 and log beta(2,1) = -11.69 +/- 0.05, respectively. Distinct optical absorbance bands at 842 and 845 nm are reported for the mononuclear and dinuclear first hydrolysis species. Standard hydrolysis constants at zero ionic strength were calculated from the experimentally determined constants using the specific ion interaction theory. The Pu(VI) hydrolysis species and constants are compared with results from previous studies for plutonium and uranium. Major differences between uranyl and plutonyl hydrolysis are described.

Journal Article↗

Fuzzy-probabilistic model for risk assessment of radioactive material railway transportation.

Transportation of radioactive materials is obviously accompanied by a certain risk. A model for risk assessment of emergency situations and terrorist attacks may be useful for choosing possible routes and for comparing the various defence strategies. In particular, risk assessment is crucial for safe transportation of excess weapons-grade plutonium arising from the removal of plutonium from military employment. A fuzzy-probabilistic model for risk assessment of railway transportation has been developed taking into account the different natures of risk-affecting parameters (probabilistic and not probabilistic but fuzzy). Fuzzy set theory methods as well as standard methods of probability theory have been used for quantitative risk assessment. Information-preserving transformations are applied to realise the correct aggregation of probabilistic and fuzzy parameters. Estimations have also been made of the inhalation doses resulting from possible accidents during plutonium transportation. The obtained data show the scale of possible consequences that may arise from plutonium transportation accidents.

Body Burden↗

Actinides in deer tissues at the rocky flats environmental technology site.

Limited hunting of deer at the future Rocky Flats National Wildlife Refuge has been proposed in U.S. Fish and Wildlife planning documents as a compatible wildlife-dependent public use. Historically, Rocky Flats site activities resulted in the contamination of surface environmental media with actinides, including isotopes of americium, plutonium, and uranium. In this study, measurements of actinides [Americium-241 (241Am); Plutonium-238 (238Pu); Plutonium-239,240 (239,240Pu); uranium-233,244 (233,234U); uranium-235,236 (235,236U); and uranium-238 (238U)] were completed on select liver, muscle, lung, bone, and kidney tissue samples harvested from resident Rocky Flats deer (N = 26) and control deer (N = 1). In total, only 17 of the more than 450 individual isotopic analyses conducted on Rocky Flats deer tissue samples measured actinide concentrations above method detection limits. Of these 17 detects, only 2 analyses, with analytical uncertainty values added, exceeded threshold values calculated around a 1 x 10(-6) risk level (isotopic americium, 0.01 pCi/g; isotopic plutonium, 0.02 pCi/g; isotopic uranium, 0.2 pCi/g). Subsequent, conservative risk calculations suggest minimal human risk associated with ingestion of these edible deer tissues. The maximum calculated risk level in this study (4.73 x 10(-6)) is at the low end of the U.S. Environmental Protection Agency's acceptable risk range.

Animals↗

Complex chromosome aberrations persist in individuals many years after occupational exposure to densely ionizing radiation: an mFISH study.

Long-lived, sensitive, and specific biomarkers of particular mutagenic agents are much sought after and potentially have broad applications in the fields of cancer biology, epidemiology, and prevention. Many clastogens induce a spectrum of chromosome aberrations, and some of them can be exploited as biomarkers of exposure. Densely ionizing radiation, for example, alpha particle radiation (from radon or plutonium) and neutron radiation, preferentially induces complex chromosome aberrations, which can be detected by the 24-color multifluor fluorescence in situ hybridization (mFISH) technique. We report the detection and quantification of stable complex chromosome aberrations in lymphocytes of healthy former nuclear-weapons workers, who were exposed many years ago to plutonium, gamma rays, or both, at the Mayak weapons complex in Russia. We analyzed peripheral-blood lymphocytes from these individuals for the presence of persistent complex chromosome aberrations. A significantly elevated frequency of complex chromosome translocations was detected in the highly exposed plutonium workers but not in the group exposed only to high doses of gamma radiation. No such differences were found for simple chromosomal aberrations. The results suggest that stable complex chromosomal translocations represent a long-lived, quantitative, low-background biomarker of densely ionizing radiation for human populations exposed many years ago.

Chromosome Aberrations↗