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PubMed2006

Colloid transport of plutonium in the far-field of the Mayak Production Association, Russia.

Sorption of actinides, particularly plutonium, onto submicrometer-sized colloids increases their mobility, but these plutonium colloids are difficult to detect in the far-field. We identified actinides on colloids in the groundwater from the Mayak Production Association, Urals, Russia; at the source, the plutonium activity is approximately 1000 becquerels per liter. Plutonium activities are still 0.16 becquerels per liter at a distance of 3 kilometers, where 70 to 90 mole percent of the plutonium is sorbed onto colloids, confirming that colloids are responsible for the long-distance transport of plutonium. Nano-secondary ion mass spectrometry elemental maps reveal that amorphous iron oxide colloids adsorb Pu(IV) hydroxides or carbonates along with uranium carbonates.

Journal Article↗
PubMed1979

Synthesis and therapeutic testing of mono- and dialkyl esters of pentetic (diethylenetriaminepentaacetic) acid for decorporation of polymeric plutonium.

The synthesis, characterization, and therapeutic evaluation of a series of partially esterified derivatives of pentetic (diethylenetriaminepentaacetic) acid are reported. These compounds were prepared in an attempt to promote increased decorporation of insoluble colloidal forms of plutonium, which are removed by pentetic acid alone. The dimethyl, diethyl, dibutyl, dioctyl, monoethyl esters were synthesized by reaction of the appropriate alcohol with the dianhydride of pentetic acid. These esters were injected intravenously into mice as their calcium chelates in saline. None of the esters was effective in removing plutonium from the liver. All esters removed approximately 20% of the plutonium in the skeleton. However, when the esters were given together with pentetic acid, only the dioctyl ester showed enhanced removal of plutonium compared to pentetic acid alone. The small increase in effectiveness and the increased acute toxicity make these esters of limited practical interest in plutonium decorporation therapy.

Animals↗
PubMed2002

Estimates of radiological risk from a terrorist attack using plutonium.

The possible use of radioactivity dispersal devices by terrorist groups has been recently reported in the news. In this paper, we discuss the threat of terrorist attacks by plutonium, with particular attention to the dispersal of plutonium by explosion or fire. Doses resulting from inhalation of radioactive aerosol induced by a plutonium explosion or fire are simulated using a Gaussian plume model (the HOTSPOT code) for different meteorological conditions. Ground contamination and resuspension of dust are also considered in the simulations. Our simulations suggest that acute effects from a plutonium dispersal attack are very unlikely. For late stochastic effects, the explosion poses a greater hazard than fire. However, even in the worst-case scenario, the dispersed plutonium would cause relatively few excess cancers (around 80 in a city of 2 million inhabitants) after many years from the explosion, and these excess cancers would remain undetected against the background of cancer fatalities.

Administration, Inhalation↗
PubMed2005

Lung cancer in Mayak workers: interaction of smoking and plutonium exposure.

Lung cancer mortality among 5,058 male workers of the Mayak Production Association has been analyzed with emphasis on the interaction of smoking and radiation exposure by using the two-step clonal expansion (TSCE) model of carcinogenesis. The cohort consists of all Mayak workers with known smoking status, who were employed in the period 1948-1972, and who either had the plutonium concentration in urine measured or who worked in the reactors, where plutonium exposure was negligible. Those who died during the first two years after the first urine sampling were excluded. The follow-up extended until the end of 1998. During this time, 2,176 workers died, including 244 lung cancer cases. Mayak workers were exposed to external (gamma and neutron) radiation, and in the radiochemical and plutonium plants to plutonium. In the preferred TSCE model, internal radiation and smoking act on the clonal expansion of pre-carcinogenic clones. Assuming a plutonium radiation weighting factor of 20, the excess relative risk per lung dose was estimated to be 0.11 (95% CI: 0.08; 0.17) Sv(-1). Most of the lung cancer deaths are found to be due to smoking. The second main factor is the interaction of smoking and internal radiation. The model is sub-multiplicative in relative risks due to smoking and radiation. In a multiplicative version of the TSCE model, internal radiation acts on initiation and transformation rates. This model version agrees with conventional epidemiological risk models, because it also suggests a higher risk estimate than the preferred TSCE model. However, it fits the data less well than the preferred model.

Biophysical Phenomena↗
PubMed2006

Predicting plutonium decorporation efficacy after intravenous administration of DTPA formulations: Study of pharmacokinetic-pharmacodynamic relationships in rats.

PURPOSE: The objectives of this study were: 1) to assess the relationship between plutonium decorporation (increased excretion and reduced retention in main organs of deposition) induced by intravenous liposome formulations of the chelating agent diethylene triamine pentaacetic acid (DTPA) and its pharmacokinetics, and 2) to model the renal excretion of plutonium after treatment with liposome-encapsulated DTPA in order to predict its efficacy and to optimise treatment schedules. MATERIALS AND METHODS: Pharmacokinetic parameters from plasma or urinary data (days 0-16 sample collections) were modelled versus decorporation efficacy, and best correlations were selected for their goodness of fit. RESULTS: The plutonium decorporation enhancement by DTPA liposomal formulations was well described by logistic models and the best correlation was observed with the area under the DTPA concentration curve of each formulation. The plutonium urinary excretion rates decreased mono-exponentially as a function of time after a single dose and the proposed model allowed a simple determination of the elimination half-life of the Pu-DTPA complex, a reasonably good approximation of the long-term efficacy of the treatments from truncated urinary data. CONCLUSIONS: Both liposomal formulations of chelating agents and pharmacokinetic approaches to plutonium decorporation should be helpful in optimising treatment protocols.

Animals↗
PubMed1994

The gastrointestinal absorption of plutonium and americium in rats and guinea pigs after ingestion of dusts from the former nuclear weapons site at Maralinga: implications for human exposure.

The gastrointestinal absorption of plutonium and americium present in dusts from the Maralinga test sites in South Australia has been measured as an input to dose assessments. The materials studied were from three different areas, designated Taranaki (Q380II), TM100 (10/2) and N. Plume (26). The three dusts were fed to groups of rats, mixed with their normal food. The Taranaki and TM100 dusts were also fed to guinea pigs, as a suspension in water. Expressed as fractional absorption from the gastrointestinal tract (f1), the values obtained for plutonium were 2 x 10(-6) and 8 x 10(-6) for Taranaki dust in rats and guinea pigs, respectively, 3 x 10(-6) and 10(-5) for TM100 dust in rats and guinea pigs, respectively, and 2 x 10(-6) for N. Plume dust in rats. The f1 values obtained for americium were 3 x 10(-6) and 2 x 10(-5) for Taranaki dust in rats and guinea pigs, respectively, 10(-5) and 5 x 10(-5) for Taranaki dust in rats and guinea pigs, respectively, and 10(-5) for N. Plume dust in rats. On the basis of these results, rounded f1 values used in the dose assessments were 10(-5) for plutonium and 10(-4) for americium, applying to all intakes of dust. These values compare with the International Commission on Radiological Protection recommendations of 10(-3) for unspecified chemical forms of both elements, 10(-4) for plutonium nitrate and 10(-5) for plutonium oxides. The effect of changes in f1 values on doses from 239Pu and 241Am is considered.

Air Pollutants, Radioactive↗
PubMed1995

Environmental plutonium in humans.

Although the current world inventory of plutonium is overwhelmingly man-made, it is important to recognize that 244Pu was a primeval radioelement and that 239Pu is formed continuously by spontaneous fission of 238U; the atom ratio U:Pu being about 10(11):1. It has been calculated that the human body has always carried a base load of, perhaps 10(3)-10(5) atoms (< 0.2 amol) of natural plutonium. Since 1945, the release of 239Pu into the environment from atmospheric nuclear weapons testing has added to this base load a civilization-related load which, at approximately 300 fmol, is at least 5 orders of magnitude greater. Within the human body plutonium is deposited mainly in the liver and skeleton where it appears to be retained tenaciously with half-times of many years. Based on 1970-1980 levels, environmental plutonium may give rise to alpha-particle radiation doses of approximately 3-7 microSv/a in human bone and approximately 10-20 microSv/a in liver, doses which from our present understanding of the radio-and chemical toxicity of plutonium are far too small to cause any recognizable health effects.

Adult↗
PubMed2004

Plutonium isotopes in the lower reaches of the River Rhône over the period 1945-2000: fluxes towards the Mediterranean Sea and sedimentary inventories.

Plutonium isotopes in the Rhône River originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. Due to a new treatment process applied to the liquid effluents, a decrease of two orders of magnitude in the industrial plutonium discharged into the River Rhône has been registered from 1991. Today, 238Pu industrial inputs to the River Rhône are still about 10 times higher than those derived from global fallout, while 239+240Pu inputs from industrial and global fallout sources are of similar importance, i.e. 1 GBq y(-1). Our results indicate that the river sedimentary compartment act either as a sink or a delayed-source term of plutonium for the freshwaters depending on the hydraulic regime and flood events. This compartment may then represent an important industrial delayed-source term for the River Rhône freshwaters in the coming years as the Marcoule reprocessing plant is being dismantled. These results were obtained from samples collected from the lower course of the River Rhône over the 1987-1998 period and analysed for 238Pu and 239+240Pu activities. Both river sedimentary inventories of plutonium isotopes and effective outputs from the River Rhône towards the Gulf of Lions have been estimated for each year over the 1945-2000 period. Regarding 239+240Pu, the sedimentary inventory accumulated since 1945 is estimated to be 172+/-35 GBq. If mobile, this amount represents a significant delayed-source term of plutonium on the scale of the Rhône watershed.

Disasters↗
PubMed2005

Plutonium in the air in Kurchatov, Kazakhstan.

Weekly air samples of 25000 m(3) volume were taken with two air samplers over a period of one year in 2000-2001 in the town of Kurchatov in Kazakhstan. For another three-month period in 2001, the samplers were run in the city of Astana, about 500 km west of Kurchatov. (137)Cs, Pu and U concentrations were determined from the filters. Pu activities in Kurchatov varied in a 100-fold range; median (239,240)Pu activities were 100 nBq/m(3) and (238)Pu activities 34 nBq/m(3). The corresponding values for Astana were considerably lower: 29 and 9 nBq/m(3), respectively, and in half of the filters the (238)Pu activity was below the detection limit. Plutonium concentration correlated with the amount of dust retained on the filters only at the highest dust loads. Also no correlation between wind speed and the plutonium activity in the filters was observed. Thus, resuspension does not seem to be the mechanism responsible for the airborne plutonium. No clear seasonal variation of Pu air concentration was observed, though levels were somewhat elevated in February to April. There was no correlation between the plutonium and (137)Cs concentrations. In most of the filters the cesium concentration was below the detection limit, but in those filters where it could be detected the cesium concentration was practically constant at 3.9+/-1.6 microBq/m(3). Dose estimation for the inhalation of the airborne plutonium gave a low value of 0.018 microSv/a for the inhabitants in Kurchatov, which is about a thousand times lower than the dose caused by the naturally occurring (210)Po. Air parcel trajectory analysis indicated that the observed Pu activities in the air could not unambiguously be attributed to the most contaminated areas at the Semipalatinsk Test Site.

Air Pollutants, Radioactive↗
PubMed2001

The availability of plutonium and americium in Irish Sea sediments for re-dissolution.

The availability of plutonium and americium, for re-dissolution from offshore sediments into Irish Sea water, has been examined. Sediments collected from the mud-patch near the Cumbrian coast were characterized in terms of spatial location, particle size, partitioning of radionuclides with respect to physico-chemical bonds and availability of actinides for release into seawater. Sequential extraction investigations revealed that plutonium was predominantly associated with strongly bound sesquioxide and organic complex fractions. Americium was associated mainly with the organic complex fraction, but a significant fraction was in carbonate form. Sediment/water re-dissolution experiments with and without stirring were compared to simulate the effect of disturbing bed sediment. After 1 week, neither set of re-dissolution data provided significant trends between dissolved activity and time. Stirred systems appeared to release 2.5 times more plutonium and americium into seawater than unstirred systems. Measured 239,240Pu and 241Am distribution coefficients (Kd values) were both typically approximately 10(5) l kg(-1). 241Am Kd values are an order of magnitude lower than previously reported for the north-eastern Irish Sea, but similar to western Irish Sea values. Overall, the fractions of plutonium and americium available for re-dissolution from bed sediment are very low at < 0.1%, with proportionally more plutonium being released than americium. These findings lend further support for the extrapolation of laboratory-derived information to environmental conditions.

Actinoid Series Elements↗
PubMed2001

Bioaccumulation and distribution of plutonium in fish from Gdansk Bay.

In this paper, the results of 238Pu and 239 + 240Pu determinations in four representative species of Baltic fish collected in Gdansk Bay; flounder, herring, cod and sprat, are presented and discussed. The plutonium isotopes are amongst the more radiotoxic nuclides. In the marine environment, the highest concentrations of plutonium are found in the sediments, but the complex biogeochemical cycle of the element means that it is also found in all other compartments. The activities of the fish samples were measured using alpha spectrometry and the concentrations of plutonium 238Pu and 239 + 240Pu were estimated for particular organs and tissues and the whole body. The 239 + 240Pu concentrations for fish species were: flounder 0.94 mBq kg-1 w.w., herring 2.22 mBq kg-1 w.w., cod 2.35 mBq kg-1 w.w. and sprat 0.33 mBq kg-1 w.w. On the basis of the 238Pu/239 + 240Pu activity ratio in the organs and tissues, the proportion of Chernobyl-derived plutonium in the Baltic Sea was calculated. The lowest values of Chernobyl plutonium were accumulated in flounder stomach, herring skin, cod intestine, the highest in cod gills and skin.

Animals↗
PubMed2002

Transport of plutonium in surface and sub-surface waters from the Arctic shelf to the North Pole via the Lomonosov Ridge.

New data on the levels and long-range transport of plutonium in the Arctic Ocean, recorded in the course of two expeditions to this zone in 1994 and 1996, are discussed in this paper. Specifically, approximately 100 plutonium measurements in surface and sub-surface water sampled at 58 separate stations throughout the Kara, Laptev and East Siberian Seas, as well as along latitudinal transects across the Lomonosov Ridge, are reported and interpreted in terms of the circulation pathways responsible for the transport of this element from the North Atlantic to the Arctic Shelf and into the Arctic interior. In addition, the behaviour of plutonium in its transit through the vast Arctic shelf seas to open waters under extreme environmental conditions is discussed in terms of the partitioning of plutonium between filtered (<0.45 microm) seawater and suspended particulate, and its association with colloidal matter. Finally, limited evidence of the presence of a colloidal plutonium component in Arctic waters subject to direct riverine input is adduced.

Arctic Regions↗
PubMed2003

Modelling the distribution of plutonium in the Pacific Ocean.

An Oceanic General Circulation Model (OGCM) including a plutonium scavenging model as well as an advection-diffusion model has been developed for modelling the distribution of plutonium in the Pacific Ocean. Calculated 239, 240Pu water profile concentrations and 239, 240Pu inventories in water and sediment of the Pacific Ocean have showed a reasonable agreement with the experimental results. The presence of local fallout plutonium in central North Pacific waters has been confirmed. The observed 240Pu/239Pu mass ratios confirm that plutonium originating from local fallout from nuclear weapons tests carried out at Bikini and Enewetak Atolls is more rapidly removed from surface waters to deeper waters than plutonium originating from global fallout. The developed OGCM can be used for modelling the dispersion of other non-conservative tracers in the ocean as well.

Diffusion↗
PubMed1999

Selective removal of plutonium 238 from a canal sediment using a carbonate-chelant soil washing technology (ACT*DE*CON).

The Mound laboratory site in Miamisburg, OH, a former plutonium processing facility, contains approximately 40000 yd(3) (30,580 m3) of plutonium- and thorium-contaminated soils and sediments at levels that require remediation. Existing applicable remediation technologies are unsatisfactory, because they are expensive and do not provide volume reduction. ACT*DE*CON is a chemical soil leaching technology for the treatment of soils that utilizes contaminant dissolution via dilute selective solutions to remove radionuclides. In bench-scale tests, process parameters were developed for the optimal treatment of the Miami Erie Canal soil at the Mound site, combining the maximum plutonium removal with an acceptable amount of soil dissolution and minimizing the costs of reagents. Parameters evaluated included soil to extractant mass ratio, temperature, rinse solution composition, kinetics, and the application of several dewatering aids. Plutonium removal rates of >95% were achieved, and the residual plutonium in the treated soil proved to be very immobile-confirming that the process had removed the most accessible species of the radionuclide. Currently being tested at Mound is an engineering scale-up that includes an attrition scrubber, a counter-current extractor, and a reverse osmosis system. Economic evaluations based on bench-scale results put the treatment cost at US$278/yd(3) (US$364/m3), compared to US$350/yd(3) (US$458/m3) for the 'box-and-bury' baseline alternative treatment system.

Carbonates↗
PubMed1999

Cancer mortality and morbidity among plutonium workers at the Sellafield plant of British Nuclear Fuels.

The mortality of all 14 319 workers employed at the Sellafield plant of British Nuclear Fuels between 1947 and 1975 was studied up to the end of 1992, and cancer incidence was examined from 1971 to 1986, in relation to their exposures to plutonium and to external radiation. The cancer mortality rate was 5% lower than that of England and Wales and 3% less than that of Cumbria. The significant excesses of deaths from cancer of the pleura and thyroid found in an earlier study persist with further follow-up (14 observed, 4.0 expected for pleura; 6 observed, 2.2 expected for thyroid). All of the deaths from pleural cancer were among radiation workers. For neither site was there a significant association between the risk of the cancer and accumulated radiation dose. There were significant deficits of deaths from cancers of mouth and pharynx, liver and gall bladder, and larynx and leukaemia when compared with the national rates. Among all radiation workers, there was a significant positive association between accumulated external radiation dose and mortality from cancers of ill-defined and secondary sites (10-year lag, P = 0.04), leukaemia (no lag, P = 0.03; 2-year lag, P = 0.05), multiple myeloma (20-year lag, P = 0.02), all lymphatic and haematopoietic cancers (20-year lag, P= 0.03) and all causes of death combined (20-year lag, P= 0.008). Among plutonium workers, there were significant excesses of deaths from cancer of the breast (6 observed, 2.6 expected) and ill-defined and secondary cancers (29 observed, 20.1 expected). No significant positive trends were observed between the risk of deaths from cancers of any specific site, or all cancers combined, and cumulative plutonium and external radiation doses. For no cancer site was there a significant excess of cancer registrations compared with rates for England and Wales. Analysis of trends in cancer incidence showed significant increases in risk with cumulative plutonium plus external radiation doses for all lymphatic and haematopoietic neoplasms for 0-, 10- and 20-year lag periods. Taken as a whole, our findings do not suggest that workers at Sellafield who have been exposed to plutonium are at an overall significantly increased risk of cancer compared with other radiation workers.

Adult↗
PubMed1984

The absorption of ingested neptunium, plutonium and americium in newborn hamsters.

Hamsters aged 1, 4, 7, 22 and 30 days were given oral doses of either plutonium-239 citrate or americium-241 nitrate. The values of gastrointestinal absorption obtained were 3.5, 1.4, 0.04, 0.007 and 0.003 per cent, respectively, for plutonium and 4.5, 1.7, 0.5, 0.006 and 0.02 per cent, respectively, for americium, compared with values in adults of 0.01 per cent for plutonium and 0.05 per cent for americium. The absorption of neptunium was measured in hamsters aged 2 and 4 days and values of 2.3 and 1.7 per cent, respectively, were obtained for 239Np as the nitrate and 5.5 and 2.1 per cent, respectively, for 239Np as the bicarbonate compared with the values in adults of 0.02 per cent for both chemical forms. Thus, the absorption of plutonium, americium and neptunium at 1-2 days of age was about 100 times greater than in adults. The results for plutonium and americium show that absorption decreased rapidly with age over the suckling period. The values of absorption obtained at the time of weaning at 22 days were lower than in adults.

Aging↗
PubMed1986

Effects of plutonium-239 on haemopoiesis. I. Quantitative and qualitative changes in CFU-S in different regions of the mouse femur and vertebrae.

Mice were injected with plutonium-239 (960 Bq/mouse) and, over a period of four months, the response of haemopoietic tissue and the self-renewal capacity of its stem cells was monitored. Cellularity, CFU-S concentration and self-renewal capacity were measured in five different regions of bone and marrow--axial and marginal marrow of the femoral shaft, femur shaft, proximal and distal ends of the femur shaft and vertebrae. Cellularities were little affected by plutonium but CFU-S were reduced in all regions, most severely in the bone shaft and marginal marrow due to the initial deposition of plutonium on the bone surface, by four days. The reduction in axial CFU-S, however, was due probably to a relatively long plasma half-life resulting from the tendency of plutonium to combine with plasma proteins. The capacity of CFU-S for self-renewal was reduced and remained low in all zones. Thus, although the highly self-renewing axial CFU-S were depleted, and remained so, due probably to a longer term redistribution of plutonium throughout the marrow, additional proliferation of the more mature CFU-S in the other zones kept their self-renewal low while replenishing their numbers and maintaining a normal cell output.

Alpha Particles↗
PubMed2003

Plutonium content of human placental tissues after occupational exposure.

The placenta and umbilical cord were obtained following a normal live delivery from a volunteer donor who had received an accidental inhalation intake of plutonium 12 years prior to her pregnancy (Case 0777). Her employer estimated the intake to be about 73 Bq Class W plutonium. Based on bioassay results and clearance models in use at that time, they calculated her body content at the beginning of pregnancy to be about 5.6 Bq with an average concentration of approximately 60 mBq kg(-1). The placenta and cord from this pregnancy, along with the placenta and cord from a donor with no known exposure to plutonium (Case 0835), were divided and assayed for plutonium by ultrasensitive fission track analysis at two collaborating laboratories. Placental 239Pu concentration values obtained by the two laboratories for Case 0777 agreed within a factor of 2 and were several-fold greater than for the control, Case 0835, as well as values that had been reported by others for unexposed populations. There was no elevated concentration of plutonium in the umbilical cord from the exposed person. The data yielded values of 0.16 and 0.27 for placental to maternal concentrations (CPl: CM) that were of the same order of magnitude as the value of 0.1 the ICRP calculated for intakes before pregnancy.

Body Burden↗