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PubMed2006

The structure and synthesis of plutonium(III) chlorides from aqueous solution.

The preparation and structure of three trivalent plutonium chloride compounds from aqueous solution is reported. Two of the three are plutonium tetraaquatetrachloro complexes exhibiting a cis and a trans arrangement of Cl about the Pu. The identification of the coordination number of 4 with respect to Cl and the isomerism are both unprecedented in actinide solution chemistry. The third complex is a hexaaquadichloro complex of Pu(III), predicted by available thermodynamic data.

Journal Article↗
PubMed2006

Emergent magnetic moments produced by self-damage in plutonium.

Plutonium possesses the most complicated phase diagram in the periodic table, driven by the complexities of overlapping 5f electron orbitals. Despite the importance of the 5f electrons in defining the structure and physical properties, there is no experimental evidence that these electrons localize to form magnetic moments in pure Pu. Instead, a large temperature-independent Pauli susceptibility indicates that they form narrow conduction bands. Radiation damage from the alpha-particle decay of Pu creates numerous defects in the crystal structure, which produce a significant temperature-dependent magnetic susceptibility, chi(T), in both alpha-Pu and delta-Pu (stabilized by 4.3 atomic percent Ga). This effect can be removed by thermal annealing above room temperature. By contrast, below 35 K the radiation damage is frozen in place, permitting the evolution in chi(T) with increasing damage to be studied systematically. This result leads to a two-component model consisting of a Curie-Weiss term and a short-ranged interaction term consistent with disorder-induced local moment models. Thus, it is shown that self-damage creates localized magnetic moments in previously nonmagnetic plutonium.

Journal Article↗
PubMed2006

Symmetry and stability of plutonium: the influence of electronic structure.

Using first-principles density-functional theory, we calculate the bond strengths between the 12 nearest neighbors in delta plutonium for both pure Pu and a Pu-3.7 at. % Ga alloy. Our results for pure Pu reveal a structure with the monoclinic space group Cm rather than face-centered cubic Fm3m, showing that the anomalously large anisotropy of delta plutonium is a consequence of greatly varying bond strengths between the 12 nearest neighbors. Further results for a Pu-3.7 at. % Ga alloy show that the nearest-neighbor bond strengths around a Ga atom are more uniform. Hence, our calculations address (i) why the ground state of Pu is monoclinic, (ii) why distortions of the delta phase are viable, with considerable implications for the behavior of the material as it ages due to anisotropic response to self-irradiation, and (iii) why Ga stabilizes face-centered cubic delta-Pu.

Journal Article↗
PubMed2005

mFISH analysis reveals complexity of chromosome aberrations in individuals occupationally exposed to internal plutonium: a pilot study to assess the relevance of complex aberrations as biomarkers of exposure to high-LET alpha particles.

We recently demonstrated that a significant proportion of apparently stable insertions induced after exposure to a mean of one alpha particle/cell, detected using three-color FISH, were part of larger unstable complexes when visualized by 24-color FISH. Interestingly, regardless of the long-term persistence capability of the cell, the complexity of each alpha-particle-induced complex appeared to be specific to the nuclear traversal of a single alpha particle. To assess whether aberrations of a similar complexity are observed in vivo and also to examine the usefulness of detecting such aberrations as a biomarker of chronic exposure to alpha particles, we have carried out a limited pilot study of Russian workers with large body burdens of alpha-particle-emitting plutonium. We found unstable cells containing non-transmissible complex aberrations in all of the plutonium-exposed subjects analyzed by mFISH. In addition, all of the complexes seen were consistent with those previously observed in vitro. Non-transmissible complex aberrations were more common than transmissible-type complexes, consistent with ongoing/chronic exposure, and insertions were dominant features of both types of complex. Accordingly, this preliminary study supports the proposal that aberration complexity and non-transmissibility are the major cytogenetic features of alpha-particle exposure that could potentially be exploited as a specific indicator of chronic exposures to high-LET alpha particles.

Biomarkers↗
PubMedDate not supplied

[Intensification of the excretory flow of plutonium-239 from the body in the late stage of its metabolism].

The paper deals with the effect of iron preparations on the excretion of plutonium 239 from a body at a later stage of the radionuclide metabolism. The experimental results show that oral administration of the iron preparation at a later stage of 239Pu metabolism enhances the radionuclide excretion both in urine and in faeces. On the basis of the results obtained the coefficients are calculated for 239Pu excretion in urine and faeces and for its content in the organs of deposition. This may be used for increasing the sensitivity of indirect dosimetry of plutonium-239 within the body.

Animals↗
PubMed1978

The movement of plutonium, americium, and curium through the food chain.

The actinides, plutonium, americium and curium, are being produced in increasing quantites as the nuclear programme is expanded. As these alpha-particle-emitting elements are hazardous to man there is considerable concern about the movement of these elements through the environment; The uptake of these elements from soil into the plants is low, as is the gastrointestinal concentration factor. Although there are complexing agents in the environment which have been shown to complex these elements there is no evidence that these complexing agents might bring about a concentration of actinides in the food chain of man.

Actinoid Series Elements↗
PubMed2001

Chemical speciation of plutonium in seawater.

Concentrations of particulate and dissolved plutonium in seawater were determined together with strong organic ligands (SOL) in particulate matter (PM). The concentration of particulate 239,240Pu in surface waters of the Western North Pacific ranged from 0.03 to 0.3 mBq m(-3) during the period from 1987 to 1997. The percentage of particulate Pu to total Pu in seawater was less than 10% in surface waters, whereas its portions were less than 1% in deep waters. In order to characterize particulate Pu in seawater, the relationships between particulate Pu, dissolved Pu and SOL concentrations in surface PM were examined. The result reveals that particulate Pu was linearly related to the SOL concentration independent of dissolved Pu concentration. Mass balance analysis suggests that a dominant chemical form of Pu in surface PM, which may exist as Pu(IV), is a complex with strong organic ligands in PM.

Pacific Ocean↗
PubMed1978

A review of parameter values used to assess the transport of plutonium, uranium, and thorium in terrestrial food chains.

A general methodology of predicting the food chain transport of atmospherically deposited radionuclides is reviewed with an emphasis on variation in parameter values important for realistic behavioral characterization of environmental releases of plutonium, uranium, and thorium. Parameters important to generic simulations of food chain transport, given a known constant deposition onto vegetation, include: fractional interception of particulates by vegetation, vegetation density, effective half-life of contamination on vegetation, soil-to-plant transfer factors, consumption rates by cattle and man, and transfer of nuclides from forage to meat and from forage to milk. Variation in these parameters, which has been encountered in field studies, is summarized. A partial reduction in the variation of predicted concentrations of actinides in foods can be accomplished by more accurately determining critical parameter values like fractional interception of deposition by vegetation, vegetation biomass, and the effective half-life of contamination on vegetation. Field research describing the site dependency and time dependency of probability density functions for model parameter values is needed to make probabilistic predictions concerning Pu, U, and Th transport in food chains and to reduce the uncertainty associated with model predictions and generic assessments of environmental impact.

Biological Transport↗
PubMed1984

The uptake of plutonium-238, 239, 240, americium-241, strontium-90 and caesium-137 into potatoes.

Transfer factors have been measured for 239 Pu + 240 Pu, 241 Am, 90 Sr and 137 Cs into potatoes grown in a blend of soil which included silt polluted with radioactive waste discharged into the Irish Sea. The experiment has been carried out over four seasons and attempts to assess the radiological consequences to the consumer which would arise if potatoes were to be grown in land heavily contaminated with the silt. During the course of the experiment plutonium and americium became less available for uptake, 90 Sr became slightly more available and 137 Cs remained nearly constant in its availability. The values of the transfer factors are among the lowest reported for these radionuclides into potatoes.

Americium↗
PubMed1993

Measurements of the gastrointestinal absorption and tissue distribution of plutonium, americium and polonium in experimental animals.

In order to set limits on environmental and occupational intakes of radionuclides, information is needed on their uptake and metabolism in man. Human data are very limited, particularly for long-lived alpha-emitting isotopes such as those of the actinides. Animal experiments are therefore an important source of data on the distribution of radionuclides in tissues, and the effects of factors such as subject age and the chemical form of elements on gastrointestinal absorption. The NRPB performs experimental programs using mainly rats and guinea pigs. In order to study the gastrointestinal absorption and tissue distribution of plutonium, americium and polonium, a variety of analytical techniques are employed. These include ion exchange and solvent extraction leading to alpha spectrometry and liquid scintillation counting. The investigation of low specific-activity environmental or industrial materials, and the very low bioavailability of elements such as the actinides, means that very low levels of activity have to be measured. Contamination at the dissection and tissue separation stage, as well as during the radiochemistry, has to be rigorously avoided. Where very detailed information is needed on the location of radionuclides within tissues, such as in the study of alpha-emitter distribution in the intestine, autoradiography is used. The application and relevance of different measurement techniques to animal studies will be discussed and examples of the results presented.

Aging↗
PubMed1994

Plutonium and the risk of cancer. A comparative analysis of Pu-body burdens due to releases from nuclear plants (Chelyabinsk-65, Gomel area) and global fallout.

Results of the analysis of dynamic body burdens of Pu in adult inhabitants of Chelyabinsk-65 (not occupationally exposed) and different areas of the Gomel region are presented for 1990-1991. The data are based on radiochemical analyses of Pu in human organs and tissues. Comparison with the published data on global Pu and our data for human autopsies (Ufa, Russia) revealed that estimates of Pubody burdens in Chelyabinsk-65 residents were up to 30 times higher than global levels and depended on the period of residence in town. The Pu body contents of Gomel citizens 4-5 years after the Chernobyl accident are on average 3-4 times higher than the global levels. Activity of Pu-238 in various organs constitutes 4.7-26.0% (on the average 13.5 +/- 5.0%) of the total alpha-activity of Pu-238 and Pu-239, 240. The expected number of cancers induced by incorporated plutonium is approximately the same for the two population groups despite their different sizes and does not differ from the global level by more than one order of magnitude.

Adult↗
PubMed1995

The assessment of plutonium and americium in contaminated wounds with high energy resolution semiconductor detectors.

A simple to use method was installed for the measurement of wounds contaminated with plutonium and americium by using a semiconductor detector. This technique does not explicitly require the knowledge of the detector efficiency but uses a plant 241Am calibration source. A computer programme has also been developed for the quantification of the contamination according to the shape and the depth of the contaminant in the wound.

Americium↗
PubMed2006

Improved determination of plutonium content and isotopic ratios in low activity samples by alpha-particle and underground L X-ray measurement.

The determination of the isotopic ratio of 239Pu and 240Pu by alpha-particle spectrometry is limited due to the small differences in the alpha-particle energies. But taking into account the differences in the L X-ray emission probabilities of the two plutonium isotopes, an additional L X-ray measurement allows the isotopic ratio of 239Pu and 240Pu to be determined. The sensitivity of this method can be improved, as described in this work, by performing the L X-ray measurement in an underground laboratory.

Algorithms↗
PubMed2005

Plutonium in groundwater at the 100K-Area of the U.S. DOE Hanford Site.

We examined the concentration, size distribution, redox state and isotopic composition of plutonium (Pu) in groundwater at the 100K-Area at the U.S. Department of Energy's (DOE) Hanford Site. Total concentrations of Pu isotopes were extremely low (10(-4) to 10(-6) pCi/kg, approximately 10(4) to 10(6) atoms/kg) but measurable for the first time in the 100K-Area wells using mass spectrometric analyses that are much more sensitive than alpha spectroscopy methods used previously. Size fractionation data from two wells suggest that 7-29% of the Pu is associated with colloids, operationally defined here as particles between 1 kDa-0.2 microm in size. These colloids were collected using a 1 kDa cross-flow ultrafiltration (CFF) system developed specifically for groundwater actinide studies to include careful controls both in the field and during processing to ensure in situ geochemical conditions are maintained and size separations can be well characterized. Pu in this colloidal fraction was exclusively in the more reduced Pu(III/IV) form, consistent with the higher affinity of Pu in the lower oxidation states for particle surfaces. While the overall concentrations of Pu were low, the Pu isotopic composition suggests at least two local sources of groundwater Pu, namely, local Hanford reactor operations at the 100K-Area and spent nuclear fuel from the N-reactor, which was stored in concrete pools at this site. Differences between this site and the Savannah River Site (SRS) are noted, since groundwater Pu at the F-Area seepage basin at SRS has been found using these same methods, to be characterized by lower colloidal abundances and higher oxidation states. This difference is not directly attributable to groundwater redox potential or geochemical conditions, but rather the physical-chemical difference in Pu sources, which at SRS appear to be dominated downstream from the seepage basins by decay of 244Cm, resulting in more oxidized forms of 240Pu. There is no clear evidence for colloid facilitated transport of Pu in groundwater at the Hanford Site, since downstream wells have both an order of magnitude lower concentrations of Pu and a lower fractional colloidal distribution.

Colloids↗
PubMed2005

Pharmacokinetics of DTPA entrapped in conventional and long-circulating liposomes of different size for plutonium decorporation.

The aim of the present study was to develop an efficient DTPA liposome formulation designed for plutonium decorporation. DTPA was encapsulated in conventional (CL) and polyethylene glycol-coated stealth liposomes (SL) prepared by extrusion followed by the freeze-thawing method and sizing from around 100 to 800 nm. DTPA encapsulation percentages were approximately 30% in CL of any size but dropped from 48% to 7% as the diameter of SL was reduced. The pharmacokinetics of [(14)C]-DTPA encapsulated in large and small vesicles was evaluated in rats after a single intravenous administration. Both liposomal composition and size reduction had a significant impact on pharmacokinetic parameters, inducing a marked increased in exposure of the body to DTPA and its delayed excretion. DTPA distribution was moderate in liver but enhanced in spleen and bone and was dose-dependent, especially when SL of 100 nm were given. In conclusion, small and stealth(R) vesicles have interesting properties in delivering DTPA to contaminated tissues.

Animals↗
PubMed2004

Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry.

Plutonium in Polish forest soils and the Bór za Lasem peat bog is resolved between Chernobyl and global fallout contributions via inductively coupled plasma mass spectrometric measurements of 240Pu/230Pu and 241Pu/239Pu atom ratios in previously prepared NdF3 alpha spectrometric sources. Compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/230Pu and 241Pu/239Pu co-vary and range from 0.186 to 0.348 and 0.0029 to 0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407 x [240Pu/239Pu] - 0.0413; r2 = 0.9924). Two-component mixing models are developed to apportion 239+240Pu and 241Pu activities; various estimates of the percentage of Chernobyl-derived 239+240Pu activity in forest soils range from < 10% to > 90% for the sample set. The 240Pu/230Pu - 241Pu/239Pu atom ratio mixing line extrapolates to estimate 241Pu/239Pu and the 241Pu/239+240Pu activity ratio for the Chernobyl source term (0.123 +/- 0.0007; 83 +/- 5; 1 May 1986). Sample 241Pu activities, calculated using existing alpha spectrometric 239+240Pu activities, and the 240Pu/230Pu and 241Pu/239Pu atom ratios, agree relatively well with previous liquid scintillation spectrometry measurements. Chernobyl Pu is most evident in locations from northeastern Poland. The 241Pu activities and/or the 241Pu/239Pu atom ratios are more sensitive than 240Pu/239Pu or 238Pu/239+240Pu activity ratios at detecting small Chernobyl 239+240Pu inputs, found in southern Poland. The mass spectrometric data show that the 241Pu activity is 40-62% Chernobyl-derived in southern Poland, and 58-96% Chernobyl in northeastern Poland. The Bór za Lasem peat bog (49.42 degrees N, 19.75 degrees E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu.

Environmental Monitoring↗
PubMed2004

Plutonium(VI) accumulation and reduction by lichen biomass: correlation with U(VI).

The uptake of plutonium(VI) and uranium(VI) by lichen biomass was studied in the foliose lichen Parmotrema tinctorum to elucidate the migration behavior of Pu and U in the terrestrial environment. Pu and U uptake by P. tinctorum averaged 0.040+/-0.010 and 0.055+/-0.015 g gdry (-1), respectively, after 96 h incubation with 4.0 x 10(14) mol 1(-1) Pu solutions of pH 3, 4 and 5. SEM observations showed that the accumulated Pu is evenly distributed on the upper and lower surfaces of P. tinctorum, in contrast to U(VI), which accumulated in both cortical and medullary layers. UV/VIS absorption spectroscopy demonstrates that a fraction of Pu(VI) in the solution is reduced to Pu(V) by the organic substances released from P. tinctorum, and the accumulated Pu on the surface is reduced to Pu(IV), while U(VI) keeps the oxidation state of VI. Since the solubility of Pu(IV) hydroxides is very low, reduced Pu(VI) does not penetrate to the medullary layers, but is probably precipitated as Pu(IV) hydroxides on the cortical lichen surface. It is concluded that the uptake and reduction of Pu(VI) by lichens is important to determine the mobilization and oxidation states of Pu in the terrestrial environment.

Air Pollutants, Radioactive↗