Review of the sources and behaviors of plutonium isotopes in the atmosphere and ocean.

Plutonium, as well as fission products such as 137Cs, had been released into the earth environment in 1945 after the first atmospheric nuclear explosion of plutonium bomb in the desert of New Mexico (USA, July 16) and later over Nagasaki (August 9), followed then by many other explosions. Thus, plutonium cycling in the atmosphere and ocean has become a major public concern as a result of the radiological and chemical toxicity of plutonium. However, plutonium isotopes and 137Cs are important transient tracers of biogeochemical and physical processes in the environment, respectively. In this review, we show that both physical and chemical approaches are needed to comprehensively understand the behaviors of plutonium in the atmosphere and ocean. In the atmosphere, plutonium and 137Cs attach with aerosols; thus, plutonium moves according to physical and chemical processes in connection with aerosols; however, since plutonium is a chemically reactive element, its behavior in an aqueous environment is more complicated, because biogeochemical regulatory factors, in addition to geophysical regulatory factors, must be considered. Meanwhile, 137Cs is chemically inert in aqueous environments. Therefore, the biogeochemical characteristics of plutonium can be elucidated through a comparison with those of 137Cs, which show conservative properties and moves according to physical processes. Finally, we suggest that monitoring of both plutonium and 137Cs can help elucidate geophysical and biogeochemical changes from climate changes.

Source, preservation and re-suspension of 239,240Pu in a well dated peat core collected from northwest China.

Owning to the high radiotoxicity in high concentrations, as well as the irreplaceability in quantifying soil erosion rates, demarcating the Anthropocene, and dating of sediment, anthropogenic 239,240Pu have drawn high attention. However, the source in specific areas, preservation characteristics in different environment media, and re-distribution process after the cessation of atmospheric nuclear weapons tests, have not been fully understood, which obscures the exact start year, temporal variation, and deposition flux of 239,240Pu in sedimentary records, and hinders the wide application of 239,240Pu in environment study. A sediment core from the Yiwu peat bog with dominance of atmospheric deposition in the source material, simple sedimentary environment, and high dust deposition flux, was collected to examine the 239,240Pu, and explore the source, preservation, and re-distribution process. The double peaks of 239,240Pu in 1952 CE and 1963 CE, as well as 240Pu/239Pu ratios of 0.163-0.190 with an average of 0.177 ± 0.010 confirmed that the 239,240Pu source originated predominantly from global fallout. The minimal vertical migration of plutonium in the Yiwu peat core was attributed to the near-neutral pH condition. The high inventory of 128 ± 7 Bq m-2, as well as the atypical negative correlation between 239,240Pu concentrations and organic matter content (r = - 0.79, P < 0.01), was attributed to the contribution of 239,240Pu re-suspended with dust from the neighboring Gobi Desert, particularly in the cold and dry years. The total re-suspended 239,240Pu was estimated to be 77 Bq m-2, exceeding the direct fallout level of 51 Bq m-2 during 1945-2016 CE. In this study, the specified deposition pattern of 239,240Pu after the cessation of atmospheric nuclear weapons was established, providing an important standard for multiple environmental studies, and the re-suspended amount of 239,240Pu in a typical arid area was quantified for the first time.

Estimation of 241Am and 239Pu activity embedded in the tissue using portable planar HPGe detector.

This paper describes a procedure for the estimation of 241Am and 239Pu activity present in the human tissue by measuring the depth of contaminant using a portable Planar High Purity Germanium detector (HPGe). The ratios of photopeak counts of X-rays or gammas obtained with the detector coupled to collimator are calculated for the estimation of depth of the contaminant and the optimum one is determined. Since Minimum Detectable Activities (MDA) for the detector coupled to a collimator are higher than that of bare detector, activity must be estimated using bare detector, after locating the contaminant. Two methods are described for the estimation of plutonium coexisting with 241Am: (i) Abundance and isotopic correction for 239Pu (ii) and 239Pu:241Am ratio. The procedure to estimate 239Pu when plutonium isotopes alone are present is also established. An optimum monitoring period to detect the minimum value of intake for both radionuclides corresponding to chelation therapy and excision is also derived.

Subsurface Transport of Plutonium in Organic and Aqueous Acidic Processing Wastes at the Hanford Site, USA.

Over 4 million liters of mixed acidic (∼pH 2.5), high ionic strength (∼5 M nitrate) plutonium (Pu) processing waste were released into the 216-Z-9 (Z-9) trench at the Hanford Site, USA, and trace Pu has migrated 37 m below the trench. In this study, we used flowthrough columns to investigate Pu transport in simplified processing waste through uncontaminated Hanford sediments to determine the conditions that led to Pu migration. In low pH aqueous fluids, some Pu breakthrough is observed at pH < 4, and increased Pu transport (14% total Pu breakthrough) is observed at pH < 2. However, Pu migrates in organic processing solvents through low pH sediments virtually uninhibited with approximately 94 and 86% total Pu breakthrough observed at pH 1 and pH 3, respectively. This study demonstrates that Pu migration can occur both with and without organic solvents at pH < 4, but significantly more Pu can be transported when partitioned into organic processing solvents. Our data suggest that under acidic conditions (pH < 4) in the vadose zone beneath the Z-9 trench, Pu present in organic processing solvents moved relatively unhindered and may explain the historical downward migration of Pu tens of meters below the Z-9 trench.

Quantitative estimation of dust transport in the desert region of northwest China by plutonium isotopes.

Dust is an important source of atmospheric pollution, and quantitative estimation of desert dust transport is crucial for air pollution control. In this study, five typical sandy soil profiles in the Tengger Desert were collected and analyzed for 239,240Pu concentration and 240Pu/239Pu atomic ratios in order to identify the source of 239,240Pu in this area and explore the sedimentary characteristics of dust in different profiles. The results revealed that the concentrations of 239,240Pu in the soil profiles were between 0.002 and 0.443 mBq/g with an exception of the deep layer soil at one site. The measured atomic ratios of 240Pu/239Pu are at the global atmospheric fallout level with a mean of 0.184 ± 0.020, indicating that global fallout is the dominant source of plutonium in this region. The total inventories of 239,240Pu in the reference sites in this area were estimated to be 39.2-44.6 Bq/m2, this is in agreement with the value from the global fallout of atmospheric nuclear weapon tests at the similar latitude (30-40 °N: 42 Bq/m2). The estimated erosion rate in the erosion profile utilizing soil erosion intensity mode is 2491 t/km2/yr and the soil erosion depth is 9.86 cm, While, the stacking rate of the accumulation profile is 1383 t/km2/yr, and the depth of accumulation is estimated to be 5.48 cm. The difference between the erosion and accumulation profiles indicated that approximately 1107 t/km2/yr of dust was exported from the Gobi landform area of the Tengger Desert, which might be transported long distance in the downwind direction.

Level, distribution and sources of Np, Pu and Am isotopes in Peter the Great Bay of Japan sea.

Transuranium elements such as Np, Pu and Am, are considered to be the most important radioactive elements in view of their biological toxicity and environmental impact. Concentrations of 237Np, Pu isotopes and 241Am in two sediment cores collected from Peter the Great Bay of Japan Sea were determined using radiochemical separation combined with inductively coupled plasma mass spectrometry (ICP-MS) measurement. The 239,240Pu and 241Am concentrations in all sediment samples range from 0.01 Bq/kg to 2.02 Bq/kg and from 0.01 Bq/kg to 1.11 Bq/kg, respectively, which are comparable to reported values in the investigated area. The average atomic ratios of 240Pu/239Pu (0.20 ± 0.02 and 0.21 ± 0.01) and 241Am/239+240Pu activity ratios (3.32 ± 2.76 and 0.45 ± 0.17) in the two sediment cores indicated that the sources of Pu and Am in this area are global fallout and the Pacific Proving Grounds through the movement of prevailing ocean currents, and no measurable release of Np, Pu and Am from the local K-431 nuclear submarine incident was observed. The extremely low 237Np/239Pu atomic ratios ((2.0-2.5) × 10-4) in this area are mainly attributed to the discrepancy of their different chemical behaviors in the ocean due to the relatively higher solubility of 237Np compared to particle active plutonium isotopes. It was estimated using two end members model that 23% ± 6% of transuranium radionuclides originated from the Pacific Proving Grounds tests, and the rest (ca. 77%) from global fallout.

A multi-collector ICP-MS method for quantification of plutonium, uranium, and americium in hair and nails of occupationally or medically exposed individuals.

The 239Pu, 238U, and 241Am concentrations and 239Pu/240Pu, 235U/238U, and 236U/238U atom ratios were measured in the hair and nail samples using a new method utilized TEVA, UTEVA, and DGA extraction chromatography and multi-collector ICP-MS. Samples were collected from individuals who donated their bodies to the United States Transuranium and Uranium Registries. The concentration of 239Pu ranged from 0.22 to 15.8 ng/kg. The 240Pu/239Pu isotopic ratios ranged from 0.026 to 0.127 which is consistent with weapons-grade plutonium. Concentration of uranium fell between 1.84 µg/kg and 29.5 µg/kg and 235U/238U ratios ranged from 4.8 × 10-3 to 7.6 × 10-3. Elevated 236U/238U atom ratios were measured in two cases and ranged from 5.0 × 10-6 - 2.4 × 10-5 indicating exposure to spent or reprocessed uranium material. The concentration of 241Am was measured in four hair samples and ranged from 0.02 to 0.21 ng/kg.

The records of 239+240Pu and 137Cs of global fallout in Lake East Dongting Sediments and Responses to watershed environmental changes.

Plutonium-239 + 240 and 137Cs in the environment can usually be used to track the impact of nuclear activities on the environment, and have become important tools in environmental geochemical studies. In this study, nine sediment cores (E1-E9) in Lake East Dongting were collected and measured for the activity concentration of 239+240Pu, 137Cs and the atomic ratio of 240Pu/239Pu, and then their vertical distribution characteristics were analyzed. The results show that: the activity concentrations of 137Cs and 239+240Pu in Lake East Dongting ranged from 5.26 ± 0.43 to 28.6 ± 2.23 Bq kg-1 and 0.29 ± 0.02 to 1.37 ± 0.09 Bq kg-1, with an average of 7.48 ± 0.68 Bq kg-1 and 0.39 ± 0.03 Bq kg-1, respectively. The atomic ratios of 240Pu/239Pu are 0.168 ± 0.012-0.211 ± 0.015, which are basically consistent with the global atmospheric deposition. The vertical profiles of 137Cs and 239+240Pu in sediment cores show obvious single-peak distribution in E1-E6 and bimodal distribution in E7-E9. The results of sedimentation rates calculated by 137Cs and 239+240Pu method ranged from 0.59 cm y-1 to 1.99 cm y-1 with a mean of 1.18 cm y-1 and 0.61 cm y-1 to 2.18 cm y-1 with a mean of 1.26 cm y-1. The inventories of 137Cs and 239+240Pu in nine sediment cores are 5.87-10.8 kBq m-2 and 307-545 Bq m-2, which are about 8-14 and 9-15 times the inventory in the global average atmospheric deposition at the same latitude respectively. Comparing the results of the sedimentation rates and the inventories from different sampling points indicates that extreme climatic events and human activities have a significant impact on sediment environment of Lake East Dongting.

Predominance of the alkaline earth(II) triscarbonatoactinyl(VI) complexes in different geochemical contexts: Review of existing data and estimation of potentially unidentified species.

From the available thermodynamic data in the literature, a review of the impact of the formation of complexes between triscarbonatoactinyl(VI) and alkaline earth(II) (Ae) is estimated under varying conditions. First, after analyzing the literature data and using the ascertained thermodynamic data available from the commissioned reviews from the Nuclear Energy Agency (Organization for the Economic Cooperation and Development) Thermochemical DataBank Project on actinides (An) U, Np, and Pu, and from recently determined AenUO2(CO3)3(4-2n)- thermodynamic functions, the formation of AenAnO2(CO3)3(4-2n)- complexes for Pu(VI) and Np(VI) are estimated using linear free energy relationships (LFERs). The data are in good agreement with the sole determination of AePuO2(CO3)32- from Jo et al. (Dalton Trans. 49, 11605), which gives a relative confidence in the LFERs, and allows the application to actual situations. From existing uranium data, first, the impact of the origin of the data on the calculated predominance is addressed under 0.1 M NaCl and atmospheric CO2(g); second, the influence of ionic strength and salinity on predominance is estimated; and finally, the influence of temperature up to 50 °C on the solubility of uraninite in a deep geological radioactive waste storage or disposal site is calculated. For neptunium and plutonium, the impact of the potential log10ß°(AenAnO2(CO3)3(4-2n)-) on Pourbaix diagrams of Pu and Np in Mg-Ca-CO3 media are estimated from Jo et al. (Dalton Trans. 49, 11605) and LFERs. Finally, the application to the speciation of Pu and Np in seawater is proposed.

Particulate matter from water moss of a large Siberian river: Morphometric, mineral, elemental and radionuclide composition.

Particulate matter trapped by tufts of water moss Fontinalis antipyretica inhabiting fast flowing waters of the Yenisei River (Siberia, Russia) contaminated with artificial radionuclides has been studied as a potential monitor of radioactive releases to the river. Particulate matter, which was removed from wet tufts of water moss of the Yenisei by rinsing them in water, constituted at least 38% of bulk dry weight of the moss biomass sample and was similar in the contents of chemical elements, minerals, organic matter, and artificial radionuclides to bottom sediments of the Yenisei. Considerable bulk percentages of artificial radionuclides in the sample of water moss, 77% of 137Cs, 44% of 60Co, 41% of 152Eu, 55% of 154Eu, 66% of 241Am, and 34-36% of plutonium were associated with extracellular particles. The comparative study and correlation analysis suggested that 137Cs was mainly associated with mineral particles trapped by moss and that organic matter was responsible for binding plutonium in samples of water moss. Consequently, analysis of extracellular particles of water moss can provide data on contents and speciation of radionuclides transported by water current. Although a considerably high proportion of particulate matter had been washed out from tufts of water moss, some extracellular mineral particulate material and a large number of epiphytic diatoms remained attached to leaves of water moss. Our study proves that particulate matter trapped by water moss can be used as an informative monitor to trace radioactive pollutants transported by water current in running waters deficient in bottom sediments and potential biomonitors.

Spatial distribution, source identification, and transportation paths of plutonium in the Beibu Gulf, South China Sea.

To investigate the spatial distribution and source of plutonium isotopes in the Beibu Gulf, surface sediments were collected and analyzed using sector field inductively coupled plasma mass spectrometry (SF-ICP-MS). The activities of 239+240Pu in surface sediments ranged from 0.012 to 0.451 mBq/g (mean: 0.171 ± 0.138 mBq/g, n = 36), indicating a decreasing trend in a counterclockwise direction from the southern bay mouth. The counterclockwise decreasing trend in the south of the bay mouth is similar to the current in the Beibu Gulf. The 240Pu/239Pu atom ratios in surface sediments ranged from 0.156 to 0.283 (mean: 0.236 ± 0.031, n = 36), slightly higher than that of the global fallout value of 0.18. This suggests that the Pu in the Beibu Gulf was a combination of global fallout and Pacific Proving Ground (PPG). The average contribution of the plutonium (Pu) derived from the PPG in the sediment was estimated to be 52 % ± 24 %.

Spatial distribution and modelling of 239+240Pu in the sediments and seawater columns of the South China Sea and Indian Ocean.

In order to investigate the 239+240Pu potential influence in the ocean, and develop a new method for rapidly monitoring radioactive pollution, the 239+240Pu spatial distribution in the South China Sea (SCS) and the Indian Ocean (IND) sediments is analyzed by SF-ICP-MS (ELEMENT 2). The inventory-weighted mean activities of 239+240Pu were 0.413 ± 0.333 mBq/g, 0.128 ± 0.044 mBq/g, and 0.483 ± 0.606 mBq/g in the sediments of the SCS, eastern IND, and Arabian Sea, respectively. The 239+240Pu activity spatial distribution in the SCS sediments was influenced by the current, the vertical distribution of Pu in seawater, and the transport of particulate matter. The 239+240Pu activity spatial distribution in the IND sediments could be impacted by Antarctic Intermediate Water. The average of 240Pu/239Pu atomic ratios were 0.258 ± 0.034, 0.219 ± 0.031, and 0.212 ± 0.028 in the sediments of the SCS, eastern IND, and Arabian Sea, respectively. The 240Pu/239Pu atomic ratios in the SCS and IND indicate that Pu from the Pacific Proving Ground (PPG) is transported to the IND via the SCS internal current and transverse ocean currents within Indonesia. In addition, a seawater advection-dispersion equation (S-ADE) model is established based on the actual physical processes of radionuclides in the seawater column and well fitting results were obtained (R2 = 0.49 to 0.99). The 239+240Pu data and the geographic information from the sample site were used to correct the Pu distribution in the seawater. The calculated 239+240Pu mean concentrations in the surface seawater were 2.465 mBq/m3 and 2.205 mBq/m3 for the SCS and the eastern IND seawater, respectively, and the result is consistent with the previous measurements. Then, the 239+240Pu stored in the study area of SCS and eastern IND was estimated to be approximately 1.0-1.4% of the global ocean based on the model. This study provides a useful model for guiding and designing future monitoring of pollution by anthropogenic Pu and other isotopes.

Chelation Modeling of a Plutonium-238 Inhalation Incident Treated with Delayed DTPA.

This work describes an analysis, using a previously established chelation model, of the bioassay data collected from a worker who received delayed chelation therapy following a plutonium-238 inhalation. The details of the case have already been described in two publications. The individual was treated with Ca-DTPA via multiple intravenous injections and then nebulizations beginning several months after the intake and continuing for four years. The exact date and circumstances of the intake are unknown. However, interviews with the worker suggested that the intake occurred via inhalation of a soluble plutonium compound. The worker provided daily urine and fecal bioassay samples throughout the chelation treatment protocol, including samples collected before, during, and after the administration of Ca-DTPA. Unlike the previous two publications presenting this case, the current analysis explicitly models the combined biokinetics of the plutonium-DTPA chelate. Using the previously established chelation model, it was possible to fit the data through optimizing only the intake (day and magnitude), solubility, and absorbed fraction of nebulized Ca-DTPA. This work supports the hypothesis that the efficacy of the delayed chelation treatment observed in this case results mainly from chelation of cell-internalized plutonium by Ca-DTPA (intracellular chelation). It also demonstrates the validity of the previously established chelation model. As the bioassay data were modified to ensure data anonymization, the calculation of the "true" committed effective dose was not possible. However, the treatment-induced dose inhibition (in percentage) was calculated.

Microbial community dynamics and cycling of plutonium and iron in a seasonally stratified and radiologically contaminated pond.

Plutonium (Pu) cycling and mobility in the environment can be impacted by the iron cycle and microbial community dynamics. We investigated the spatial and temporal changes of the microbiome in an iron (Fe)-rich, plutonium-contaminated, monomictic reservoir (Pond B, Savannah River Site, South Carolina, USA). The microbial community composition varied with depth during seasonal thermal stratification and was strongly correlated with redox. During stratification, Fe(II) oxidizers (e.g., Ferrovum, Rhodoferax, Chlorobium) were most abundant in the hypoxic/anoxic zones, while Fe(III) reducers (e.g., Geothrix, Geobacter) dominated the deep, anoxic zone. Sulfate reducers and methanogens were present in the anoxic layer, likely contributing to iron and plutonium cycling. Multinomial regression of predicted functions/pathways identified metabolisms highly associated with stratification (within the top 5%), including iron reduction, methanogenesis, C1 compound utilization, fermentation, and aromatic compound degradation. Two sediment cores collected at the Inlet and Outlet of the pond were dominated by putative fermenters and organic matter (OM) degraders. Overall, microbiome analyses revealed the potential for three microbial impacts on the plutonium and iron biogeochemical cycles: (1) plutonium bioaccumulation throughout the water column, (2) Pu-Fe-OM-aggregate formation by Fe(II) oxidizers under microaerophilic/aerobic conditions, and (3) Pu-Fe-OM-aggregate or sediment reductive dissolution and organic matter degradation in the deep, anoxic waters.

Evidence of fast neutron operating in Oklo.

Since the discovery of the first reactor zone (RZ) at the Oklo uranium deposit in 1972, many isotopic studies have been performed to understand the mechanism of the operation as fission reactors and to trace the migration behaviors of fissiogenic isotopes produced in the Oklo RZs. As the representative parameters to characterize the operating conditions of RZs, neutron fluence generated in RZ, duration of RZ operation, restitution factor of 235U from α decay of 239Pu produced by neutron capture of 238U and the proportion of fission events due to 235U, 238U and 239Pu are compiled and compared with individual RZs. In particular, one of the Oklo RZs, RZ 13, shows several specific features in the view point of isotopic and nuclear characteristics. By comparison of the data between RZ13 and other RZs, fission contribution of 238U for RZ13 is found to be significantly higher than those of other RZs.

Parallels between natural Oklo reaction zones and industrial reactors dynamics.

The first man-made nuclear reactor was developed by Fermi and collaborators at the University of Chicago and reached criticality in December 1942. This was the confirmation that men were able to use sustained fission reactions in order to produce energy. Following this success, nuclear reactors studies gave rise to several families of reactors corresponding to different orientations and technical choices. They are linked mainly to the choice of fuel (natural uranium, enriched uranium, plutonium, thorium), coolant (water, carbon dioxide, helium, sodium, ...) and moderator for slow neutron reactors (graphite, light water, heavy water). Out of all these choices, the pressurized water reactor (PWR) family is the closest to the Oklo natural reactors. Many intriguing similarities are observed and discussed in the present article. Our present-day understanding of the PWR operating conditions has been a great help for understanding the Oklo reactors.

Bioaccumulation of radionuclides in hoofed animals inhabiting the Semipalatinsk Test Site.

The article assesses the content of radionuclides in hoofed animals inhabiting the Semipalatinsk Test Site by calculation. Hoofed animals' faeces were sampled to determine the content of radionuclides in their diets. Based on values determined for the content of radionuclides in animals; diets, the content of radionuclides in the meat and milk of farm animals-cows (Bos taurus taurus), sheep (Ovis), goats (Capra hircus) and horses (Equus caballus Lin., 1758) as well as in the meat of wild animals-european moose (Alces alces Lin., 1758), argali (Ovis ammon Lin., 1758), roe deer (Capreolus pygargus Pal., 1771) and saiga (Saiga tatarica Lin., 1766) was calculated. No excess of permissible values of the content of 137Cs and 90Sr in the meat of farm animals was found to be expected, even for a conventional 'conservative' scenario, in which maxima of the radionuclide activity concentration in a vegetable feed (faeces) are taken as a basis. 241Am and 239+240Pu in the meat of farm hoofed animals are not standardized. Their predicted maxima of activity concentration are very low, and even in the 'conservative' scenario, they do not exceed 1.8×10-2 Bq kg-1, 1.4×10-1 Bq kg-1 and 1.6×10-1 Bq kg-1, respectively. In the milk of farm animals, the content of 137Cs and 90Sr does not exceed permissible values. 241Am and 239+240Pu in the milk of farm animals are not standardized. Their predicted activity concentration values in the milk of sheep and goats do not exceed 6.5×10-2 Bq l-1, for cows- 2.6×10-2 Bq l-1, for horses- 3.1×10-2 Bq l-1. Permissible values of 137Cs and 90Sr in the meat of wild hoofed animals are not exceeded either. In the meat of argali, roe deer and saigas, relatively high levels of 137Cs are predictable. 241Am and 239+240Pu in meat of wild animals are not standardized. Their predicted activity concentration values in the meat of moose and argali do not exceed 3.2×10-1 Bq kg-1 and 1.6×10-1 Bq kg-1, respectively, for roe deer and saiga-5.4×10-2 Bq kg-1. Thus, in case of free grazing in the STS territory, no excess of permissible values of standardized radionuclides (137Cs and 90Sr) in the meat and milk of hoofed animals is predictable.

Unfolding of 239Pu-Be and 252Cf neutron energy spectra using passive multi-layer neutron spectrometer.

In the study, the passive multi-layer neutron spectrometer, based on thermoluminescence detectors, was tested in a calibration laboratory with 239Pu-Be and 252Cf isotopic sources. MCNP code was used for the calculation of the response functions for the neutron energy range from 1 meV to 100 MeV. It was also utilised for initial guess spectra calculations. Deconvolution was performed with MAXED and GRAVEL deconvolution codes resulting in the neutron spectra defined at the measuring point in the calibration laboratory.

Modified human respiratory tract model to describe the retention of plutonium in scar tissues.

The Human Respiratory Tract Model described in Publication 130 of the International Commission on Radiological Protection provides some mechanisms to account for retention of material that can be subject to little to no mechanical transport or absorption into the blood. One of these mechanisms is 'binding', which refers to a process by which a fraction ('bound fraction') of the dissolved material chemically binds to the tissue of the airway wall. The value of the bound fraction can have a significant impact on the radiation doses imparted to different parts of the respiratory tract. To properly evaluate-and quantify-bound fraction for an element, one would need information on long-term retention of the element in individual compartments of the respiratory tract. Such data on regional retention of plutonium in the respiratory tract of four workers-who had inhaled materials with solubility ranging from soluble nitrate to very insoluble high-fired oxides-were obtained at the United States Transuranium and Uranium Registries. An assumption of bound fraction alone was found to be inconsistent with this dataset and also with a review of the literature. Several studies show evidence of retention of a large amount of Pu activity in the scar tissues of humans and experimental animals, and accordingly, a model structure with scar-tissue compartments was proposed. The transfer rates to these compartments were determined using Markov Chain Monte Carlo analysis of the bioassay and post-mortem data, considering the uncertainties associated with deposition, dissolution and particle clearance parameters. The models predicted that a significant amount-between 20 and 100% for the cases analyzed-of plutonium retained in the respiratory tract was sequestered in the scar tissues. Unlike chemically-bound Pu that irradiates sensitive epithelial cells, Pu in scar tissues may not be dosimetrically significant because the scar tissues absorb most, if not all, of the energy from alpha emissions.

Biokinetic model analysis with DTPA administration for a case of accidental inhalation of actinides in Japan.

Accidental inhalation intake of plutonium isotopes and 241Am occurred at a Pu research facility in Japan in 2017, and the five workers involved in this accident were treated by the administration of Ca/Zn-diethylenetriaminepentaacetic acid (DTPA). For the worker who was most internally exposed, the therapy was continued over 1 y after the accident. Urinary samples collected before and after each administration were subject to bioassay to evaluate the efficacy of the dose reduction. This study performed numerical analyses using a biokinetic model dealing with 241Am-DTPA with reference to the European Coordinated Network on Radiation Dosimetry approach, which assumes that the complex of actinides and Ca/Zn-DTPA is generated in the designated compartments in the biokinetic model. The results of the model prediction well captured the trend of the observed urinary excretion in the long-term bioassay and would be useful to evaluate the efficacy of the Ca/Zn-DTPA administration for the worker involved in the accident.