Associated with the use of 238Pu in thermoelectric power sources for space probes is the potential for human exposure, primarily by inhalation and most likely as 238PuO2. Several models have been developed for assessing the level of intake and predicting the resulting radiation dose following human exposure to 239Pu. However, there are indications that existing models do not adequately describe the disposition and dosimetry of 238Pu following human exposure. In this study, a canine model that accounts for these differences has been adapted for use with human excretion data. The model is based on existing knowledge about organ retention of plutonium. An analysis of the sensitivity of the model to changes in aerosol-associated properties indicated that predictions of urinary excretion are most sensitive to changes in particle solubility and diameter and in the ratio of fragment:particle surface area. Application of the model to urinary excretion data from seven workers exposed to a 238Pu ceramic aerosol gave estimated intakes of 390-8,200 Bq and associated initial pulmonary burdens of 80-1,700 Bq. The resulting 50-y dose commitments to critical organs per Bq of 238Pu intake were estimated to be 0.5 mSv for the thoracic region, 0.2 mSv for the liver, and 1 mSv for the bone surfaces.
Curium isotopes are major by-products in irradiated nuclear reactor fuel and comprise a significant fraction of the alpha-emitting radionuclide inventory. Although little use is currently being made of purified Cm sources, such usage is possible if reprocessing of spent fuel becomes feasible. Because little information is available on the biokinetics and dosimetry of inhaled Cm compounds, a study was conducted in which adult beagle dogs received a single inhalation exposure to either a monodisperse aerosol of 244Cm2O3 (1.4 micron activity median aerodynamic diameter [AMAD]; sigma g = 1.16) or a polydisperse aerosol of 244Cm (NO3)3 (1.1 micron AMAD; sigma g = 1.74). At times ranging from 4 h to 2 y after exposure, animals were sacrificed and their tissues analyzed for Cm content. The data describing the uptake and retention of 244Cm in the different organs and tissues and the measured rates of excretion of these dogs formed the basis on which a biokinetic model of Cm metabolism was constructed. This Cm model was based on a previously published model of the biokinetics of 241Am that was shown to be applicable to data from human cases of inhalation exposure to 241Am aerosols. This Cm model was found to be adequate to describe the biological distribution of Cm in dogs and was also applied to the sparse data from humans. Reasonable agreement was found between the model predictions for lung retention of Cm and for urinary excretion patterns in humans.
The lung retention of uranium was determined in rats that inhaled aerosols of commercial yellowcake powders obtained from two mills (Mill A and Mill D) and whose chemical composition and solubilities in vitro were significantly different. Analysis by IR absorption indicated Mill A yellowcake contained 82% ammonium diuranate (ADU) and 18% U3O8. The Mill D powder contained 25% ADU and 75% U3O8. In vitro dissolution studies indicated for the Mill A sample, approximately 85% of the uranium had a dissolution half-time (T 1/2) of less than one day, with the remainder dissolving with a half-time of 500 days. For the Mill D sample, 25% had T 1/2 less than one day and 75% had T 1/2 of 300 days. Groups of 50 rats were exposed by nose-only inhalation to aerosols of either the Mill A or the Mill D yellowcake. Rats were sacrificed in groups of five at intervals through six months after exposure. Selected tissues and excreta samples were assayed by fluorometry to determine their uranium contents. For the Mill A yellowcake, 78% initial lung (broncho-alveolar) burden cleared with T 1/2 of 0.5 days, and 22% with T 1/2 of 240 days. For the Mill D yellowcake, 25% initial lung burden cleared with T 1/2 of 3.5 days and 75% with T 1/2 of 110 days. Thus, the lung clearance of uranium in the rat mimicked the in vitro dissolution data and supported the contention that ADU should be considered as a Class D compound (T 1/2 = 0.5 days) and U3O8 behaves in the lung as a Class Y (T 1/2 greater than 100 days) material.
A study was conducted in rats to determine solubility and subsequent metabolism of an inhaled aerosol of curium treated at high temperatures. Young adult Fischer-344 rats received a single inhalation exposure to one of three monodisperse aerosols of 244Cm2O3 (0.70, 1.3, or 2.6 micron activity median aerodynamic diameter) heat-treated at 1150 degrees C. Animals were maintained individually in metabolism cages for excreta collection and serially sacrificed in groups of two male and two female rats from 2 to 33 days after inhalation exposure. Additionally an injection study with curium citrate was done to define the systemic behavior of Cm in this rat model. The in vivo solubility was inversely related to the aerosol particle size. The relationship of the results of this study to results from other experimental inhalation studies with curium oxide aerosols is discussed, as is the relevance to bioassay interpretation and risk assessment in man.
A new approach to the estimation of plutonium (Pu) levels in the skeleton based on measurements of Pu excretion in the feces following treatment with diethylenetriaminepentaacetic acid (DTPA) is presented. The estimation method was tested in groups of mice receiving either 0.5 or 5 pCi/kg of *'*u(IV) citrate, and treated with Na3[CaDTPA] starting either at 1 hr or 24 hr after Pu administration. In the case of DTPA treatment begun at 1 hr, the ratio of skeletal Pu content at 1 hr, S, to DTPA-induced fecal excretion of Pu, F, was 1.08+0.03. When DTPA treatment was begun at 24 hr, the corresponding S/F ratio was 1.68 + 0.08 and was independent of Pu injection level. In the mouse, therefore, a reasonable estimate of skeletal Pu content just prior to treatment can be determined from the amount of Pu measured in the feces following DTPA therapy. Application of this method to species other than the mouse is examined, with anticipation that the method might be applicable to cases of human exposure.
Radionuclide decorporation is the only effective method of reducing radiation dose for persons contaminated accidentally. In this study, dogs that had inhaled a moderately soluble aerosol of 244Cm2O3 were treated with either discrete intravenous injections of the chelating agent diethylenetriaminepentaacetic acid (Zn-DTPA) or with subcutaneous infusion of Zn-DTPA at either 30 or 120 mumol kg-1 d-1. Each treatment regimen was continued for 64 d, whereupon all animals were killed, and collected excreta and tissue samples were analyzed for curium. All DTPA treatment methods were effective. A total of 89% of the initial pulmonary burden (IPB) was removed by DTPA injection, whereas 94% IPB was removed by the low dose of infused DTPA and 97% by the high dose treatment. Thus, low and high infused doses of DTPA prevented the translocation of greater than 99.5% of curium to liver and 97-99% to bone and kidney. The resultant dose reductions to these organs were superior to those achieved by intravenous DTPA injections.
Although many data have been accumulated concerning the distribution and retention of plutonium in mammals, the bulk of it has been obtained with levels of 23'Pu that far exceed the exposure levels experienced in man. Accordingly we have investigated the role of injected mass of plutonium on its distribution and retention in mouse tissues, using four alpha-emitting plutonium isotopes of widely differing specific activities: 236Pu (532 pCi/pg Pu), 239pu (0.0613 pCi/pg), zQPu (0.0039 pCi/pg), 2uPu (1.93 x pCi/pg). Young adult female B6CFJAnl mice were injected intravenously with 1 pCi/kg of either 236Pu, 2 3~u or ' ' ' Pu or 0.3pCi/kg of 2uPu. Groups of five mice receiving each isotope were sacrificed from 4 to 96 days after Pu injection and selected tissues analyzed radiochemically for Pu content.The data obtained indicate that the early distribution and retention of ' "Pu, which was injected at a mass level (2ng/kg) equivalent to 20% of the maximum permissible body burden (MPBB) of 23?u, did not differ from that of 239pu, even though the injected masses differed by more than 8000. The isotopes of lower specific activity, '"*Pu and zuPu.which were injected at mass equivalents of 28,000 and 99,OOO times the MPBB of 2 3~u , respectively, showed differences in tissue distribution from that of "'Pu that suggest the occurrence of aggregation of 242Pu and 2uPu in uiuo. THE ACCUMULATED data for human occupational exposure to plutonium indicate that, in the majority of the cases, the levels of contamination have been at or below the recommended maximum permissible body burden (MPBB) for 2 3~u , i.e. 0.04pCi. Richmond (Ri74) reports that of 203 AEC contractor personnel measured to have more than 25% of the MPBB during the period 1957-1970, 82% were at or below the 40nCi level. The remaining 18% had between 1 and
Disposal of radioactive wastes in underground facilities requires continuous monitoring for airborne radioactive materials, both on the surface and underground. In addition to a natural background of nonradioactive and radioactive aerosols, there may be a sizeable dust contribution from ongoing work such as mining and vehicular traffic. In the monitoring of alpha-emitting radionuclides, these aerosols may lead to self-absorption in the source and a deterioration of the energy spectrum of the detected alpha particles. In this paper, the influence of a realistic background aerosol on the performance of an alpha monitoring system is evaluated theoretically. It is shown that depositing alpha emitters and background aerosol on a surface for counting leads rapidly to a considerable loss of counts, a deterioration of the alpha spectra, an eventual saturation of the count rates, and interference from the natural background of Rn daughters.
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