Validation of a system of models for plutonium decorporation therapy.

A recently proposed system of models for plutonium decorporation (SPD) was developed using data from an individual occupationally exposed to plutonium via a wound [from United States Transuranium and Uranium Registries (USTUR) Case 0212]. The present study evaluated the SPD using chelation treatment data, urine measurements, and post-mortem plutonium activities in the skeleton and liver from USTUR Case 0269. This individual was occupationally exposed to moderately soluble plutonium via inhalation and extensively treated with chelating agents. The SPD was linked to the International Commission on Radiological Protection (ICRP) Publication 66 Human Respiratory Tract Model (HRTM) and the ICRP Publication 30 Gastrointestinal Tract model to evaluate the goodness-of-fit to the urinary excretion data and the predictions of post-mortem plutonium retention in the skeleton and liver. The goodness-of-fit was also evaluated when the SPD was linked to the ICRP Publication 130 HRTM and the ICRP Publication 100 Human Alimentary Tract Model. The present study showed that the proposed SPD was useful for fitting the entire, chelation-affected and non-affected, urine bioassay data, and for predicting the post-mortem plutonium retention in the skeleton and liver at time of death, 38.5 years after the accident. The results of this work are consistent with the conclusion that Ca-EDTA is less effective than Ca-DTPA for enhancing urinary excretion of plutonium.

Capstone depleted uranium aerosol biokinetics, concentrations, and doses.

One of the principal goals of the Capstone Depleted Uranium (DU) Aerosol Study was to quantify and characterize DU aerosols generated inside armored vehicles by perforation with a DU penetrator. This study consequently produced a database in which the DU aerosol source terms were specified both physically and chemically for a variety of penetrator-impact geometries and conditions. These source terms were used to calculate radiation doses and uranium concentrations for various scenarios as part of the Capstone Human Health Risk Assessment (HHRA). This paper describes the scenario-related biokinetics of uranium, and summarizes intakes, chemical concentrations to the organs, and E(50) and HT(50) for organs and tissues based on exposure scenarios for personnel in vehicles at the time of perforation as well as for first responders. For a given exposure scenario (duration time and breathing rates), the range of DU intakes among the target vehicles and shots was not large, about a factor of 10, with the lowest being for a ventilated operational Abrams tank and the highest being for an unventilated Abrams with DU penetrator perforating DU armor. The ranges of committed effective doses were more scenario-dependent than were intakes. For example, the largest range, a factor of 20, was shown for scenario A, a 1 min exposure, whereas, the range was only a factor of two for the first-responder scenario (E). In general, the committed effective doses were found to be in the tens of mSv. The risks ascribed to these doses are discussed separately.

Dose assessment for inhalation intakes in complex, energetic environments: experience from the US Capstone study.

Because of the lack of existing information needed to evaluate the risks from inhalation exposures to depleted uranium (DU) aerosols of US soldiers during the 1991 Persian Gulf War, the US Department of Defense funded an experimental study to measure the characteristics of DU aerosols created when Abrams tanks and Bradley fighting vehicles are struck with large-caliber DU penetrators, and a dose and risk assessment for individuals present in such vehicles. This paper describes some of the difficulties experienced in dose assessment modelling of the very complex DU aerosols created in the Capstone studies, e.g. high concentrations, heterogeneous aerosol properties, non-lognormal particle size distributions, triphasic in vitro dissolution and rapid time-varying functions of both DU air concentration and particle size. The approaches used to solve these problems along with example results are presented.

Effective dose scaling factors for use with uranium series cascade impactor data: a reassessment using the IMBA code.

Air sampling with a multi-stage cascade impactor enables one to assess airborne radioactivity as a function of particle size, significantly enhancing the accuracy of the dose assessment. The application of cascade sampling data to inhalation dose assessments can require more computational effort if something other than a mono-sized distribution per impactor stage is to be considered. To overcome this limitation, Kim et al. (Health Phys 89:359-374; 2005) introduced the concept of an effective dose scaling factor SF(E) enabling one to consider more realistic impactor stage radioactivity distributions (uniform, linearly decreasing, or linearly increasing variations with particle size). The SF(E) is the ratio of the effective dose given under a uniform or linearly changing radioactivity distribution across the particle size interval to that given for a mono-sized radioactivity distribution for the same impactor stage. The latter approach can initially be used (which requires less computational effort) followed by a rescaling of the effective dose either upward or downward by the SF(E) value. In this earlier study, the LUDEP code was employed which utilizes the ICRP 66 human respiratory tract model along the radionuclide biokinetic models given in ICRP Publication 30. In the present study, inhalation dose coefficients and effective dose scaling factors were reexamined for several radionuclides of the (238)U series using the IMBA program, which employs more recent and physiologically realistic biokinetic models published by the ICRP. An update of the effective dose scaling factors is thus the primary focus of this study rather than an extensive inter-comparison of the IMBA and LUDEP codes. Inhalation dose coefficients calculated by the two programs differ by up to a factor of 5 for Type F (238)U and (234)U, but are within only 2% of each other for Type S radionuclides. The ICRP 69 biokinetic model of uranium predicts retention in bone and kidneys that is slightly higher than predicted in ICRP Publication 30, but is significantly higher in the liver and other soft tissues by up to 1 or 2 orders of magnitude. Nevertheless, effective dose scaling factors generated using the IMBA program are nearly identical to those calculated by the LUDEP program as their magnitude is primarily dictated by the dependence of particle deposition and lung clearance with particle size, and less by the systemic biodistribution of the radionuclide following absorption to blood. For both codes, greater than 10% re-scaling of the effective dose is required for third-stage (4.5 to 12 microm) and filter-stage (0.03 to 0.35 microm) particles in the approximation of uniform or linearly decreasing radioactivity distributions per particle stage. For linearly increasing distributions, greater than 10% corrections in the effective dose are found irregularly across impactor stage, radionuclide, and solubility class, especially for rather steep (1:5) impactor stage activity ratios.

Bioaccumulation and behavioural effects of depleted uranium in rats exposed to repeated inhalations.

Depleted uranium has numerous industrial and military uses. Contamination by inhalation of airborne compounds is probably the most important route of exposure. In humans, there are no data clearly demonstrating neurotoxicity of uranium, yet some experimental studies suggest a link between neurological toxicity and uranium exposure. In this work, the bioaccumulation of uranium in male rats after exposure to repeated depleted uranium dioxide inhalation (30 min inhalation at 197 mgm(-3), 4 days a week for 3 weeks) has been studied, together with the behavioural effects. The uranium concentrations in the brain 1 day after the end of the exposure period varied as follows: olfactory bulb>hippocampus>frontal cortex>cerebellum, subsequently decreasing rapidly. The spontaneous locomotion activity of exposed rats was increased 1 day post exposure and the spatial working memory was less efficient 6 days post exposure, compared with control rats. These data suggest that depleted uranium is able to enter the brain after exposure to repeated inhalation, producing behavioural changes.

Uptake of radionuclides by vegetation at a High Arctic location.

Radionuclide levels in vegetation from a High Arctic location were studied and compared to in situ soil concentrations. Levels of the anthropogenic radionuclide 137Cs and the natural radionuclides 40K, 238U, 226Ra and 232Th are discussed and transfer factor (TF) values and aggregated transfer (Tag) values are calculated for vascular plants. Levels of 137Cs in vegetation generally followed the order mosses > lichen > vascular plants. The uptake of 137Cs in vascular plants showed an inverse relationship with the uptake of 40K, with 137Cs TF and Tag values generally higher than 40K TF and Tag values. 40K activity concentrations in all vegetation showed little correlation to associated soil concentrations, while the uptake of 238U, 226Ra and 232Th by vascular and non-vascular plants was generally low.

Depleted uranium dust from fired munitions: physical, chemical and biological properties.

This paper reports physical, chemical and biological analyses of samples of dust resulting from munitions containing depleted uranium (DU) that had been live-fired and had impacted an armored target. Mass spectroscopic analysis indicated that the average atom% of U was 0.198 +/- 0.10, consistent with depleted uranium. Other major elements present were iron, aluminum, and silicon. About 47% of the total mass was particles with diameters <300 microm, of which about 14% was <10 microm. X-ray diffraction analysis indicated that the uranium was present in the sample as uranium oxides-mainly U3O7 (47%), U3O8 (44%) and UO2 (9%). Depleted uranium dust, instilled into the lungs or implanted into the muscle of rats, contained a rapidly soluble uranium component and a more slowly soluble uranium component. The fraction that underwent dissolution in 7 d declined exponentially with increasing initial burden. At the lower lung burdens tested (<15 microg DU dust/lung) about 14% of the uranium appeared in urine within 7 d. At the higher lung burdens tested (~80-200 microg DU dust/lung) about 5% of the DU appeared in urine within 7 d. In both cases about 50% of that total appeared in urine within the first day. DU implanted in muscle similarly showed that about half of the total excreted within 7 d appeared in the first day. At the lower muscle burdens tested (<15 microg DU dust/injection site) about 9% was solubilized within 7 d. At muscle burdens >35 microg DU dust/injection site about 2% appeared in urine within 7 d. Natural uranium (NU) ore dust was instilled into rat lungs for comparison. The fraction dissolving in lung showed a pattern of exponential decline with increasing initial burden similar to DU. However, the decline was less steep, with about 14% appearing in urine for lung burdens up to about 200 microg NU dust/lung and 5% at lung burdens >1,100 microg NU dust/lung. NU also showed both a fast and a more slowly dissolving component. At the higher lung burdens of both DU and NU that showed lowered urine excretion rates, histological evidence of kidney damage was seen. Kidney damage was not seen with the muscle burdens tested. DU dust produced kidney damage at lower lung burdens and lower urine uranium levels than NU dust, suggesting that other toxic metals in DU dust may contribute to the damage.

Locating a "hot spot" in the lungs when using an array of four HPGe detectors.

Considerable errors in the activity determination in lungs can be induced for the case of a "hot spot". Modern lung counter systems use several HPGe detectors, and the count rate ratios of the detectors can be used to locate the "hot spot" and apply correction algorithms. Some criteria for location determination of a point source in the lungs were investigated, and it is shown that an average error of up to about 10% can be achieved.

Uranium deposition and retention in a USTUR whole body case.

This report describes a whole body donation from a person with a documented occupational intake of uranium. USTUR Case 1002 was an adult male who died from an acute cerebellar infarct at the age of 83. He worked as a power operator, utility operator, and metal operator for 28 years in a facility that processed and handled radioactive materials. Although he suffered a number of burns from hot metal and acids, cuts, abrasions, and puncture wounds during his many years of work, there were no corresponding health physics or medical records to indicate that these occurrences needed or required excision or decontamination due to the suspicion of the deposition of radioactive material. Over the course of his employment, USTUR Case 1002 submitted numerous urine samples for uranium, plutonium, and fission product analysis. The highest single uranium value measured during this time period was approximately 30 microg L(-1) recorded during the second year of his employment. A urinary bioassay sample taken before termination of employment measured 4.3 microg L(-1). The mean urinary uranium concentration per liter per year calculated from the employee's bioassay records covering the first eleven years of monitoring averaged less than 3 microg L(-1). The ratio of 234/238U activity in the lung tissue was about 1, the same as that found in natural uranium. The highest concentration of uranium was found in a tracheobronchial lymph node. The uranium content in the various tissues of the body followed a rank order lung > skeleton > liver > kidney. Concentration of uranium in the kidney tissue was approximately 1.98 ng g(-1), about 3 orders of magnitude less than the generally accepted threshold level for permanent kidney damage of 3 microg U g(-1) and roughly equal to the 1.4 ng g(-1) reported for Reference Man. The autopsy disclosed findings not uncommon in the aged: severe atherosclerosis, areas of sclerotic kidney glomeruli with stromal fibrous scarring, and moderate to severe arterionephrosclerosis. Lung sections contained parenchymal areas of acute vascular congestion and a mild degree of anthracosis.

Assessment of intakes of mixtures of radionuclides.

Australia has several uranium mines and a large number of mineral sand mines, with associated processing facilities. Exposures resulting from these mining and processing operations usually involve intakes of mixtures of radionuclides. This work describes the development of a suite of first order, linear compartment models, based on the ICRP Publication 66 respiratory tract model, and an analytical solution to the decay equations, for assessing the consequences of such intakes. The computer programs based on these models directly compute excretion, organ retention and organ and whole-body doses for intakes of either single radionuclides or any mixture of radionuclides belonging to the same radioactive decay chain. The intake can be via inhalation, ingestion or injection, and can be acute, chronic or of limited duration. The starting concentration and degree of secular (dis)equilibrium can be specified for each radionuclide. No assumptions need to be made about the relative magnitudes of the radioactive half-lives of the different nuclides.

Characterisation and dissolution of depleted uranium aerosols produced during impacts of kinetic energy penetrators against a tank.

Aerosols produced during impacts of depleted uranium (DU) penetrators against the glacis (sloping armour) and the turret of a tank were sampled. The concentration and size distribution were determined. Activity median aerodynamic diameters were 1 microm (geometric standard deviation, sigma(g) = 3.7) and 2 microm (sigma(g) = 2.5), respectively, for glacis and turret. The mean air concentration was 120 Bq m(-3), i.e. 8.5 mg m(-3) of DU. Filters analysed by scanning electron microscopy (SEM) and X ray diffraction showed two types of particles (fine particles and large molten particles) composed mainly of a mixture of uranium and aluminium. The uranium oxides were mostly U3O8, UO2.25 and probably UO3.01 and a mixed compound of U and Al. The kinetics of dissolution in three media (HCO3-, HCl and Gamble's solution) were determined using in-vitro tests. The slow dissolution rates were respectively slow, and intermediate between slow and moderate, and the rapid dissolution fractions were mostly intermediate between moderate and fast. According to the in-vitro results for Gamble's solution, and based on a hypothetical single acute inhalation of 90 Bq, effective doses integrated up to 1 y after incorporation were 0.54 and 0.56 mSv, respectively, for aerosols from glacis and turret. In comparison, the ICRP limits are 20 mSv y(-1) for workers and 1 mSv y(-1) for members of the public. A kidney concentration of approximately 0.1 microg U g(-1) was predicted and should not, in this case, lead to kidney damage.

Anomalies between radiological and chemical limits for uranium after inhalation by workers and the public.

Exposure limits for workers and the public are based on both chemical toxicity and radiation dose. As a consequence of the different procedures used in their calculation they are incompatible, and adherence to one limit may result in a serious breach of the other. This paper explores the background to these limits, the problems posed by their application and proposes how best to achieve compliance with both limits.

Feasibility studies for assessing internal exposure to 233U.

The potential internal occupational exposure encountered as a consequence of the 232Th-233U fuel cycle are likely to arise predominantly from the inhalation of 232Th, 233U and (232Th + 233U) compounds of absorption Types M and S. In the past, although direct and indirect methods for assessments of internal exposure to 232Th and its daughters were developed, standardised and employed, no such attempts have been made with regard to 233U and 233U + 232Th. Therefore, feasibility studies for assessing internal exposure to 233U have been conducted using three methods: urine bioassay, in vivo counting and measurement of thoron gas in the exhaled breath of a worker. This paper describes details of these studies and discusses the results obtained.

Airborne uranium contamination--as revealed through elemental and isotopic analysis of tree bark.

A new strategy for characterisation of airborne uranium contamination based on ICP mass spectrometric analysis of tree bark is described. The uranium content of tree barks (50 samples) obtained from diverse locations (remote, rural, industrial) varied over almost four orders of magnitude (0.001-8.3 micrograms/g U) with maximum concentrations recorded in the vicinity of a nuclear fuel fabrication plant (0.70-8.3 micrograms/g U). Elevated concentrations were also observed near a coal-fired power station (0.25-0.38 microgram/g U). Isotopic analysis revealed significant deviation from the natural uranium isotope ratio (235U/238U, 0.00725) at four nuclear installations (235U/238U, 0.0055-0.0097). These findings indicate that tree bark serves as an effective biomonitor for uranium and, with isotopic analysis, discrimination between nuclear and non-nuclear emissions is realised.

Radiocaesium and radiostrontium uptake by turnips and broad beans via leaf and root absorption.

One of the immediate consequences of massive radioisotope release into the atmosphere is contamination of the biosphere. This contamination can affect plants either by direct deposition onto the leaves, or by contaminating the soil followed by absorption by the roots. Knowledge of the efficacy of the two routes of radionuclide incorporation into the food chain is fundamental to understanding the mechanisms by which radioactive contamination reaches man. The present work analyzes the incorporation of 134Cs and 85Sr via root and leaf uptake into the parts consumed by man, for two very different crops: turnip (Brassica napus) and broad bean (Vicia faba). The root uptake studies consider the available soil fraction for these two radionuclides, and indicate greater availability for 85Sr than for 134Cs which is fixed rapidly in the soil. For the study of leaf uptake, leaves were contaminated at three different stages of plant growth; the results indicate an inverse dependence of the transfer coefficients on the time elapsed from the moment of the contamination to harvesting of the edible parts.

Metabolism of uranium in the rat after inhalation of two industrial forms of ore concentrate: the implications for occupational exposure.

Aerosols produced from two commercially available ore concentrates in which the uranium was present essentially in the one as ammonium diuranate (ADU) and in the other as uranium octoxide (U3O8) were administered to rats. The results show that: 1 uranium in the ADU bearing material was cleared rapidly from the lungs, mainly to the blood, such that the retention kinetics were similar to those for a class D (highly transportable) compound as defined by ICRP; 2 uranium in the U3O8 bearing material was removed from the lungs principally by mechanical processes, the retention kinetics in this case being similar to those defined for a class Y (poorly transportable) compound; 3 for both materials the distribution of uranium amongst body tissues and the fraction of the systemic content excreted in urine were similar to those obtained after the injection of soluble hexavalent compounds; 4 for workers potentially exposed to both these materials, urine monitoring and lung radioactivity counting measurements should be used in addition to air sampling procedures for assessing the intake of uranium. 5 intakes of the ADU bearing material should be restricted to those permitted for short-term exposures on the basis of chemical toxicity, whereas those for the U3O8 bearing material should be governed by radiation dose.