Assessment of intake of a complex radionuclide bearing dust formed at a nuclear power plant

The aim of this work was to provide an experimental basis for assessing intakes of an industrial actinide-bearing dust from measurements of⁶⁰Co and¹³⁷Cs in the body or urine. Whilst these radionuclides comprised 72% and 19% of the radioactivity present, greater than 90% of the committed effective dose will result from the low concentrations of the actinides present, 0.4%. To assess the dose coefficient for the dust and predict the biokinetics of⁶⁰Co and¹³⁷Cs in workers, absorption parameters for transfer from lungs to blood obtained from an animal study were combined with information on particle deposition and clearance from the ICRP human respiratory tract model and with tissue distribution and excretion data from the most recent systemic models. All other radionuclides were assumed to have Type M absorption characteristics. The dose coefficient for the dust, 1.29·10^–7 Sv·Bq^–1 was estimated to contain 113 kBq⁶⁰Co, 29 kBq¹³⁷Cs and 0.64 kBq of the actinides. The predicted retention and excretion characteristics of⁶⁰Co and¹³⁷Cs in workers after acute or chronic exposure to the dust suggested that measurements of these radionuclides in the body or urine could detect intakes equivalent to a few percent of an annual dose limit of 20 mSv·y^–1.     

Implications of postmortem human tissue analysis on biokinetic models for actinides

Changes and refinements to original biokinetic models, based on postmortem radiochemical measurements of the concentration and distribution of actinides in tissues obtained from volunteer donors with known occupational experience with actinides, are discussed with emphasis on applications to operational health physics. Analysis of five whole body donations to the United States Transuranium Registry indicates that the²³⁹Pu model put forth in ICRP Publication 30 is generally applicable, although there is a significant fraction missing from the model that is retained in the muscle. For²⁴¹Am, the more recent model put forth in ICRP Publication 48 fits the autopsy data better than the model in Publication 30, although the observed retention half-time in the liver is on the order of two to three years rather than 20 years proposed by the model. An estimated 20% of the initial systemic deposition for²⁴¹Am goes to the muscle, where it has a residence half-time estimated at ten years. For both Pu and Am, less than 5% of the skeletal actinide in the skeleton is found in the marrow. The highest concentrations appear to be associated with the periosteum and endosteum. A significantly greater fraction of inhaled Pu and Am is retained in the lungs than is predicted by current models. Differences in the actinide distribution between lung and the associated lymph nodes are observed in smokers as compared with non-smokers.     

Recent developments in biokinetic models and the calculation of internal dose coefficients

In most cases the measurement of radioactivity in an environmental or biological sample will be followed by some estimation of dose and possibly risk, either to a population or an individual. This will normally involve the use of a dose coefficient (dose per unit intake value) taken from a compendium. In recent years the calculation of dose coefficients has seen many developments in both biokinetic modelling and computational capabilities. ICRP has recommended new models for the respiratory tract and for the systemic behavior of many of the more important elements. As well as this, a general age-dependent calculation method has been developed which involves an effectively continuous variation of both biokinetic and dosimetric parameters, facilitating more realistic estimation of doses to young people. These new developments were used in work for recent ICRP, IAEA and CEC compendia of dose coefficients for both members of the public (including children) and workers. This paper presents a general overview of the method of calculation of internal doses with particular reference to the actinides. Some of the implications for dose coefficients of the new models are discussed. For example it is shown that compared with data in ICRP Publications 30 and 54: the new respiratory tract model generally predicts lower deposition in systemic tissues per unit intake; the new biokinetic models for actinides allow for burial of material deposited on bone surfaces; age-dependent models generally feature faster turnover of material in young people. All of these factors can lead to substantially different estimates of dose and examples of the new dose coefficients are given to illustrate these differences. During the development of the new models for actinides, human bioassay data were used to validate the model. Thus, one would expect the new models to give reasonable predictions of bioassay quantities. Some examples of the bioassay applications, e.g., excretion data for the plutonium model, are discussed briefly.     

A critical review of bioassay techniques for actinides in light of ICRP recommendations for monitoring workers

A critical review is presented of bioassay techniques for actinides in light of ICRP recommendations for monitoring workers. It is obvious that very sensitive techniques are required to meet these recommendations. Alpha spectrometry, the most commonly employed technique for measuring actinides in bioassay samples, has limited sensitivity. There are, however, certain techniques which are sensitive enough to meet the recommendations of ICRP, such as, fission track analysis for²³⁹Pu and²³⁵U, neutron activation analysis for²³²Th, mass spectrometry for a number of radionuclides, and many techniques for uranium. ICP-mass spectrometry does not have enough sensitivity to be implemented as a method of choice for the bioassay of actinides at present, however, it is quite promising.     

Specific absorption parameters for uranium octoxide and dioxide applicable to the ICRP Publication 66 respiratory tract model

Literature data from in vivo chest measurements and urinary excretion rates of individuals exposed to U₃O₈ and UO₂ were used to compare the results predicted by different models with empirical observations in humans. As a result the use of the respiratory tract model proposed in ICRP Publication 66 with its default absorption parameters underestimates urinary excretion of inhaled U₃O₈ and UO₂. The new respiratory tract model also overpredicts the Fecal/Urine activity ratio, independently of the systemic model. For U₃O₈ and UO₂ the choice of systemic model has very little influence on the predicted urinary excretion of inhaled compounds. On the other way, the choice of the respiratory tract model does influence the predicted urinary excretion significantly. In this work specific absorption parameters for U₃O₈ and UO₂ were derived to be used in the respiratory tract model proposed in ICRP Publication 66. The predicted biokinetics of these compounds were compared with those derived for Type M and Type S compounds of uranium.     

Clearance of Radioactivity Deposited in the Respiratory Tract to Blood: Progress in a Multinational Interspecies Comparison Project

Due to the diversity of the chemical forms of radionuclides inhaled in industry and the environment, the assessment of intake and dose is based frequently on biokinetic studies of the materials in laboratory animals. The ICRP respiratory tract and systemic models provide an effective framework for extrapolating the results of such studies to humans, but there is a paucity of data concerning the crucial assumption that the absorption rates from lungs into blood for a given material are independent of the mammalian species. To address this uncertainty, biokinetic studies involving five chemical compounds and four mammalian species are being conducted. The compounds, with the species in parenthesis, are Pu-nitrate (man, primate, rat), Gd-oxide (man, primate, dog, rat), Np- oxide and nitrate (primate, rat), and U-octoxide (primate, dog, rat). This paper describes progress to date.     

Absorption kinetics of uranium tri-n-butyl phosphate in the rat: Implications for occupational exposure

The absorption kinetics for uranium into blood after deposition as tri-n-butylphosphate (UTBP) in the rat lung were combined with human data on particle deposition and clearance from the ICRP Publication 66 respiratory tract model and information from the most recent ICRP biokinetic model for uranium to predict the consequences for exposure of workers. These predictions suggest that, (1) the biokinetics of UTBP are similar to those for a Type F compound as defined by ICRP, (2) the dose coefficient is essentially independent of the aerosol size and isotopic composition, (3) the mass of uranium equivalent to the ALI can vary by 13 fold depending upon the isotopic composition, (4) intakes of uranium as UTBP other than chronic intakes as highly enriched forms should be restricted on the basis of the chemical toxicity of uranium, (5) the assessment of intake by urine bioassay measurements should be interpreted with caution unless the exposure conditions are well defined and (6) severe kidney damage is unlikely at intakes corresponding to the ALI or daily limit.     

Rapid column extraction method for actinides and strontium in fish and other animal tissue samples

The analysis of actinides and radiostrontium in animal tissue samples is very important for environmental monitoring. There is a need to measure actinide isotopes and strontium with very low detection limits in animal tissue samples, including fish, deer, hogs, beef and shellfish. A new, rapid separation method has been developed that allows the measurement of plutonium, neptunium, uranium, americium, curium and strontium isotopes in large animal tissue samples (100–200 g) with high chemical recoveries and effective removal of matrix interferences. This method uses stacked TEVA Resin®, TRU Resin® and DGA Resin® cartridges from Eichrom Technologies (Darien, IL, USA) that allows the rapid separation of plutonium (Pu), neptunium (Np), uranium (U), americium (Am), and curium (Cm) using a single multi-stage column combined with alphaspectrometry. Strontium is collected on Sr Resin® from Eichrom Technologies (Darien, IL, USA). After acid digestion and furnace heating of the animal tissue samples, the actinides and ^89/90Sr are separated using column extraction chromatography. This method has been shown to be effective over a wide range of animal tissue matrices. Vacuum box cartridge technology with rapid flow rates is used to minimize sample preparation time.     

Incorporation monitoring by measurements of activity concentrations in air

The incorporation monitoring of workers handling actinides is in many cases not possible by individual methods: The sensitivity of bioassay of methods (in vivo, in vitro) is not sufficient to detect amounts as required by the low annual limits of intake. Similar difficulties may occur with the use of radionuclides with very short physical half-lives. In these cases, the measuring of activity concentrations in the air is the only way to monitor the workers and to meet legal requirements. The essential problem connected with this approach is to make sure, that the air sample analyzed represents the average air inhaled actually. Correspondingly, the new system regulating the incorporation monitoring in Germany requires additional measures to ensure this representatively.     

Relevance of ICRP metabolic model of Th in bio-assay monitoring

This paper compares the urinary excretion levels of Th obtained in bio-assay monitoring using the neutron activation technique with those predicted by applying the ICRP metabolic model to the measured Th activity in chest and total body of a group of Thorium plant workers. The results indicated much lower urinary Th excretion as compared to what was expected on the basis of the ICRP model. Lower urinary excretion in occupational subjects is explained in terms of negligible contribution of skeleton and soft tissue to the activity excreted in urine. It is suggested that the existing model should be modified to enable it to be applicable to the bio-assay monitoring of occupational workers.     

A comparison of239+240Pu post-mortem measurements with estimates based on current ICRP models

Measurements of^239+240Pu in human tissues, from nuclear weapons testing, provide an invaluable source of data for verifying the uptake and distribution of radionuclides in the body. Measured concentrations of^239+240Pu in lung, tracheobronchial lymph nodes, liver and skeleton have been compared with concentrations calculated using estimated plutonium intakes, the ICRP Publication 66 Respiratory Tract Model and the ICRP Publication 67 biokinetic model for plutonium. Measurement data tend to fall between the concentrations estimated on the basis of Type M and Type S absorption parameters. This indicates that the models represent the movement of plutonium through the body reasonably well.     

Using animal dosimetry models to interpret human bioassay data for actinide exposures

Bioassay and dosometry models are needed to estimate intakes of radionuclides, and to calculate radiation doses to target tissues following such in takes. Because of the diversity of exposure materials, individual biological variabilities, and the general lack of adequate bioassay information and knowledge of the metabolism of radionuclides, current models are based mostly on empiricism. This paper describes biokinetic/dosimetry models for U, Am, and Cm. They are based on experimental data developed from studies in dogs that inhaled one of the above radionuclides in specific chemical forms and specific particle sizes. The models, which are based on similar biological principles, and, therefore, have similar structure, are applied to the very sparse human bioassay data available from cases of exposure to either U, Am, or Cm. The results thus far indicate that the lung retention for the different actinides are well described by the models, that urinary bioassay data can be described within limited time periods, and that the fecal excretion rate is not adequately described. Improvements in modeling are predicted on increased publication of human bioassay data, and better cooperative interaction between model developers and health protection professionals responsible for industrial bioassay programs.     

Evaluation of the Linear-Elution-Strength Model for the Prediction of Retention and Selectivity in Isothermal Gas Chromatography

Linear-elution strength theory and temperature-programmed gas chromatography is evaluated as a rapid method for predicting isothermal retention factors and column selectivity. Retention times for a wide range of compounds are determined at the program rates of 3 and 12 °C/min for the temperature range 60 to 160 °C on three open-tubular columns (DB-1701, DB-210 and EC-Wax) and used to predict isothermal retention factors for each column over the temperature range 60 to 140 °C. The temperature-program predicted isothermal retention factors are compared with experimental values using linear regression and the solvation parameter model. It is shown that isothermal retention factors predicted by the linear-elution-strength model only approximately represents the experimental data. The model fails to predict the slight curvature that exists in most plots of the experimental retention factor (log k) as a function of temperature. In addition, regression of the temperature-program predicted isothermal retention factors against the experimental values indicates that the slopes and intercepts deviate significantly from their target values of one and zero, respectively, in a manner which is temperature dependent. The temperature-program predicted isothermal retention factors result in system constants for the solvation parameter model that are different to those obtained from the experimental retention factors. These results are interpreted as indicating that linear-elution-strength theory predicts retention factors that fail to accurately model stationary phase interactions over a wide temperature range. It is concluded that temperature-program methods using linear-elution-strength theory are unsuitable for constructing system maps for isothermal separations.     

Liquid chromatographic determination of rifampin in human plasma, bronchoalveolar lavage fluid, and alveolar cells

A technique is presented for the measurement of rifampin in humans by reversed-phase column chromatography and postcolumn photo irradiation. The assay employs diazepam as an internal standard and provides specific, rapid, and reliable determinations for drug concentration in plasma, bronchoalveolar lavage (BAL), and alveolar cells (AC). The preparation of plasma and AC samples utilizes a simple deproteinization step, whereas BAL supernatants require a solid-phase extraction. The assay produces sharp peaks with retention times of 6.2 and 15 min for rifampin and diazepam, respectively. The detection limits for rifampin were 0.5 microgram/mL for plasma, 0.015 microgram/mL for BAL supernatants, and 0.03 microgram/mL for AC suspensions. The assay has excellent performance characteristics, making it suitable for pharmacological studies in humans, and it is being used to support a study of the intrapulmonary pharmacokinetics of rifampin.     

Modified respiratory tract model for uranium: Its implications on bioassay interpretations

The excretion of inhaled poorly transportable compounds of uranium relative to chest content has been measured in humans by a substantial number of measurements of urine, feces, andin vivo measurements over the chest. The use of these measurements have permitted us to compare the results predicted by the models with empirical observations in humans. The ICRP-30 model for inhaled class Y compounds of uranium along with the ICRP-30 systemic model, no matter what the particle size, grossly underpredicts urinary excretion over time than that observed in human occupationally exposed to poorly transportable compounds of uranium by inhalation. Conversely, if urinary excretion were to be used to estimate the contents of poorly transportable uranium compounds in the lung using ICRP-30 models, the results would be significantly overestimated. The new ICRP (ICRP-66) respiratory tract model also grossly underestimates urinary excretion of inhaled poorly transportable uranium compounds and exacerbates the problem, at least for the default values of the parameters of the model. A lung model derived from the original ICRP-30 lung model, which is named modified, has been proposed in this work. It predicts urinary excretion better, even though it is not entirely satisfactory in predicting urine/fecal ratio in excreta.     

Sensitivity of doses and associated uncertainties in bioassay estimates to ICRP Publication 66 Respiratory Tract Dosimetric Model with respect to the parameters: Ventilation rates, time budget, total and regional deposition, oral versus nasal breathing and clearance rates of compartments

An analysis of the reliability of the ICRP's dose coefficients for intake of radionuclides, applied on the Human Respiratory Tract Dosimetry Model proposed in ICRP Publication No. 66 was carried out, with respect to the following variables: ventilation rates, time budget, total deposition, regional deposition for the four respiratory tract compartments (alveolar-interstitium, bronchioles, bronchi and extrathoracic), oral versus nasal breathing patterns, and variation in clearance rates of compartments. The analysis was done by calculating reliability factors defined as the square root of the ratio of larger to smaller dose coefficient calculated at the extreme values for the model parameter being tested, in intervals of values of the effective dose. Calculations for each of the variables were carried out for an adult, using these 12 radionuclides: ³H, ⁶⁰Co, ⁹⁰Sr, ⁹⁵Zr, ¹⁰⁶Ru, ¹²⁵Sb, ¹³¹I, ¹³⁷Cs, ²¹⁰Pb, ²²⁶Ra, ²³⁸U and ²³⁹Pu. For AMAD = 0.1 mm the analysis associated with the total deposition in the compartments indicated a Reliability Category II. For AMADs = 1.0 and 10 mm the analysis associated with the deposition in the extrathoracic compartments indicated a Reliability Category II. For AMAD = 10 mm the deposition in the compartments of the tracheobronchial region also showed a Reliability Category II. Most results for all other parameters for the studied AMADs were found to be in Category I. The corresponding impacts on the uncertainties in the predicted bioassay results for these twelve radionuclides were also determined. This analysis is especially helpful when doses are estimated through bioassay measurements employing the ICRP Publication 66respiratory tract model.     

Applications of laser photoacoustic spectroscopy using an optical parametric oscillator to the study of complexation equilibria in dilute aqueous solutions

A 30 Hz YAG laser pumped, narrow-line, optical parametric oscillator (OPO) has been used to investigate the chemical states of selected compounds in aqueous solution. The OPO system has the advantage that it can scan wavelengths over large ranges without significant loss of output power. The visible spectra of rare earth complexes in dilute aqueous solutions (as chemical analogs for the actinides) have been studied and preliminary qualitative results for erbium acetate complexes at the 100 micromolar level are in good agreement with literature data. Quantitative measurements of the protonation constant for phenol red at the 100 nanomolar level were measured. The particular implementation of the OPO system used in this work introduced a number of spectral artifacts due to optical signal overlap with near-infrared water absorption bands. In addition, it was demonstrated that the concentration limiting factor for photoacoustic spectroscopy is the intrisic absorption of water in the visible region of the spectrum.     

Size exclusion chromatographic cleanup for GC/MS determination of organophosphorus pesticide residues in household and vehicle dust

Size exclusion chromatography (SEC) was used as a cleanup method for the analysis of organophosphorus pesticides in household and vehicle dusts. The pesticides investigated were diazinon, methyl parathion, chlorpyrifos, malathion, phosmet, and azinphosmethyl. These compounds are of interest due to their use in agricultural tree fruit production and/or urban pest control. Pesticides were determined via gas chromatography/mass spectrometry with selected-ion monitoring and cool on-column injection. The lower limit of method validation was 0.20 microg/g. Method limits of detection in dust ranged from 0.012-0.055 microg/g. Dust samples were collected with vacuums from the homes and vehicles of people living and working in a rural agricultural region in the central part of Washington State. The analytes were extracted from the dust by sonication in acetone. The extracts were solvent-exchanged to cyclohexane, frozen, thawed, and centrifuged prior to SEC injection. Following SEC, the eluent was split into 2 fractions, concentrated, and injected on-column into the gas chromatograph. This method represents the first complete publication describing the SEC cleanup of organophosphorus pesticides in dusts. Recoveries of pesticides in dusts ranged from 63.5-110.8 +/- 4.9-19.6% over a fortification range of 0.20-10.00 microg/g. This optimized, automated, and reproducible SEC method does not require further treatment or cleanup for trace determination of these organophosphorus pesticides.     

Assessment of Iodine in the Diet of People Living Around a Nuclear Reprocessing Plant: Dose-Related Consequences of an Intake of 129I

It is important that in radioiodine dosimetry for low levels of daily intake, allowance must be made for the normal daily intake of stable iodine. This intake varies from one region to another, and variations are observed from one person to the next within a region, depending on eating habits. Measuring iodine in the urine over 24 hours can indirectly assess these variations. Analysis of the total iodine in the urine was carried out for 69 French people living in a temperate maritime region or in mainland France. This study justifies individual assessment of the coefficient of iodine transfer to the thyroid by means of this survey based on the urinary iodine analysis. The consequences for man of the release of ¹²⁹I around a nuclear reprocessing plant were analyzed by applying the methodology published previously by the authors. A software program based on the iodine biokinetic model recommended by the ICRP was used to calculate the daily urine excretion of ¹²⁹I for five different diets of total iodide in a ratio of 10^-4 for ¹²⁹I/¹²⁷I. This model makes it possible to set a practical detection limit of 20 mBq (0.003 µg). This approach is important from a practical point of view for health physicists involved in routine monitoring of workers in the nuclear field and members of the public exposed to radioiodine released into the environment.     

中国正常成年人体内的钙含量

介绍了中国１００例正常成年人２０个脏器组织中１５种元素的含量检测研究。结果表明,中国与ＩＣＲＰ相比,人体内元素含量值存在差异,从而为修订ＩＣＲＰ参考人参数提供了中国人上述元素含量的参数。