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.

Depleted and enriched uranium exposure quantified in former factory workers and local residents of NL Industries, Colonie, NY USA.

BACKGROUND: Between 1958 and 1982, NL Industries manufactured components of enriched (EU) and depleted uranium (DU) at a factory in Colonie NY, USA. More than 5 metric tons of DU was deposited as microscopic DU oxide particles on the plant site and surrounding residential community. A prior study involving a small number of individuals (n=23) indicated some residents were exposed to DU and former workers to both DU and EU, most probably through inhalation of aerosol particles. OBJECTIVES: Our aim was to measure total uranium [U] and the uranium isotope ratios: (234)U/(238)U; (235)U/(238)U; and (236)U/(238)U, in the urine of a cohort of former workers and nearby residents of the NLI factory, to characterize individual exposure to natural uranium (NU), DU, and EU more than 3 decades after production ceased. METHODS: We conducted a biomonitoring study in a larger cohort of 32 former workers and 99 residents, who may have been exposed during its period of operation, by measuring Total U, NU, DU, and EU in urine using Sector Field Inductively Coupled Plasma - Mass Spectrometry (SF-ICP-MS). RESULTS: Among workers, 84% were exposed to DU, 9% to EU and DU, and 6% to natural uranium (NU) only. For those exposed to DU, urinary isotopic and [U] compositions result from binary mixing of NU and the DU plant feedstock. Among residents, 8% show evidence of DU exposure, whereas none shows evidence of EU exposure. For residents, the [U] geometric mean is significantly below the value reported for NHANES. There is no significant difference in [U] between exposed and unexposed residents, suggesting that [U] alone is not a reliable indicator of exposure to DU in this group. CONCLUSIONS: Ninety four percent of workers tested showed evidence of exposure to DU, EU or both, and were still excreting DU and EU decades after leaving the workforce. The study demonstrates the advantage of measuring multiple isotopic ratios (e.g., (236)U/(238)U and (235)U/(238)U) over a single ratio ((235)U/(238)U) in determining sources of uranium exposure.

An intake of C14-labelled dichlorobenzene.

An intake of C14 in the form of dichlorobenzene was followed up with 90 spot urine samples over a period of almost 2 weeks. This dataset has been fitted by a model consisting of three exponential terms. The intake and effective dose have been calculated. This case has been used to examine the effects of recent proposals by ICRP concerning the calculation of effective dose and the use of non-standard biokinetic models.

An analysis of workers' tritium concentration in urine samples as a function of time after intake at Korean pressurised heavy water reactors.

In general, internal exposure from tritium at pressurised heavy water reactors (PHWRs) accounts for ∼20-40 % of the total radiation dose. Tritium usually reaches the equilibrium concentration after a few hours inside the body and is then excreted from the body with an effective half-life in the order of 10 d. In this study, tritium metabolism was reviewed using its excretion rate in urine samples of workers at Korean PHWRs. The tritium concentration in workers' urine samples was also measured as a function of time after intake. On the basis of the monitoring results, changes in the tritium concentration inside the body were then analysed.

Screening methods for estimating tritium dose.

Tritium intake may occur in certain workplaces by design or by accident. If the health physics staff has developed a formal bioassay program, then it is likely that dose estimates from tritium intake are readily determinable. However, in the case of tritium intake at a facility where no formal program exists, it may be necessary to make simple confirmatory estimates of dose due to tritium exposure. Lifetime dose estimates may be calculated by using data from urine samples taken over a period of time. If urine data are unavailable, estimates of committed dose equivalent may be made with air sample data and knowledge of workplace activities.

Internal dose assessment of 210Po using biokinetic modeling and urinary excretion measurement.

The mysterious death of Mr. Alexander Litvinenko who was most possibly poisoned by Polonium-210 ((210)Po) in November 2006 in London attracted the attention of the public to the kinetics, dosimetry and the risk of this high radiotoxic isotope in the human body. In the present paper, the urinary excretion of seven persons who were possibly exposed to traces of (210)Po was monitored. The values measured in the GSF Radioanalytical Laboratory are in the range of natural background concentration. To assess the effective dose received by those persons, the time-dependence of the organ equivalent dose and the effective dose after acute ingestion and inhalation of (210)Po were calculated using the biokinetic model for polonium (Po) recommended by the International Commission on Radiological Protection (ICRP) and the one recently published by Leggett and Eckerman (L&E). The daily urinary excretion to effective dose conversion factors for ingestion and inhalation were evaluated based on the ICRP and L&E models for members of the public. The ingestion (inhalation) effective dose per unit intake integrated over one day is 1.7 x 10(-8) (1.4 x 10(-7)) Sv Bq(-1), 2.0 x 10(-7) (9.6 x 10(-7)) Sv Bq(-1) over 10 days, 5.2 x 10(-7) (2.0 x 10(-6)) Sv Bq(-1) over 30 days and 1.0 x 10(-6) (3.0 x 10(-6)) Sv Bq(-1) over 100 days. The daily urinary excretions after acute ingestion (inhalation) of 1 Bq of (210)Po are 1.1 x 10(-3) (1.0 x 10(-4)) on day 1, 2.0 x 10(-3) (1.9 x 10(-4)) on day 10, 1.3 x 10(-3) (1.7 x 10(-4)) on day 30 and 3.6 x 10(-4) (8.3 x 10(-5)) Bq d(-1) on day 100, respectively. The resulting committed effective doses range from 2.1 x 10(-3) to 1.7 x 10(-2) mSv by an assumption of ingestion and from 5.5 x 10(-2) to 4.5 x 10(-1) mSv by inhalation. For the case of Mr. Litvinenko, the mean organ absorbed dose as a function of time was calculated using both the above stated models. The red bone marrow, the kidneys and the liver were considered as the critical organs. Assuming a value of lethal absorbed dose of 5 Gy to the bone marrow, 6 Gy to the kidneys and 8 Gy to the liver, the amount of (210)Po which Mr. Litvinenko might have ingested is therefore estimated to range from 27 to 1,408 MBq, i.e 0.2-8.5 microg, depending on the modality of intake and on different assumptions about blood absorption.

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.

Relative role of plutonium excretion with urine and feces from human body.

The ratio of plutonium content in 35 pairs of daily fecal and urine samples from 19 former MAYAK workers several decades after the end of occupational exposure was measured in clinical conditions. No dependence of the ratio Pu(feces)/Pu(urine) on plutonium aerosol transportability, sex, and age of workers was revealed in the late times after the end of occupational exposure. It was found that at the late times after the end of occupational exposure, the ratio of feces/urine is characterized by the lognormal distribution with the median value, 0.57, and error for this index characterized geometric deviation, sigmag = 1.12 Urinary and fecal excretions were analyzed after chronic exposure to inhaled plutonium compounds of different transportability for another group of 345 workers. During 500-16,000 d after the started chronic inhalation, plutonium biokinetic model ("Doses-2000") used in Southern Ural Biophysics Institute (SUBI) and based on the ICRP Publication 66 overestimated the feces/urine ratio by an order of magnitude as compared with the observed values. It indicates a necessity for further improvement of the biokinetic model used in SUBI.

Human biokinetics of inhaled terbium oxide.

Four healthy men inhaled a monodisperse aerosol of 160Tb-labelled terbium oxide particles. The behaviour of the tracer was studied through measurements of body radioactivity and of its urinary and faecal excretion. Estimated early faecal losses in the four subjects ranged from 3% to 31% of the initial respiratory-tract deposit; most of the residue had become systemic within a year, with the principal deposit apparently in bone. Interference from this systemic deposit prevented accurate determination of the long-term pulmonary clearance kinetics, but the pattern was broadly what would be expected for Type M materials in the ICRP's Human Respiratory Tract Model. Averaged trends in the whole-body residue after approximately 1 year suggest a clearance half-life of approximately to 5 y.

Comparison of absorption after inhalation and instillation of uranium octoxide.

Values for the absorption parameters were compared after inhalation or intratracheal instillation of 1.5 microm mass median aerodynamic diameter (MMAD) 233U3O8 particles into the lungs of HMT strain rats. The two sets of parameter values were similar, as were the calculated dose coefficients and predicted biokinetics for workers. Hence the inhalation and instillation techniques can probably both be used to generate values of the absorption parameters for U3O8.

Assessment of the internal effective dose of workers independent of inhaled particle size (II).

For 60Co (Type S) and 54Mn (Type M), for which the whole-body content can be measured, it is possible to minimise the errors of the estimated effective doses caused by uncertainty of the activity median aerodynamic diameter (AMAD) by assuming the AMAD to be 5 microm and by measuring the body content on day 5 after inhalation. For the radionuclides to be measured in the lung content, e.g. 239Pu (Type S), it may be necessary to estimate the AMAD, because the lung burdens on any day are not always proportional to the whole-body content which reflects the effective doses. There is no problem in assuming the AMAD to be 5 microm for external counting and for urinalysis of Type F compounds, because of the rapid absorption of such compounds into the blood and the same biokinetics. The breathing rate is assumed to be 1.2 m3 h(-1).

Two case studies of highly insoluble plutonium inhalation with implications for bioassay.

Two well characterised Pu inhalation cases show some remarkable similarities between substantially different types of Pu oxide. The circumstances of exposure, therapy, bioassay data, chemical solubility studies and dosimetry associated with these cases suggest that highly insoluble Pu may be more common than previously thought, and can pose significant challenges to bioassay programmes.

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.

An intake of americium oxide powder: implications for biokinetic models for americium.

A worker inhaled 241AmO2 powder. Air sampling showed low activities but a nose blow revealed 92 Bq. Results from faecal sampling and lung and whole-body monitoring indicated an intake of about 200 Bq, but urine sampling, though commencing only 1 d after intake, showed below-threshold activities (< 0.2 mBq). This conflicts with predictions based on the ICRP Publication 67 biokinetic model for americium and the ICRP Publication 66 model for the human respiratory tract, if default lung parameters are used.

'Dose per unit content' functions: a robust tool for the interpretation of bioassay data.

The purposes of this study were to investigate the influence of the consequences of the lack of primary bioassay information and to elaborate approaches which could improve the reliability of dose assessments. The aggregated time-dependent functions 'dose per unit organ (excretion) content' z(t) have been proposed in this study as a convenient and reliable tool for bioassay. The analysis of the variation of z with changes of AMAD has demonstrated the existence of areas of the relative invariance of z, which permits the selection of one (reference) function z for the whole area of stability. Within the framework of such an approach an arbitrary set of bioassay data can be approximated by the linear combination F(t) = sum(i) E(i)/z(t - tau(i)), where F(t) = function of time t, which approximates the observed bioassay time trend; tau(i) = time shift of the acute intake i; E(i) = effective dose, associated with the acute intake i (the two last parameters are results of the approximation procedure).

Dosimetric implications of atmospheric dispersal of tritium near a heavy-water research reactor facility.

An estimate of the tritium dose to the public in the vicinity of the heavy water research reactor facility at AECL-Chalk River Laboratories, Ontario, Canada, has largely been accomplished from analyses on regularly-collected samples of air, precipitation, drinking water and foodstuffs (pasture, fruit, vegetables and milk) and environmental dose models. To increase the confidence with which public doses are calculated, tritium doses were estimated directly from the ratio of tritiated species in urine samples from members of the general public. Single cumulative 24 h urine samples from a few adults living in the vicinity of the heavy-water research reactor facility at Chalk River Laboratories, Canada were collected and analysed for tritiated water and organically bound tritium. The participants were from Ottawa (200 km east), Deep River (10 km west) and Chalk River Laboratories. Tritiated water concentrations in urine ranged from 6.5 Bq.l-1 for the Ottawa resident to 15.9 Bq.l-1 for the Deep River resident, and were comparable to the ambient levels of tritium-in-precipitation at their locations. The ultra-low levels of organically bound tritium in urine from these same individuals were measured by 3He-ingrowth mass spectrometry and were 0.06 Bq.l-1 (Ottawa) and 0.29 Bq.l-1 (Deep River). For Chalk River Laboratories workers, tritiated water concentrations in urine ranged from 32 Bq.l-1 to 9.2 x 10(4) Bq.l-1, depending on the ambient levels of tritium in their workplace. The organically bound tritium concentrations in urine from the same workers were between 0.08 Bq.l-1 and 350 Bq.l-1. With a model based on the ratio of tritiated water to organically bound tritium in urine, the estimated dose arising from organically bound tritium in the body for the Ottawa and Deep River residents was about 26% and 50%, respectively, of the body water tritium dose. The workers in a reactor building at Chalk River Laboratories had less than 10% dose contribution from organically bound tritium, but had higher overall tritium dose due to frequent intakes of tritiated water vapour in the workplace. The results of this study suggest that most of the tritium dose to workers at Chalk River and general population near Chalk River is the result of tritiated water intakes and not due to dietary intake of organically bound tritium.