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PubMed2005

Uranium oligomerization in chloride-based high temperature melts: in situ XAS studies.

In situ EXAFS spectroscopic studies of uranium compounds in high temperature alkali chloride melts indicate the presence of oligomeric species. An investigation into UCl(3) and UCl(4) dissolved in LiCl reveals long range ordering of uranium atoms in the molten state which is not maintained on quenching. Studies of uranium dioxide dissolved in LiCl-KCl eutectic with HCl exhibit long range ordering in both molten and quenched states, and the EXAFS data can be modeled using multiple coordination shells.

Journal Article↗
PubMed2001

222Rn emanation from uranium-glazed ceramics.

Orange-red uranium-glazed dinnerware was found to emanate 222Rn to produce an average of less than 0.1 Bq 222Rn decay per piece, which should have no associated health risks. Comparison of 222Rn emanation to 226Ra in glazes (measured by alpha spectrometry) indicated inefficient emanation (<5%) of 222Rn, consistent with the low radon levels observed and with the presence of 222Rn progeny in glazes. These studies also showed that reagent grade uranium compounds may emanate measurable 222Rn.

Ceramics↗
PubMed2000

Orally administered ethane-1-hydroxy-1,1-biphosphonate reduces the lethal effect of oral uranium poisoning.

Intoxication with uranium compounds is both an occupational risk for the workers engaged in the different processes of the elaboration of nuclear fuel and a risk for the population at large in terms of contaminated water and food. The toxic effects of uranium can be reduced by the administration of a biphosphonate, ethane-1-hydroxy-1,1-biphosphonate (EHBP), subcutaneously or intraperitoneally. The aim of the present work was to examine whether orally administered EHBP reduces the lethal effect of a single orally administered toxic dose of uranyl nitrate. Nine groups of 20 male Balb-c mice were used. Five groups received 350 mg kg(-1) of uranyl nitrate orally administered by gavage, four were co-treated 20 min later with EHBP either by gavage (350, 500, or 700 mg kg(-1)) or by subcutaneous injection (50 mg kg(-1)), and one group was not treated. Four groups of animals received only EHBP in doses and routes the same as those used in the intoxicated animals. Survival was assessed for 14 d. On day 14 the surviving animals of all groups were killed. An additional group of uranium intoxicated animals was killed on day 2 after the start of the experiment. Kidneys were examined histologically. On day 3 all the animals treated with uranyl nitrate alone and 20% of the animals treated with 700 mg kg(-1) of EHBP alone were dead. Survival at day 14 of the groups of mice intoxicated with uranyl nitrate and treated with EHBP (50 mg kg(-1) orally or 50 mg kg(-1) subcutaneously) was 45.0 and 49.6%, respectively. Tubule necrosis lesions were present in kidneys of mice intoxicated with uranyl nitrate, whereas lesions were less severe in mice treated with EHBP. Oral administration of EHBP is effective for reducing the lethal effect of uranium, and it is at least as useful as subcutaneous administration for prompt therapy of oral uranium exposure, achieving a survival rate of almost 50%.

Administration, Oral↗
PubMed1984

Techniques for yellowcake dissolution studies in vitro and their use in bioassay interpretation.

The high variability in solubility of yellowcake produced by different mills complicates the interpretation of routine bioassay data. A simple in vitro dissolution test is needed for yellowcake to improve this interpretation. A series of experiments was designed to evaluate the relative importance of solvent composition, method, pH and temperature in determining yellowcake dissolution according to a model developed from the known composition of a test yellowcake and data from inhalation exposures of humans to UO3 or U3O8. Useful in vitro dissolution results can be obtained using either simulated serum ultrafiltrate or simulated lung fluid as the solvent if dissolved and undissolved yellowcake are separated by a membrane filter. In vitro dissolution experiments estimated the soluble portion of the test yellowcake within +/- 6% (mean +/- 2 S.E.) and showed that the dissolution rates of the more soluble and less soluble portions corresponded to Class D and Class Y compounds, respectively. It was not necessary to maintain physiological pH or temperature conditions to approximate the "human" model. The greatest utility of in vitro dissolution results was in the estimation of the more soluble fraction of the yellowcake and to indicate whether prior excretion of a Class D uranium compound and possible kidney damage could have occurred before detection of an exposure. Some guidelines for the use of in vitro dissolution data in biassay interpretation are suggested based on ICRP Publication 30 recommendations.

Aerosols↗
PubMed1999

Implementation of ICP-MS protocols for uranium urinary measurements in worker monitoring.

The uranium concentration in human urine spiked with natural uranium and rat urine containing metabolized depleted uranium was determined by ICP-MS. The use of ICP-MS was investigated without any chemical treatment or after the different stages of a purification protocol currently carried out for routine monitoring. In the case of spiked urine, the measured uranium concentrations were consistent with those certified by an intercomparison network in radiotoxicological analysis (PROCORAD) and with those obtained by alpha spectrometry in the case of the urine containing metabolized uranium. The quantitative information which could be obtained in the different protocols investigated shows the extent to which ICP-MS provides greater flexibility for setting up appropriate monitoring approaches in radiation protection routines and accidental situations. This is due to the combination of high sensitivity and the accuracy with which traces of uranium in urine can be determined in a shorter time period. Moreover, it has been shown that ICP-MS measurement can be used to quantify the 235U isotope, which is useful for characterizing the nature of the uranium compound, but difficult to perform using alpha spectrometry.

Animals↗
PubMed2003

Properties, use and health effects of depleted uranium (DU): a general overview.

Depleted uranium (DU), a waste product of uranium enrichment, has several civilian and military applications. It was used as armor-piercing ammunition in international military conflicts and was claimed to contribute to health problems, known as the Gulf War Syndrome and recently as the Balkan Syndrome. This led to renewed efforts to assess the environmental consequences and the health impact of the use of DU. The radiological and chemical properties of DU can be compared to those of natural uranium, which is ubiquitously present in soil at a typical concentration of 3 mg/kg. Natural uranium has the same chemotoxicity, but its radiotoxicity is 60% higher. Due to the low specific radioactivity and the dominance of alpha-radiation no acute risk is attributed to external exposure to DU. The major risk is DU dust, generated when DU ammunition hits hard targets. Depending on aerosol speciation, inhalation may lead to a protracted exposure of the lung and other organs. After deposition on the ground, resuspension can take place if the DU containing particle size is sufficiently small. However, transfer to drinking water or locally produced food has little potential to lead to significant exposures to DU. Since poor solubility of uranium compounds and lack of information on speciation precludes the use of radioecological models for exposure assessment, biomonitoring has to be used for assessing exposed persons. Urine, feces, hair and nails record recent exposures to DU. With the exception of crews of military vehicles having been hit by DU penetrators, no body burdens above the range of values for natural uranium have been found. Therefore, observable health effects are not expected and residual cancer risk estimates have to be based on theoretical considerations. They appear to be very minor for all post-conflict situations, i.e. a fraction of those expected from natural radiation.

Aerosols↗
PubMed2003

PROCORAD's international intercomparisons highlight the evolution of techniques used to determine uranium in urine.

Inter-laboratory tests are a means of assessing the analytical coherence of medical laboratories. In radiotoxicology, this kind of exercise makes it possible to keep up with laboratory know-how and with the evolution and relative performances of analytical techniques. The intercomparison exercises organised by PROCORAD (Association for the Promotion of Quality Controls in Radiotoxicological Bioassays) provide an opportunity to compare and contrast radiochemistry and metrology for the in vitro analysis of urine and faeces. For uranium compounds, the development of new techniques such as inductively coupled plasma-mass spectrometry (ICP-MS), alpha spectrometry, and laser spectrofluorimetry makes it possible to compare the effectiveness of these protocols with respect to radiation protection monitoring, both in routine and special situations. Detection limits, flexibility, repeatability, reproducibility and isotopic quantification are the criteria considered in this study. The authors present the evolution of performances for the analysis of uranium in urine over the years. However, the goal of the laboratories taking part in these annual exercises is not only to check the accuracy of their results but also to have analytical discussions and the opportunity to exchange experiences that will enrich the group's general competence.

France↗
PubMed2006

The effect of repeated inhalation on the distribution of uranium in rats.

For the assessment of doses after inhalation of airborne uranium compounds by workers, the International Commission on Radiological Protection (ICRP) developed compartmental models that are used to calculate reference dose coefficients and retention and excretion functions. It is assumed that each acute intake has no effect on the biokinetics of later intakes. Consequently, retention and excretion after multiple or chronic exposure are predicted using the same models as after acute exposure. This assumption was tested here on rats exposed to repeated inhalation of uranium dioxide (UO2). First, excretion and organ retention were determined after a single inhalation of UO2. The follow-up of incorporated activity was used to design a biokinetic model for uranium inhaled by rats. Second, the biokinetics of uranium were monitored in two experiments of repeated inhalations of uranium dioxide under different intake patterns. For these two experiments, the organs' retention and excretion after repeated UO2 inhalation were predicted using the biokinetic model and compared to the experimental measurement. Under the two sets of experimental conditions considered, the prediction of the biokinetic model based on acute exposure data was consistent with the biokinetics observed after repeated UO2 inhalations, with the possible exception of retention in the skeleton.

Animals↗
PubMed2005

[Some health parameters in personnel contacting highly enriched uranium].

The authors analysed 20-years and longer observations over health state of personnel having occupational contact with highly enriched uranium. Findings are no determined effects as clinical manifestations of chronic uranium intoxication, presented by most frequently involved systems (hemopoietic, bronchopulmonary) and main organs accumulating uranium (liver, kidneys, bones). Long-term observations revealed malignancies in 11% of the examinees. Further medical observations over the personnel (risk group) are required to evaluate risk of aleatory effects in prolonged contact with various uranium compounds.

Adult↗
PubMed2001

Uranium bioassay--beyond urinalysis.

Assessment of occupational or environmental exposure to uranium compounds is largely based on urinalysis. However, urine samples generally reflect either recent exposure (within a few days after an incident) or chronic exposure and, furthermore, diurnal fluctuations in "spot samples" make it difficult to estimate the extent of the internal dose received. Thus, if urine samples are not collected within a relatively short time after accidental exposure or if the samples are not representative due to collection logistics, internal dosimetry calculations based only on urinalysis may be misleading. With the advent of efficient and sensitive methods for determination of uranium in hair and nails, some of these drawbacks may be overcome. It is proposed that with little additional cost, determination of the uranium in hair may yield better insights for internal dosimetry of uranium exposure.

Circadian Rhythm↗
PubMed2005

Genotoxic and inflammatory effects of depleted uranium particles inhaled by rats.

Depleted uranium (DU) is a radioactive heavy metal coming from the nuclear industry and used in numerous military applications. Uranium inhalation can lead to the development of fibrosis and neoplasia in the lungs. As little is known concerning the molecular processes leading to these pathological effects, some of the events in terms of genotoxicity and inflammation were investigated in rats exposed to DU by inhalation. Our results show that exposure to DU by inhalation resulted in DNA strand breaks in broncho-alveolar lavage (BAL) cells and in increase of inflammatory cytokine expression and production of hydroperoxides in lung tissue suggesting that the DNA damage was in part a consequence of the inflammatory processes and oxidative stress. The effects seemed to be linked to the doses, were independent of the solubility of uranium compounds and correlating with the type of inhalation. Repeated inhalations seemed to induce an effect of potentiation in BAL cells and also in kidney cells. Comet assay in neutral conditions revealed that DNA damage in BAL cells was composed partly by double strands breaks suggesting that radiation could contribute to DU genotoxic effects in vivo. All these in vivo results contribute to a better understanding of the pathological effect of DU inhalation.

Animals↗
PubMed1987

Mortality among workers at a uranium processing facility, the Linde Air Products Company Ceramics Plant, 1943-1949.

A retrospective cohort mortality study of 995 white males employed more than 30 d at a uranium processing facility in upstate New York between 1943 and 1949 investigated the association between excess observed deaths and long-term occupational exposure via inhalation to uranium compounds. Two comparison groups were used, the white male population of the United States and the white male population in the New York counties of Erie and Niagara. The vital status determination was 94.3% complete through 31 December 1979. With the use of the national comparison group, statistically significantly increased standardized mortality ratio (SMR) values were observed for all causes (SMR 118), laryngeal cancer (SMR 447), all circulatory diseases (SMR 118), arteriosclerotic heart disease (SMR 119), all respiratory diseases (SMR 152), and pneumonia (SMR 217). Site-specific outcomes of special interest with a statistically increased number of deaths above expected were laryngeal cancer (observed 5) and pneumonia (observed 17). No association was found with length of employment or work in the most hazardous areas of the plant. The comparison with regional rates gave similar results.

Ceramics↗
PubMed1995

Uranium dust exposure and lung cancer risk in four uranium processing operations.

We examined the relation between uranium dust exposure and lung cancer mortality among workers employed in four uranium processing or fabrication operations located in Missouri, Ohio, and Tennessee. Among workers who had at least 30 years of potential follow-up, we identified 787 lung cancer cases from death certificates and matched one control to each case. Health physicists estimated individual annual lung doses from occupational exposure primarily to insoluble uranium compounds, using contemporary monitoring data. With a 10-year lag, cumulative lung doses ranged from 0 to 137 centigrays (cGy) for cases and from 0 to 80 cGy for controls. Health physicists assigned annual external radiation doses to workers having personal monitoring records. Archivists collected smoking information from occupational medical records. Odds ratios for lung cancer mortality for seven cumulative internal dose groups did not demonstrate increasing risk with increasing dose. We found an odds ratio of 2.0 for those exposed to 25 cGy and higher, but the 95% confidence interval of 0.20 to 20 showed great uncertainty in this estimate. There was a suggestion of an exposure effect for workers hired at age 45 years or older. Further analyses for cumulative external doses and exposures to thorium, radium, and radon did not reveal any clear association between exposure and increased risk, nor did dichotomizing workers by facility.

Adult↗
PubMed2004

The hydrogen salicylate ion as ligand. Complex formation equilibria with dioxouranium (VI), neodymium (III) and lead (II).

The complexation equilibria of the hydrogen salicylate ion, HL(-), have been studied, at 25 degrees C, by potentiometric measurements with a glass electrode in 1 M NaClO4 for uranyl and Nd(III) ions and in 3 M NaClO4 for Pb(II) ion. The ligand concentration (CL) was varied between 10(-3) and 0.05 M. In the system with U(VI) the concentrations ranged between: 10(-3) < or = [U(VI)] < or = 0.01 M, 0.5 < or = CL /[U(VI)] < or = 10 and 10(-2) < or = [H+] < or = 10(-5) M; for neodymium system: 2 x 10(-3) < or = [Nd(III)] < or = 0.01, 1 < or = CL /[Nd(III)] < or = 10 and 10(-2) < or = [H+] < or = 10(-7) M; for lead system: 10(-3) < or = [Pb(II) < or = 3 x 10(-3), 1 < or = CL /Pb(II)] < or = 2 and 10(-5) < or = [H+] < or = 10(-7.3) M. The experimental data have been explained with the formation of UO2HL+, UO2L, UO2(OH)L(-), (UO2)2(OH)L2(-) UO2(HL)L(-), NdHL(2+), NdL(+), Nd(OH)L, PbHL(+), PbL and PbL2(2-). Equilibrium constants are given for the investigated ionic media and at infinite dilution.

Hydrogen-Ion Concentration↗
PubMed2005

A simple method for the absolute determination of uranium enrichment by high-resolution gamma spectrometry.

A simple method for the determination of uranium enrichment using high-resolution gamma spectrometry is presented in this paper. The method relies solely on the gamma-ray emission probabilities of 235U and 234mPa, and an iterative procedure for the least squares fit of a polynomial to a set of experimentally determined data. To ensure the reliability of the 234mPa gamma-ray emission probabilities employed, a new determination of these probabilities was carried out using a combination of gamma spectrometry and Cerenkov counting of a purified 234Th solution. Using these new data, a maximum difference of approximately 5% has been found between the experimental and declared uranium enrichment in a set of solid and liquid samples containing uranium compounds.

Journal Article↗
PubMed2003

When does gold behave as a halogen? Predicted uranium tetraauride and other MAu4 tetrahedral species, (M = Ti, Zr, Hf, Th).

Quantum chemical calculations suggest that a series of molecules with the general formula MAu4 are stable, where M = U, Th, and a group-4 atom. They correspond to Au in the formal valence state -1 and indicate that gold can act as a ligand similar to the halogen series. Of the MAu4 species studied, UAu4, the first predicted mixed gold uranium compound, has a short M-Au bond distance, 2.71 A, which would locate Au between Br and I from the bond length point of view in the U-tetrahalide series. Energetically, the U-Au bond is weaker than the corresponding U-Br and U-I bonds.

Journal Article↗
PubMed1988

Radiation doses and cause-specific mortality among workers at a nuclear materials fabrication plant.

A historical cohort mortality study was conducted among 6,781 white male employees from a nuclear weapons materials fabrication plant for the years 1947-1979. Exposures of greatest concern are alpha and gamma radiation emanating primarily from insoluble uranium compounds. Among monitored workers, the mean cumulative alpha radiation dose to the lung was 8.21 rem, and the mean cumulative external whole body penetrating dose from gamma radiation was 0.96 rem. Relative to US white males, the cohort experienced mortality deficits from all causes combined, cardiovascular diseases, and from most site-specific cancers. Mortality excesses of lung and brain and central nervous system cancers were seen from comparisons with national and state rates. Dose-response trends were detected for lung cancer mortality with respect to cumulative alpha and gamma radiation, with the most pronounced trend occurring for gamma radiation among workers who received greater than or equal to 5 rem of alpha radiation. These trends diminished in magnitude when a 10-year latency assumption was applied. Under a zero-year latency assumption, the rate ratio for lung cancer mortality associated with joint exposure of greater than or equal to 5 versus less than 1 rem of both types of radiation is 4.60 (95% confidence limits (CL) 0.91, 23.35), while the corresponding result, assuming a 10-year latency, is 3.05 (95% CL 0.37, 24.83). While these rate ratios, which are based on three and one death, respectively, lack statistical precision, the observed dose-response trends indicate potential carcinogenic effects to the lung of relatively low-dose radiation. There are no dose-response trends for mortality from brain and central nervous system cancers.

Adolescent↗
PubMed1999

Medical effects of internal contamination with uranium.

The purpose of this work is to present an outline of the metabolic pathways of uranium isotopes and compounds, medical consequences of uranium poisoning, and an evaluation of the therapeutic alternatives in uranium internal contamination. The chemical toxicity of uranium has been recognized for more than two centuries. Animal experiments and human studies are conclusive about metabolic adverse affects and nephro- toxicity of uranium compounds. Radiation toxicity of uranium isotopes has been recognized since the beginning of the nuclear era, with well documented evidence of reproductive and developmental toxicity, as well as mutagenic and carcinogenic consequences of uranium internal contamination. Natural uranium (238U), an alpha emitter with a half-life of 4.5x10(9) years, is one of the primordial substances of the universe. It is found in the earth's crust, combined with 235U and 234U, alpha, beta, and gamma emitters with respective half-lives of 7.1x10(8) and 2.5x10(5) years. A special emphasis of this paper concerns depleted uranium. The legacy of radioactive waste, environmental and health hazards in the nuclear industry, and, more recently, the military use of depleted uranium in the tactical battlefield necessitates further insight into the toxicology of depleted uranium. The present controversy over the radiological and chemical toxicity of depleted uranium used in the Gulf War warrants further experimental and clinical investigations of its effects on the biosphere and human organisms.

Animals↗