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Uranium and thorium in urine of United States residents: reference range concentrations.

We measured uranium and thorium in urine of 500 U. S. residents to establish reference range concentrations using a magnetic-sector inductively coupled argon plasma mass spectrometer (ICP-MS). We found uranium at detectable concentrations in 96.6% of the urine specimens and thorium in 39.6% of the specimens. The 95th percentile concenetration for uranium was 34.5 ng/L (parts per trillion); concentrations ranged up to 4080 ng/L. Thorium had a 95th percentile concentration of 3.09 ng/L; concentrations ranged up to 7.7 ng/L.

Body Burden↗

The analysis of naturally-occurring radionuclides from uranium and thorium decay series in table mineral waters.

This project required the highly sensitive analysis of low-level alpha- and beta-emitters naturally occurring in table mineral water sold on the Swiss market. These radionuclides occur in the three major decay series-uranium-238, uranium-235, and thorium-232. The radionuclides analysed were 238U, 235U, 234U, 232Th, 230Th, 228Th, 210Po, 210Pb, and 226Ra. Many other radionuclides were determinable as a result of their equilibrium with an analysed nuclide. Efficient, element specific separation techniques were developed, allowing for the spectral analysis of each element without interference from other radioactive elements. Radioactive tracers, 232U, 230Th, and 209Po, were necessary to determine the percentage yield. These yields often varied greatly between different mineral waters, especially for thorium, ranging from 30 to 100%. Uranium, thorium and polonium isotopes could be directly analysed for by alpha-spectrometry. 226Ra was determined through the ingrowth of its daughter 222Rn by liquid scintillation counting. From the samples remaining after 210Po removal, the isotope's re-ingrowth from 210Pb determined the original 210Pb content. Limits of detection ranged from 0.1 to 2.0 mBq/l. The following contents were determined 234U + 238U 30-720 mBq/l; 232Th + 230Th < 1-5 mBq/l; 228Th 2-40 mBq/l; 226Ra 5-370 mBq/l; 210Po 1-90 mBq/l; 2,0Pb 1-90 mBq/l.

Mineral Waters↗

Application of extraction chromatography to the separation of thorium and uranium dissolved in a solution of high salt concentration.

Extraction chromatography with commercially available UTEVA resin (for uranium and tetravalent actinide) was applied for the separation of Th and U from control solutions prepared from a multi-element control solution and from sample solutions of solidified simulated waste. Thorium and U in control solutions with 1-5mol/dm(3) HNO(3) were extracted with UTEVA resin and recovered with a solution containing 0.1mol/dm(3) HNO(3) and 0.05mol/dm(3) oxalic acid to be separated from the other metallic elements. Extraction behavior of U in the sample solutions was similar to that in the control solutions, but extraction of Th was dependent on the concentration of HNO(3). Thorium was extracted from 5mol/dm(3) HNO(3) sample solutions but not from 1mol/dm(3) HNO(3) sample solutions. We conjecture that thorium fluoride formation interferes with extraction of Th. Addition of Al(NO(3))(3) and Fe(NO(3))(3), which have higher stability constant with fluoride ion than Th, does improve extractability of Th from 1mol/dm(3) HNO(3) sample solution.

Aluminum Compounds↗

Determination of thorium, uranium and potassium elemental concentrations in surface soils in Cyprus.

A comprehensive study was conducted to determine thorium, uranium and potassium elemental concentrations in surface soils throughout the accessible area of Cyprus using high-resolution gamma-ray spectrometry. A total of 115 soil samples was collected from all over the bedrock surface of the island based on the different lithological units of the study area. The soil samples were air-dried, sieved through a fine mesh, sealed in 1000-ml plastic Marinelli beakers, and measured in the laboratory in terms of their gamma radioactivity for a counting time of 18 h each. From the measured gamma-ray spectra, elemental concentrations were determined for thorium (range from 2.5 x 10(-3) to 9.8 microg g(-1)), uranium (from 8.1 x 10(-4) to 3.2 microg g(-1)) and potassium (from 1.3 x 10(-4) to 1.9%). The arithmetic mean values (A.M. +/- S.D.) calculated from all samples are: (1.2+/-1.7 microg g(-1)), (0.6+/-0.7) microg g(-1), and (0.4+/-0.3%), for thorium, uranium and potassium, respectively, which are by a factor of three-six lower than the world average values of 7.4 microg g(-1) (Th), 2.8 microg g(-1) (U) and 1.3% (K) derived from all data available worldwide. The best-fitting relation between the concentrations of Th and K versus U and also of K versus Th, is essentially of linear type with a correlation coefficient of 0.93, 0.84 and 0.90, respectively. The Th/U, K/U and K/Th ratios (slopes) extracted are equal to 2.0, 2.8 x 10(3) and 1.4 x 10(3), respectively.

Cyprus↗

Determination of thorium in environmental and workplace materials by ICP-MS.

The paper outlines the advantages of the use of Inductively Coupled Plasma Mass Spectrometry (ICP-MS) over radiometric techniques to measure natural thorium, 232Th. Experimental parameters that must be taken into account in the sample digestion, preparation and ICP-MS analysis of environmental (soils, rocks, sediments) or workplace (thorium oxide, reference solutions) materials are described. The methods presented are applied to various reference materials, with the aim of providing suitable procedures to be useful for other important thorium containing materials (such as monazite sands or welding electrodes). The participation in a European Commission intercomparison exercise is detailed and a comparison with alpha spectrometry is made.

Environmental Exposure↗

Thorium in the workplace measurement intercomparison.

The monitoring of radionuclides in the nuclear industry has been recognized as the most straightforward way of assessing health and safety issues associated with the exposure of the workforce to potentially harmful radiation doses. Much of this is achieved by measurements in the workplace itself and by the bioassay and monitoring of workers in the industry. However, there also exists a significant 'non-nuclear' industry where workers are exposed to radioactive materials, for example where this involves thorium, which is made wide use of in the aerospace and other high technology industries. As such work involves the processing of thorium bearing materials, the workforce is potentially exposed to 232Th and its daughter nuclides. Thus, to monitor the workforce effectively, it is important to be able to measure both 232Th and the decay products of 232Th where they are in an unknown state of radioactive equilibrium and this is where monitoring laboratories may experience some difficulty. Accordingly, the Health and Safety Laboratory in the UK has organized a EC wide project on the monitoring of thorium in the 'non-nuclear' workplace; this project is currently ongoing. We report the results of the first intercomparison of this project involving two solutions of 232Th, one in radioactive equilibrium and one not in equilibrium with its daughters. The results are presented with some comments on how this intercomparison has progressed and how these first results will inform the rest of the project.

Evaluation Studies as Topic↗

Effect of thorium on the growth and capsule morphology of Bradyrhizobium.

The thorium effect on Bradyrhizobium growth was assayed in liquid media. Th4+ inhibited the growth of Bradyrhizobium (Chamaecytisus) BGA-1, but this effect decreased in the presence of suspensions of live or dead bacterial cells. Th4+ induced the formation of a gel-like precipitate when added to a dense suspension of B. (Chamaecytisus) BGA-1 cells. Viable Bradyrhizobium cells remained in suspension after precipitate formation. Thorium was recovered in the precipitate, in which polysaccharide, lipopolysaccharide and proteins were also found. After Th4+ addition, the morphology of B. (Chamaecytisus) BGA-1 or Bradyrhizobium japonicum USDA 110 sedimented cells studied by scanning electron microscopy changed from an entangled network of capsulated bacteria to uncapsulated individual cells and an amorphous precipitate. Energy-dispersive X-ray spectroscopy showed that thorium was mainly in the amorphous fraction. Precipitate was also formed between B. (Chamaecytisus) BGA-1 and Al3+, which was also toxic to this bacterium. Precipitate induced by Th4+ or Al3+ was found in all Bradyrhizobium and Sinorhizobium strains tested, but not in Rhizobium, Salmonella typhimurium, Aerobacter aerogenes or Escherichia coli. These results suggest a specific defence mechanism based on metal precipitation by extracellular polymers.

Aluminum↗

[Hepatocellular carcinoma following intravenous thorium X therapy].

Twelve years after receiving radiation therapy with thorium X (280 microCi) for long-standing Bechterew's disease (ankylosing spondylitis) a 52-year-old man was found, by ultrasonography and computed tomography, to have a round mass, 11 x 12 cm, in the left lobe of the liver. Laparoscopy discovered coarse, discoloured nodes on the surface of the right and left lobes of the liver which histologically showed hepatocellular carcinoma. There were no known risk factor for liver carcinoma (like cirrhosis, positive hepatitis B serology, alcohol abuse, haemochromatosis or alpha 1-antitrypsin deficiency). As exploratory laparotomy found the tumour to be inoperable, 15 chemotherapeutic embolizations were performed. An abdominal wall metastasis was resected after 17 months. At the time of this report, 20 months after the diagnosis was first made, the patient is in a poor general condition. Internal radiotherapy with thorium X was used, all else having failed, in the treatment of severe ankylosing spondylitis. Although it is not possible to prove a direct causal relationship between the thorium X radiation and development of a liver carcinoma, the coincidence is remarkable.

Carcinoma, Hepatocellular↗

Assessment of airborne hazards in the thorium processing industry.

Airborne thorium thoron and its decay products contribute significantly to the hazards in the thorium industry. These have been assessed and compared with the standards. Assessment also included the unattached fractions of the decay products, the thoron working levels and the aerodynamic particle size distribution of airborne thorium.

Air Pollutants↗

Thorium in mineral products.

Many ores contain low levels of thorium. When these ores are processed, the associated radioactivity can be found in mineral concentrates, intermediates and final products. There is an incentive for industries to remove radioactivity from mineral products to allow the movement and sale of these materials, both nationally and internationally, without the need for licensing. Control of thorium in various products involves the development and optimisation of process steps to be able to meet product specifications. The Australian Nuclear Science and Technology Organisation (ANSTO) has undertaken a range of R & D programmes targeting the treatment of thorium-bearing minerals. This paper discusses the application of a microprobe technique for siting radioactivity in zircon and ilmenite and the problems experienced in measuring the concentrations in solid rare earth products.

Minerals↗

Thorium determination in intercomparison samples and in some Romanian building materials by gamma ray spectrometry.

Thorium content in zircon sand, thorium ore and a thorium liquid sample (EU Laboratories Network Intercomparison), as well as in some Romanian building materials: sand, wood, tufa, asbestos-cement. cement mill dust, coal fly ash, bricks, and tile (28 samples) was deterimined by gamma ray spectrometry. For the building materials, 226Ra, 40K and 137Cs specific activities were also measured. The results were compared with the Romanian legal norms concerning the highest admissible levels for 232Th, 226Ra. and 40K radioactivity. and to Th, U, and K concentration values previously determined in our laboratory on similar types of samples.

Construction Materials↗

Analytical methods for thorium determination: a journey from conventional methods to novel applications.

Thorium may be determined using a variety of analytical methods. These may be based on chemical or physical principles or may make use of the radioactive decay of the individual thorium isotopes. The method to be used for a certain analytical purpose is selected as a function of the matrix of the sample and of the concentration of thorium. The present paper describes different methodologies, their range of application and discusses selected results. The methods described cover a concentration range of more than twelve orders of magnitude, i.e. from concentrated solutions to micrometre-sized particles. Emphasis is given to active radiometric techniques, chemical and instrumental analysis.

Mass Spectrometry↗

Long term health effects of thorium compounds on exposed workers: the complete blood count.

Two hundred seventy-three men exposed to thorium and other rare earths between 1940 and 1973 at a plant which refined monazite sand were studied at Argonne National Laboratory from 1976 to 1980. In vivo measurements of body burden were made by counting gamma rays emitted by daughter products of retained thorium and by measuring exhaled thoron. Health status was ascertained through questionnaire, physical examination, and clinical laboratory tests. Measured body burden was found to be higher in those with a history of longer exposure. All parameters of the complete blood count were examined for evidence of an effect due to thorium. Comparisons of high and low body burden groups showed that only age and cigarette smoking had an effect on complete blood count parameters.

Adult↗

Chromosome damage in peripheral lymphocytes from American thorium workers.

An analysis of the frequency of chromosome aberrations in lymphocytes from 47 thorium workers and three external controls is presented. Thirty-seven of these cases were divided into three age-matched groups based upon the means of the sums of their emanating radium-224 and bismuth-212 (Ra + Bi) burdens. The low burden group (mean Ra + Bi burden = -0.06 +/- 0.03 nCi) had two two-break chromosome aberrations in 1200 cells, the moderate burden group (mean Ra + Bi burden = 0.21 +/- 0.03 nCi) had three such aberrations in 1000 cells and the high burden group (mean Ra + Bi burden = 0.99 +/- 0.21 nCi) had five such aberrations in 1500 cells. While there is a two-fold increase in the two-break aberration frequency in pooled data from the two higher exposure groups (8/2500 cells) as compared with the lowest exposure group (2/1200 cells), the difference between these subsamples is not statistically significant (p = 0.32). The frequency of dicentrics and centric ring chromosomes (8/3300 cells) in the pooled higher body burden groups from the total sample (mean Ra + Bi burden = 0.56 +/- 0.09 nCi) does however show a very highly significant increase over the historical control frequency. A similar analysis based on total months of employment in the thorium-processing industry did not show a positive relationship between duration of employment and aberration frequency. In broad outline, our results are compatible with those from similar studies on Brazilian thorium workers and Thorotrast patients.

Adult↗

Plutonium concentration in human tissues: comparison to thorium.

The concentration of 238Pu, and 239,240Pu, and of 228Th, 230Th, and 232Th were measured in 10 sets of human tissues from Washington, DC, and 12 sets from Grand Junction, CO. The tissues were collected at autopsy by qualified pathologists from normal healthy persons most of whom died suddenly. The subjects had acquired plutonium from fallout of global nuclear testing and burnup of a space nuclear generator utilizing 238Pu. The median concentration of 239,240Pu was 0.08 pCi/kg in lung, 0.46 pCi/kg in tracheobronchial lymph nodes, 0.60 pCi/kg in liver, 0.02 pCi/kg in kidney and 0.17 pCi/kg in bone in Washington, DC subjects. Similarly, the concentration of 239,240Pu in Grand Junction subjects was found to be 0.17 pCi/kg in lung, 0.68 pCi/kg in lymph nodes, 0.55 pCi/kg in liver, 0.03 pCi/kg in kidney, 0.22 pCi/kg in bone and 0.08 pCi/kg in spleen. The median concentration in four gonads was 0.02 pCi/kg; the concentration in one thyroid was 0.01 pCi/kg. 238Pu was below the limit of detection in most organs except the liver where it ranged from 0.02 to 0.17 pCi/kg with a median concentration of 0.06 pCi/kg. The organ distribution pattern shows that most of the plutonium was accumulated in bone and liver with 54-60% in bone and 34-43% in liver. Only 3-6% was found in lung including lymph nodes; kidney, spleen, thyroid and gonads together contained around 1%. The analytical results show three major differences between plutonium and thorium concentrations and organ distributions: (1) for plutonium the liver is a major locus for storage (approximately 40% of that found in the total body), whereas little thorium is accumulated in the liver (around 4%); (2) the relative amounts of 230Th and 232Th are much higher in lung and lymph nodes (10-28%) than currently for plutonium (3-6%); (3) the ratio of throium concentrations in lymph nodes to lung is significantly higher than the ratio of plutonium concentration in lymph nodes to lung showing thereby that fallout plutonium is more soluble than natural thorium.

Body Burden↗

Evaluation of in vitro dissolution rates of thorium in uranium mill tailings.

Dissolution rates of thorium from the uranium mill tailings piles at two Department of Energy Uranium Mill Tailings Remedial Action Project (UMTRAP) sites have been evaluated. The thorium dissolution rates were evaluated in vitro using simulated lung fluid. The former uranium mills at the UMTRAP sites employed different chemical processes (acid leach and alkaline pressure leach) to extract the uranium from the ore, and the thorium dissolution rates at these sites were found to be markedly different. A site specific annual limit on intake (ALI) value for 230Th was calculated for the UMTRAP site that was associated with a multiple component dissolution curve.

Extracellular Space↗

Contents of cesium, iodine, strontium, thorium, and uranium in selected human organs of adult asian population.

Contents of cesium, iodine, strontium, thorium, and uranium in some selected human organs were estimated for adult Asian population using data obtained in four Asian countries: China, India, Philippines, and Republic of Korea, as part of a Coordinated Research Program of the International Atomic Energy Agency on "Ingestion and Organ contents of elements of importance in radiation protection." These countries together represent more than 40% of the world population. Highly sensitive analytical techniques were employed to measure cesium in skeletal muscle, iodine in thyroid, strontium in skeleton, thorium and uranium in skeleton, liver, kidneys, and lungs where, in comparison to other organs, these elements are present in higher concentrations. The organ contents for adult Asian population, when compared with the corresponding data proposed for Reference Man by International Commission on Radiological Protection (ICRP), showed about 40 times lower kidneys content and about 10 times lower skeleton content of uranium. The content of thorium in skeleton for Asian population was also half of the ICRP Reference Man value. Interestingly, organ contents for the other elements such as iodine in thyroid, cesium in skeletal muscle, and strontium in skeleton were comparable for Asian and the Caucasian population (represented by ICRP Reference Man). Organ contents for these elements were also calculated by applying the new ICRP models of these elements to their daily intakes. The comparison of the calculated and measured organ contents showed that despite uncertainties in the organ content values arising due to the inter-country variations in daily dietary intakes, the contents were within a factor of two to three. This observation is significant since human data both on organ contents and ingestion were obtained at environmental level of intakes. The study suggests that currently available ICRP models for these elements are quite realistic.

Adult↗

Age dependence of natural uranium and thorium concentrations in bone.

The age dependence of the natural concentration of uranium and thorium in the skeleton was investigated using human vertebrae bone collected from two Canadian locations (Winnipeg, Manitoba, and Regina, Saskatchewan). The concentration of both radioelements in digested ashed bone samples was determined using sector-field inductively coupled plasma mass spectrometry. The geometric means for uranium level in bones showed a significant statistical difference between the two locations studied. Similarly for thorium, a statistical difference was observed, although this difference was considered marginal. The thorium concentration differed only marginally with respect to age group, indicating that its behavior in the body could be age-independent. Conversely, the uranium level in bones was found to change for the age groups tested, an indication of age-specific deposition. The age profile for uranium was comparable to the calcium turn-over rate, indicating that uranium deposition is probably, in part, dictated by this metabolic process, showing the role of present uptake into the uranium concentration in bones for populations exposed to significant uranium intake.

Aging↗