Radioactive series disequilibria in underground uranium deposits of the Singhbhum Shear Zone, Eastern India

Radionuclides of the ²³⁸U series (²²⁶Ra, ²¹⁰Pb, ²³⁴Th and ²³⁴U), ²³⁵U series (²²⁷Ac and ²³¹Pa) and ²³²Th series (²²⁸Th and ²²⁸Ra) series were measured by High Resolution Gamma Spectrometry system in twenty-five uranium ore samples from underground uranium deposits in the Singhbhum Shear Zone of Eastern India. The activity concentrations were observed to vary within a wide range in most of the deposits, as is the case in most rocks of crustal origin. The uranium ore from these deposits were not of high ore grade (U concentrations ranged from 0.015 to 0.082%). Activity ratios of key daughter–parent pairs from the decay chains, viz. ²²⁶Ra/²³⁸U, ²²⁶Ra/²¹⁰Pb, ²³¹Pa/²³⁵U, ²²⁷Ac/²³⁵U, ²³⁰Th/²³⁸U, ²³⁴U/²³⁸U, ²²⁶Ra/²³⁰Th and ²²⁸Th/²²⁸Ra indicated migration/accumulation of uranium and radium in some samples. The ²²⁶Ra/²³⁰Th ARs suggested that the deposits were not closed to groundwater movement for a maximum time period of 8ky. Thiel plot of the ²³⁴U/²³⁸U vs. ²³⁰Th/²³⁸U activity ratios indicated uranium accumulation and complex processes of uranium redistribution.     

Development of a sequential method for the determination of238U,234U,232Th,230Th,228Th,228Ra,226Ra,and210Pb. in environmental samples

A sequential analytical method for the determination of²³⁸U,²³⁴U,²³²Th,²³⁰Th,²²⁸Th,²²⁸Ra,²²⁶Ra and²¹⁰Pb in environmental samples was developed. Uranium and thorium isotopes are first chromatographically sepaaated using tri-n-octyl phosphine oxide (TOPO) supported on silica gel. The uranium isotopes are determined by alpha-spectrometry following extraction with TOPO onto a polymeric membrane. Thorium isotopes are co-precipitated with lanthanum fluoride before counting in an alpha spectrometer. Radium isotopes and²¹⁰Pb are separated by co-precipitation/precipitation with mixed barium/lead sulphate. Radium-226 is determined by gross alpha counting of the final BaSO₄ precipitate and²²⁸Ra by gross beta counting of the same source. Lead-210 is determined through beta counting of its daughter product²¹⁰Bi.     

Hokutolite collected from riverbed at Peitou Hot Spring in Taiwan: With emphasis on radiochemical studies

Summary Hokutolite, and hot spring water and river water collected recently at Peitou Hot Spring in Taiwan were analyzed for U, Th, Ra and ²¹⁰Pb isotopes. Concentrations of major chemical elements were also measured. Hokutolite had its typical chemical composition make-up for this area. The concentrations of ²³⁸U, ²³⁴U, ²³² Th, ²³⁰ Th, ²²⁸ Th, ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb in samples scrapped into 7 layers from the surface to the bottom of a hokutolite specimen were 0.0021-0.0068, 0.0022-0.0075, 1.47-2.07, 1.00-1.29, 1.56-1.97, 56.7-68.6, 1.46-2.06 and 25.9-36.0 Bq/g, respectively. All the radionuclides exhibited a relatively uniform distribution, and radioequilibrium was confirmed among ²³² Th, ²²⁸Ra and ²²⁸ Th. From the relationship between the decay and growth of Th-series nuclides it was considered that the hokutolite studied was isolated from the stream water at least 70-80 years ago. The U/Th-series radionuclides in the hot spring water were in rather high concentrations and the enrichment of ²²⁸Ra and ²²⁸ Th to ²³² Th was the most prominent feature. Evaluation of the distribution coefficients (K_d) using the data on hot spring water or river water and hokutolite indicated that Th (K_d = 10⁴-10⁵) in water was likely to be precipitated (and/or co-precipitated) with BaSO₄ as Th(SO₄)₂ with a relatively high concentration into hokutolite, together with Ra (K_d = 10⁶-10⁷).     

Natural radioactivity in bioassay by alpha-spectrometry measurements

Personnel of nuclear facilities are checked regularly for internal contamination by bioassay measurements. Although these persons are generally not involved in any incident, natural radioactivity from U, Th and Ra can be found in their urine or faeces. Uranium total activity in urine has been found with a range of 0.051 to 3.0 mBq/24 h and in faeces from 14.5 to 380 mBq/d. ²³⁴U/²³⁸U ratio for urine is 1.48 but this ratio varies from 0.47 to 19. By comparison, the ²³⁴U/²³⁸U ratio found in urine from workers in volved with natural uranium or 4.5% enriched uranium is 1.0 and around 4.0 respectively. ²³⁰Th, ²²⁸Th and sometimes ²³²Th have also been detected. The total thorium activity varies from 0.137 to 5.6 mBq/24 h in urine and from 9 to 183 mBq/d in faeces. ²²⁸Th has generally been found in excess of ²³²Th. All these measurements were performed by alpha-spectrometry. The few ²²⁶Ra results have been measured using the Lucas or emanation method.     

Geochemical record of U and Th isotopes in bottom sediments of Lake Kawaguchi at the foot of Mt. Fuji, Central Japan

Sediment cores from Lake Kawaguchi at the foot of Mt. Fuji in Japan were analyzed for U and Th isotopes (²³⁸U, ²³⁴U, ²³²Th, ²³⁰Th and ²²⁸Th) in the light of the linkage to paleoenvironmental changes. These isotopic concentrations and their ratios varied widely with depth of sediment core. A marked disequilibrium (1.1–1.5) higher than the value of 1.0 was observed for ²³⁴U/²³⁸U activity ratios, indicating that U from lake water with high ²³⁴U/²³⁸U ratio (ca. 1.6) was transferred to the bottom sediment by adsorption and/or adhesion onto the settling particles. By using model equations, the U found in the sediment core was separated into lithogenous and autogenous U fractions. These depth profiles were compared with parameters such as organic matter and biogenic-SiO₂ contents and amount of rainfall. Some variations of selected parameters with depth coincided with those of lithogenous or autogenous U. The results obtained suggest that variation in the lithogenous and/or autogenous U in the sediment with depth might be helpful in tracing the geochemical behavior of U and the past environmental changes in the area surrounding Lake Kawaguchi.The authors would like to express their gratitude to Dr. Y. Ohtsuka of Department of Radioecology, Institute for Environmental Sciences and Dr. K. Sasaki of Department of Cultural Properties and Heritage, Kanazawa Gakuin University for sampling of water and rock samples at Lake Kawaguchi.     

Geochemical record of U and Th isotopes in bottom sediments of Lake Kawaguchi at the foot of Mt. Fuji, Central Japan

Sediment cores from Lake Kawaguchi at the foot of Mt. Fuji in Japan were analyzed for U and Th isotopes (²³⁸U, ²³⁴U, ²³²Th, ²³⁰Th and ²²⁸Th) in the light of the linkage to paleoenvironmental changes. These isotopic concentrations and their ratios varied widely with depth of sediment core. A marked disequilibrium (1.1–1.5) higher than the value of 1.0 was observed for ²³⁴U/²³⁸U activity ratios, indicating that U from lake water with high ²³⁴U/²³⁸U ratio (ca. 1.6) was transferred to the bottom sediment by adsorption and/or adhesion onto the settling particles. By using model equations, the U found in the sediment core was separated into lithogenous and autogenous U fractions. These depth profiles were compared with parameters such as organic matter and biogenic-SiO₂ contents and amount of rainfall. Some variations of selected parameters with depth coincided with those of lithogenous or autogenous U. The results obtained suggest that variation in the lithogenous and/or autogenous U in the sediment with depth might be helpful in tracing the geochemical behavior of U and the past environmental changes in the area surrounding Lake Kawaguchi.The authors would like to express their gratitude to Dr. Y. Ohtsuka of Department of Radioecology, Institute for Environmental Sciences and Dr. K. Sasaki of Department of Cultural Properties and Heritage, Kanazawa Gakuin University for sampling of water and rock samples at Lake Kawaguchi.     

The natural radioactivity of Brazilian phosphogypsum

Phosphogypsum is a high volume by-product from the phosphoric acidindustries containing naturally occurring radionuclides. Envisaging the usesof phosphogypsum, a characterization of this material in terms of spatialdistribution of radionuclides was carried out by core samples taken from stacksof two important Brazilian phosphoric acid facilities. Samples were analyzedfor ²³⁸U, ²³⁴U, ²³²Th, ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb and ²¹⁰Po using alpha- and gamma-spectrometryand UV-VIS spectrophotometry. Specific activities of ²³⁸U, ²³⁴U, ²²⁶ Ra and ²¹⁰Po obtained were comparablewith data reported in the phosphogypsum literature, while higher values werefound for ²³² Th and ²²⁸Ra.     

Radiochemical determination of uranium and radium isotope in natural water using liquid scintillation counter

²³⁴U, ²³⁸U, ²²⁶Ra, and ²²⁸Ra were analyzed in 14 Korean hot spring waters. Uranium was extracted with mixture of extractive scintillation cocktail containing HDEHP and ²³⁴U, ²³⁸U were analyzed with LSC. Radium isotopes were separated using Ba coprecipitation method and counted with LSC and ²²⁸Ra was also analyzed its daughter ²²⁸Ac with HPGe γ-detector. Among them ²²⁶Ra was ranged <0.01–0.155 Bq/L and ²²⁸Ra is below detection limit <0.1 Bq/L. And also, uranium content was ranged <0.01–49.7 μg/L and ²³⁴U/²³⁸U ratio was ranged 0.69–1.17.     

Fractionation of thorium and uranium isotopes in the acid leaching experiments on monazite

A series of leaching experiments with water and gradually harsher acid solutions have been carried out on a monazite.²²⁸Th/²³²Th,²³⁰Th/²³²Th, and²³⁴U/²³⁸U activity ratios in the acid fractions show a common variation pattern: high — low — close to bulk values, which can be explained in terms of preferential solution effect of recoil atoms. Compared with²²⁸Th, the preferential solution effect of²³⁴U is suppressed due to self-annealing of recoil tracks.     

Behavior of uranium and thorium isotopes in soils of the Boréon area, Mercantour Massif (S.E. France): Leaching and weathering rate modeling

Four cores were collected in weathered rocks and soils in the Boréon forest area (1765 m, Mercantour Massif, France). The samples were analyzed for the isotopes ²³⁰Th, ²³²Th, ²³⁴U and ²³⁸U. The activity and isotopic ratio profiles suggest that uranium was mobilized (leaching and precipitation) during the weathering process, as well as thorium but in a much less proportion. A model was drawn up to evaluate the U leaching rate and the time that some levels of the weathered rocks have been subjected to weathering. It utilizes LATHAM and SCHWARCZ’s two equations,¹⁵ expressed as ²³⁴U/²³⁸U and ²³⁰Th/²³⁸U activity ratios, which assume that the alpha recoil effect allows easier leaching for ²³⁴U than ²³⁸U and no Th mobility. But this last assumption does not correspond to the observations made in the Boréon area, since it appears that in some soil deeper layers ²³⁰Th and ²²⁸Th are in radioactive deficit relatively to their parents. As there are four unknown quantities (the time, the leaching rates of ²³⁸U, ²³⁴U, ²³⁰Th), the problem to be solved requires two more equations; these can be obtained utilizing the U activity ratio in water, and taking into account the ²³²Th behavior. In some sites the ²³⁸U leaching rate is high in deeper soil levels (near the fresh rocks); this would correspond to a loss of half the U amount in less than 24 000 years.     

Natural radionuclides in groundwaters

The²³⁴U and²³⁰Th radionuclides are highly retarded by factors of 10⁴ to 10⁵ in basalt groundwater (Hanford) and briny groundwaters from Texas, and geothermal brine from the Salton Sea Geothermal Field (SSGF). In basalt groundwaters (low ionic strength), Ra is highly sorbed, while in brines (high ionic strength), Ra is soluble. This is probably because the sorption sites are saturated with Na⁺ and Cl^– ions, and RaCl₂ is soluble in brines.²¹⁰Pb is soluble in SSGF brine, probably as a chloride complex. The²³⁴U/²³⁰Th ratios in basalt groundwaters and brines from Texas and SSGF are nearly unity, indicating that U is in the +4 state, suggesting a reducing environment for these aquifers.     

Intercalibrated radionuclide activities in spiked water samples of the IAEA worldwide open proficiency test

Proficiency testing is one of methods for regularly assessing the accuracy of the analytical data produced by laboratories for particular measurements. In 2008 and 2010, we participated in the IAEA 2008 and 2010 worldwide open proficiency tests on the determination of natural radionuclides in water spiked with ²²⁶Ra, ²³⁴U and ²³⁸U for activity analysis and with ⁹⁰Sr and ²³⁰Th for gross alpha/beta analysis. Feedback statistics from the IAEA final report showed that the radioactivities of all of the samples fell within an acceptable range according to the IAEA. For ²²⁶Ra analysis, our result showed that ²²⁹Th–²²⁵Ra is suitable as a chemical tracer, although there are doubts that different co-precipitation efficient between parent ²²⁹Th and its daughter nuclide ²²⁵Ra in published literature. The impact factors of the analysis results, such as the lower limit of detection, standard substances, the background and efficiency for daily determination, are discussed in detail.     

The dietary intake of238U,234U,230Th,232Th,228Th and226Ra from food and drinking water by inhabitants of the Walbrzych region

Intake with food and water of the natural radionuclides of the uranium and thorium series was determined for adult population of the south-western region in Poland, where in the 1950-ies an exploration of uranium ore was conducted. Concentration of the radionuclides was determined in food products and drinking water and their annual intake was estimated on the basis of the average annual consumption. The intake of²³⁸U,²³⁴U and²³⁰Th occurred mainly with water (33% to 68%), whereas the intake of²³²Th,²²⁸Th and²²⁶Ra was mainly with vegetables, potatoes, milk and flour. From the intake and dose coefficients the annual effective doses from the ingested radionuclides were calculated. The total dose was 5.6 Sv, of which 74% originated from²²⁶Ra.     

Determination of uranium and thorium isotopes in mineral spring waters

Concentrations levels of uranium and thorium isotopes have been analyzed in the m mineral spring waters of a high background region of Brazil: Poços de Caldas and Águas da Prata. The procedure was based on the determination of²³⁸U,²³⁴U,²³²Th,²³⁰Th and²²⁸Th by -spectrometry after separation and purification of the isotopes of interest by using anion-exchange chromatography and preparation of the samples for -measurements by electrodeposition. The concentration varied from <1.1 to 28.4 mBq.l^–1 and from <1.6 to 141 mBq.l^–1 for²³⁸U and²³⁴U, respectively. Thorium isotope measurements varied from <0.2 to 1.8 mBq.l^–1 from <0.3 to 4.9 mBq.l^–1 and from <0.8 to 19.9 mBq.l^–1 for²³²Th,²³⁰Th and²²⁸Th, respectively. Calculations of thorium and uranium isotopic activity ratios were carried out giving values ranging from 1.9 to 7.2, from 1.2 to 3.0 and from 7.7 to 15.3 for²³⁴U/²³⁸U,²³⁰Th/²³²Th and²²⁸Th/²³²Th, respectively. The effective doses due to the intake of²³⁸U and²³⁴U present in these waters are expected to reach values up to 1.4×10^–3 mSv y^–1 and 8.0×10^–3 mSv y^–1, respectively.     

A device for uranium series leaching from glass fiber in HEPA filter

For the disposal of a high efficiency particulate air (HEPA) glass filter into the environment, the glass fiber should be leached to lower its radioactive concentration to the clearance level. To derive an optimum method for the removal of uranium series from a HEPA glass fiber, five methods were applied in this study. That is, chemical leaching by a 4.0?M HNO₃?C0.1?M Ce(IV) solution, chemical leaching by a 5 wt% NaOH solution, chemical leaching by a 0.5?M H₂O₂?C1.0?M Na₂CO₃ solution, chemical consecutive chemical leaching by a 4.0?M HNO₃ solution, and repeated chemical leaching by a 4.0?M HNO₃ solution were used to remove the uranium series. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 5?h by the 4.0?M HNO₃?C0.1?M Ce(IV) solution were 2.1, 0.3, 1.1, and 1.2?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 36?h by 4.0?M HNO₃?C0.1?M Ce(IV) solution were 76.9, 3.4, 63.7, and 71.9?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after leaching for 8?h by a 0.5?M H₂O₂?C1.0?M Na₂CO₃ solution were 8.9, 0.0, 1.91, and 6.4?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after consecutive leaching for 8?h by the 4.0?M HNO₃ solution were 2.08, 0.12, 1.55, and 2.0?Bq/g. The residual radioactivity concentrations of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th in glass after three repetitions of leaching for 3?h by the 4.0?M HNO₃ solution were 0.02, 0.02, 0.29, and 0.26?Bq/g. Meanwhile, the removal efficiencies of ²³⁸U, ²³⁵U, ²²⁶Ra, and ²³⁴Th from the waste solution after its precipitation?Cfiltration treatment with NaOH and alum for reuse of the 4.0?M HNO₃ waste solution were 100, 100, 93.3, and 100%.     

A new reference material for radionuclides in the mussel sample from the Mediterranean Sea (IAEA-437)

A new Reference Material (RM) for radionuclides in mussel (Mytilus galloprovincialis) from the Mediterranean Sea (IAEA-437) is described and the results of the certification process are presented. Four radionuclides (⁴⁰K, ²³⁴U, ²³⁸U, and ^239+240Pu) have been certified, and information values on massic activities with 95% confidence intervals are given for nine radionuclides (¹³⁷Cs, ²¹⁰Pb(²¹⁰Po), ²²⁶Ra, ²²⁸Ra, ²²⁸Th, ²³⁰Th, ²³²Th, ²³⁵U, and ²⁴¹Am). Results for less frequently reported radionuclides (⁹⁰Sr, ¹²⁹I, ²³⁸Pu, ²³⁹Pu, and ²⁴⁰Pu) are also reported. The RM can be used for quality assurance/quality control of the analysis of radionuclides in mussel samples, for the development and validation of analytical methods and for training purposes. The material is available in 200 g units.     

Radiological characterization and environmental impact in northwestern coast of Egypt

A study of environmental radioactivity along the northwestern coast of Egypt was performed by the Central Laboratory for Environmental Radioactivity Measurements Inter-comparison and Training within the framework of the research project: Radiological Studies/Measurements of Natural and Man-made Radionuclides in the Environment. The present paper contains important conclusions, correlations and interpretations of the environmental measurements. The samples collection and measurements were conducted according to the Egyptian Atomic Energy Authority monitoring plan for locations along the northwestern coast of Egypt and its main tributaries of interest. The specific activities of ²²⁶Ra (²³⁸U series), ²²⁸Ra (²³²Th series), ⁴⁰K and ¹³⁷Cs (Bq/kg dry weight) were measured using gamma-ray spectrometers based on hyper-pure germanium detectors. The absorbed radiation dose rates in air (nGy/h) due to natural radionuclides in shore sediment and radium equivalent activity index (Bq/kg) were calculated. The specific activity ratios of ²²⁸Ra/²²⁶Ra were calculated for evaluation of the geo-chemical behavior of these radionuclides. Samples textures and CaCO₃ and total organic matter contents of sediments were also determined while the pH, major cations and anions such as Na⁺, K⁺, Ca⁺⁺, Mg⁺⁺and Cl^?, SO₄ ^– and HCO₃, respectively were also determined in water samples.     

Radium,uranium and thorium concentrations in low specific activity scales and in waters of some oil and gas production plants

Low specific activity scales consisting of alkaline earth metal carbonates and sulfates are often present in some gaseous and liquid hydrocarbon plants; these scales contain a certain concentration of radium, uranium and thorium, which can cause a risk of -irradiation and of internal radiocontamination when they must be mechanically removed. That being stated,²³⁸U,²³²Th and²²⁶Ra were determined in scales, sludges and waters coming from different plants.²³⁸U and²³²Th concentrations were found very low; the isotopes²³⁸U and²³⁴U resulted in radioactive equilibrium, whilst²³²Th and²²⁸Th were not always in equilibrium.²²⁶Ra concentration was higher in scales and sludges than in waters.     

Uranium age-dating using in-situ isotope ratios by thermal ionization mass spectrometry for nuclear forensics

The model dates of two enriched uranium materials were determined using a new method for nuclear forensics investigation. In this method, without spike addition, the ²³⁰Th/²³⁴U ratio was calculated from the measured ratios of ²³⁰Th/²³⁴Th and ²³⁴U/²³⁸U and from calculated ²³⁴Th/²³⁸U ratio in secular equilibrium. The model date obtained for the low-enriched uranium material was in agreement with the known production date. For the highly enriched uranium material, a more recent model date than the known production date was obtained. The ²³⁴U interference on ²³⁴Th counting in thermal ionization mass spectrometer measurement was suspected as a potential cause.

     

Factors Controlling Natural Radionuclides Migration in Sedimentary Rock Samples,Gabal Um‐Hamd,Southwestern Sinai,Egypt

The activity concentrations of some radionuclides (²³⁸U, ²³⁴U, ²³⁰Th, ²²⁶Ra, ²³²Th, ⁴⁰K and ²³⁵U) were measured by γ‐ray spectrometry in order to study their behavior and the relation between them in Carboniferous rock samples collected from Gabal (mountain) Um‐Hamd, southwestern Sinai, Egypt. The whole samples are located in the two limbs and trough of a synclinal form structure to identify the radionuclides migration processes which have occurred in these rock samples. The average activity concentrations of ²³⁸U, ²³²Th, ²²⁶Ra, and ⁴⁰K measured in the all samples except sandy dolostone sample are higher than the worldwide average values as reported by UNSCEAR 2008. The activity ratios (²³⁴U/²³⁸U) for half of the samples are in equilibrium, while the other half samples are below unity indicates migration‐out of uranium. The hazard indices were also calculated. The variations in lithologic types and the configuration of the structural synform played its roles beside the physical and chemical properties of different radionuclides in their fractionations.