Radiochemical characterization of spring waters in Balaton Upland, Hungary, estimation of radiation dose to members of public

Hungary is rich in spring waters. A survey studying the naturally occurring alpha emitter radionuclides in 30 frequently visited and regularly consumed spring waters was conducted out in the Balaton Upland region of Hungary.²²⁶Ra, ²²⁴Ra, ²³⁴U, ²³⁸U and ²¹⁰Po activity concentrations were determined by using alpha spectrometry after separation from matrix elements. Average concentration (mBq L^{− 1}) of ²²⁶Ra, ²²⁴Ra, ²³⁴U, ²³⁸U and ²¹⁰Po in the spring waters is varied from 2.1 to 601, from < 1.1 to 65.4, from 3.9 to 741.9, from < 0.44 to 274.3 and from 2 to 15.2 respectively. In most cases radioactive disequilibrium was observed between uranium and radium isotopes. The doses for the analyzed samples of spring water are in the range 3.59–166.73 μSv y^{− 1} with an average 18.2 μSv y^{− 1} .This is well below the 100 μSv y^{− 1} reference level of the committed effective dose recommended by WHO. Only one water sample had a dose higher than 100 μSv y^{− 1}, mainly due to the contribution from radium (²²⁶Ra, ²²⁴Ra) and ²¹⁰Po isotopes. This study provides important information for consumers and authorities about their internal radiological exposure risk from spring water intake.     

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.     

Comparison of transfers for natural radionuclides (238U, 234Th, 226Ra, 210Pb & 210Po) from five different soils to four different barley genotypes

Transfer Factors (Fv) of ²³⁸U, ²²⁶Ra, ²³⁴Th, ²¹⁰Po and ²¹⁰Pb from five different agricultural soils in semi-arid region (Syria) to four different barley genotypes were studied in an agricultural potted experiment. The geometric mean of the Fv values were (0.08) for ²¹⁰Pb, and (0.02) for ²¹⁰Po, while it ranged from 0.18 to 0.42 ,from 0.08 to 0.15 and from 0.22 to 0.4 for ²³⁸U, ²³⁴Th and ²²⁶Ra, respectevily. The Fv values of ²³⁸U and ²²⁶Ra were within the recommended global medians, while the Fv values of ²³⁴Th, ²¹⁰Pb and ²¹⁰Po were higher. There is no clear relationship between the soil properties and Fv of all studied radionuclides to barley genotypes. Moreover, the expression of glutathione (GSH) gene, which is belived to be involoved in heavy metal removal was generally low in all studied varieties grown in all soil types.

     

Disequilibrium of uranium series radionuclides in soil and plants of South India

Soil and plants of South India were analysed using standard methods for equilibrium state between radionuclides ²²⁶Ra, ²¹⁰Pb, and ²¹⁰Po of uranium series. A disequilibrium state was observed, with mean ²¹⁰Pb/²²⁶Ra, ²¹⁰Po/²²⁶Ra, and ²¹⁰Po/²¹⁰Pb as 21.71, 5.52, and 0.40; 10.01, 4.21, and 0.43; and 30.86, 9.34, and 0.35 in Coastal Karnataka, Malnad Karnataka, and Malnad Kerala, respectively. ²¹⁰Po/²¹⁰Pb in soil was 0.29, 0.30, and 0.49 respectively, for the three regions. Unsupported ²¹⁰Pb and ²¹⁰Po might have caused the observed disequilibrium state. The investigation helps to monitor radionuclide distribution and dynamics in soil and plants of the study area.

     

Effective doses due to intake of radiotoxic radionuclides 226Ra, 210Po and 210Pb through drinking water of coastal Karnataka

The concentrations of ²²⁶Ra, ²¹⁰Po and ²¹⁰Pb have been measured, by high efficiency 5″ × 5″ NaI(Tl) gamma ray spectrometer and chemical deposition method, in surface water samples from major rivers Kali, Sharavathi and Netravathi of coastal Karnataka. Measurements of ²²⁶Ra, ²¹⁰Po and ²¹⁰Pb in surface water from these rivers are important because the river water is main source of potable water in this region due to inadequate supply of treated water. The mean activity of ²²⁶Ra, ²¹⁰Po and ²¹⁰Pb in the surface water of the river Kali was found to be 5.13 mBq L⁻¹, 1.28 and 1.37 Bq L⁻¹, for Sharavathi River the mean activity was found to be 3.37 mBq L⁻¹, 1.30 and 1.44 Bq L⁻¹. In Netravathi River the mean activity of ²²⁶Ra, ²¹⁰Po and ²¹⁰Pb was found to be 3.30 mBq L⁻¹, 1.00 and 1.20 Bq L⁻¹. From the measured concentration of ²²⁶Ra, ²¹⁰Po and ²¹⁰Pb, the Effective dose to the population of the region was computed. The results of these systematic studies are presented and discussed in the paper.     

Determination of <Superscript>3</Superscript>H, <Superscript>226</Superscript>Ra, <Superscript>222</Superscript>Rn and <Superscript>238</Superscript>U in Austrian ground- and drinking water

Screening measurements for ³H, ²²⁶Ra, ²²²Rn and ²³⁸U in ground water were performed within a ground- and drinking water project in Austria. The aim of this project is to get an overview of the distribution of natural radionuclide activity concentration levels in ground water bodies. In some cases this water is used for drinking water abstraction. In this paper methods and results of the screening measurements are presented. Regions with high activity concentrations were identified and in these regions further investigation for ²²⁸Ra, ²¹⁰Pb and ²¹⁰Po will be conducted.     

Determination of natural radioactivity in Euphrates river

Levels of naturally occuring radionuclides (radium isotopes, U isotopes, ²¹⁰Po and ²¹⁰Pb) in water, sediments and biota samples collected from Euphrates river during the 1999–2000 period have been determined. Results have shown that the water contained relatively high levels of ²²⁶Ra; the largest value of 1150 mBq·l^–1 was observed. These relatively high levels of ²²⁶Ra, which is one of the main radioactive contaminants in the oil industry, may be due to past discharges of production water from the oil fields situated near the river banks. ²²⁶Ra/²³⁸U activity ratio was found to be more than unity in all water samples varying between 13 and 242. In addition, the results of sediment analyses have also shown lower values for ²²⁸Ra/²²⁶Ra activity ratio than unity in those samples collected nearby the oil fields. Moreover, concentrations of other naturally occurring radionuclides such as uranium isotopes, ²¹⁰Po and ²¹⁰Pb for most samples (water, sediments and biota) were found to be within the natural levels and in agreement with those values reported for other local and international studies. Only mussel species were found to contain high levels of ²¹⁰Po, about 1335 Bq·kg^–1 dry mass was observed in Anodonta sp species. However, the results of this study can be considered a baseline for monitoring of future changes. A regional research project (including Turkey, Syria and Iraq) to study this river (from the Anatolia Mountains to the Arabian Gulf) is necessary to determine the impact of all potential sources of contaminants.This revised version was published online in November 2005 with corrections to the Cover Date.     

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.     

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.     

Radioactivity in coffee

This research was dedicated to the study of the background levels of ²¹⁰Po and natural gamma emitters as ⁴⁰K, ²¹⁴Pb, ²¹⁴Bi, ²²⁸Ac, ²¹²Pb and ²¹²Bi in coffee powder and in coffee beverage; also the artificial ¹³⁷Cs was determined. In the coffee powder the mean ²¹⁰Po activity resulted 7.25 ± 2.25 × 10^?2 Bq kg^?1. ⁴⁰K showed a mean activity of 907.4 ± 115.6 Bq kg^?1. The mean activity concentration of ²¹⁴Pb and ²¹⁴Bi, indicators of ²²⁶Ra, given as mean value of the two radionuclides, resulted 10.61 ± 4.02 Bq kg^?1. ²²⁸Ac, ²²⁸Ra indicator, showed a mean activity concentration of 13.73 ± 3.20 Bq kg^?1. The mean activity concentration of ²¹²Pb, ²²⁴Ra indicator, was 8.28 ± 2.88 Bq kg^?1. ²⁰⁸Tl, ²²⁴Ra indicator, presented a mean activity concentration of 11.03 ± 4.34 Bq kg^?1. In all samples, the artifical ¹³⁷Cs resulted below the detection limit (2.0 Bq kg^?1). The arithmetical mean value of percentage of ²¹⁰Po extraction in coffee beverage resulted 20.5 ± 6.9. The percentage of transfer of gamma emitters,⁴⁰K, ²¹⁴Pb, ²¹⁴Bi, ²²⁸Ac, ²¹²Pb, ²⁰⁸Tl resulted of 80.0, 33.5, 24.7, 30.0, 35.1 and 53.5 % for ⁴⁰K, ²¹⁴Pb, ²¹⁴Bi, ²²⁸Ac, ²¹²Pb and ²⁰⁸Tl respectively.     

Assessment of 226Ra and 228Ra activity concentration in west coast of India

An investigation on the distribution of ²²⁶Ra and ²²⁸Ra activity concentration in coastal surface sea water from Okha in Gujarat to Ratnagiri in Maharashtra state along the west coast of India was carried out. In-situ pre-concentration technique was used to measure radium isotopes by passing 1,000 L of seawater through MnO₂ impregnated polypropylene filter cartridges at all the locations. ²²⁶Ra was estimated using gamma ray peak of its daughter radionuclides ²¹⁴Bi and ²¹⁴Pb. ²²⁸Ra was estimated from its daughter ²²⁸Ac. In the coastal waters, ²²⁶Ra and ²²⁸Ra activity concentration were observed to be in the range of 1.5–2.9 and 2.5–8.6 Bq m^?3 with a mean of 2.2 and 4.9 Bq m^?3 respectively. The activity of ²²⁸Ra was observed to be more than ²²⁶Ra in all the locations. The variation in spatial distribution of the radium isotopes activity concentration and its ratio with respect to location is discussed in the paper. The radioactive database obtained represents reference values for coastal environment of India.     

Gross alpha and beta activities of airborne particulate samples from Wawel Royal Castle Museum in Cracow, Poland

PM-10, PM-2.5 and PM-1.0 concentrations were measured over an 8 h period at sites both inside and outside the museum of Wawel Royal Castle in Cracow, Poland. Gross alpha (α) and beta (β) activities seemed to vary across the particle size range with generally higher levels of activities in the PM-2.5 particle fraction, and higher activities in the PM-10 fraction, while both the highest and the lowest beta activities were found in PM-1.0 fraction. However, statistically there was no significant difference. The highly radioactive PM-1.0 fraction comprised mainly ²¹⁰Pb and the ²¹⁰Pb progeny, ²¹⁰Bi and ²¹⁰Po, and can be attributed to anthropogenic sourced outdoor radioactive particles brought indoors by visitors. ²¹⁰Pb is considered to be a good tracer of secondary aerosols produced by gas-to-particle conversion. Inside the Museum, the highest level of gross alpha activity was detected in the PM-10 fraction, and was mainly due to the uranium isotopes (²³⁴U, ²³⁵U and ²³⁸U) and their daughter products (²²⁶Ra, ²³²Th, ²¹⁰Po or ²²⁴Ra), and ¹³⁷Cs. The minimum and maximum total indicative doses per 8 h are caused by ¹³⁷Cs and ²³²Th, respectively.     

226Ra, 228Ra and 210Pb Isotopes in Some Water Samples of Mines

A method for the determination of ²²⁶Ra, ²²⁸Ra and ²¹⁰Pb in water samples of mining regions by measuring the and intensities with the help of a liquid scintillation counter is presented. The high-energy part of the -particle spectrum emitted by ²¹⁰Bi is used for the determination of ²¹⁰Pb content in the samples. An attempt is also given to explain the radioactive disequilibrium between ²²⁶Ra and ²¹⁰Pb in the samples investigated.     

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.     

238U, 234U and 226Ra concentrations in mineral waters and their contribution to the annual committed effective dose in Turkey

Activity concentrations of ²³⁴U, ²³⁸U and ²²⁶Ra in mineral waters were determined on the basis of nine water bottling facilities using alpha particle spectrometry. The mineral water samples were collected from three geographic regions of Turkey. The radiochemical separation used in the uranium analysis is based on the isolation of uranium radioisotopes from other radionuclides such as Th, Am, Pu and Np using UTEVA resin. Alpha sources were prepared using electrodeposition method. The activity concentration of ²²⁶Ra was determined after deposition on a membrane using BaSO₄ co-precipitation method. The activity concentrations (mBq L^?1) of ²²⁶Ra, ²³⁸U and ²³⁴U ranged from <0.56 to 165, from <0.42 to 439 and from <0.42 to 464, respectively. The measured activity concentrations were used for the calculation of the average total annual effective ingestion doses for children and adults. The committed effective doses were calculated for three different scenarios according to mineral water consumption rate. In the most extreme scenario (for age group 12–17), all water samples except MW1 and MW2 cause annual committed effective doses below the reference level (0.1 mSv year^?1) recommended by World Health Organization (WHO).     

Radioactivity of coals and fly ashes

The level and the behavior of the naturally occurring primordial radionuclides ²³⁸U, ²²⁶Ra, ²¹⁰Pb, ²³²Th, ²²⁸Ra and ⁴⁰K in coals and fly ashes are described. The activity concentrations of the examined coals and originated from coal mines in Greece ranged from 117 to 435 Bq·kg⁻¹ for ²³⁸U, from 44 to 255 Bq·kg⁻¹ for ²²⁶Ra, from 59 to 205 Bq·kg⁻¹ for ²¹⁰Pb, from 9 to 41 Bq·kg⁻¹ for ²²⁸Ra and from 59 to 227 Bq·kg⁻¹ for ⁴⁰K. These levels are comparable to those appeared in coals of different countries worldwide. The activity concentrations of the examined fly ashes and produced in coal-fired power plants in Greece ranged from 263 to 950 Bq·kg⁻¹ for ²³⁸U, from 142 to 605 Bq·kg⁻¹ for ²²⁶Ra, from 133 to 428 Bq·kg⁻¹ for ²¹⁰Pb, from 27 to 68 Bq·kg⁻¹ for ²²⁸Ra and from 204 to 382 Bq·kg⁻¹ for ⁴⁰K. The results showed that there is an enrichment of the radionuclides in fly ash relative to the input coal during the combustion process. The enrichment factors (EF) ranged from 0.60 to 0.76 for ²³⁸U, from 0.69 to 1.07 for ²²⁶Ra, from 0.57 to 0.75 for ²¹⁰Pb, from 0.86 to 1.11 for ²²⁸Ra and from 0.95 to 1.10 for ⁴⁰K.     

Determination of228Ra in drinking water

A procedure for the analysis of²²⁸Ra in drinking water has been developed. The procedure involves separation of radium by an initial coprecipitation with lead sulfate. The isolated Pb(Ra)SO₄ is then dissolved in sodium diethylenetriamine pentaacetate (DTPA). Radium-228 is co-precipitated from this solution with barium sulfate while the DTPA supernate which contains pre-existing²²⁸Ac is discarded. The purified Ba(Ra)SO₄ precipitate is then allowed to ingrow, generating²²⁸Ac, which is then dissolved in DTPA, isolating both²²⁶Ra and²²⁸Ra in the precipitate while²²⁸ Ac remains in the aqueous supernate. The supernate is partitioned against di-(2-ethylhexyl phosphoric acid), HDEHP, dissolved in n-heptane, which retains the²²⁸Ac. Actinium-228 is then stripped from the organic phase by partitioning against 1M HNO₃. Finally, the²²⁸Ac is coprecipitated onto cerium oxalate. The precipitate is collected on a filter and counted in a low-background beta counter. Radium-228 standards with concentrations ranging from 0.044 to 1.6 Bq were used to establish the detector counting efficiency for²²⁸Ac in cerium oxalate samples, as well as monitoring the chemical yield and absorption factors. The resultant average value of 30.3±2.1 cpm/Bq (uncertainty given at 95% level of confidence) was obtained. Various²²⁸Ra cross checks from U. S. Environmental Protection Agency (EPA) with concentrations of 0.063–0.52 Bq/l were analyzed in order to assess the performance of the procedure. The minimum detectable concentration (MDC) of²²⁸Ra in water with this procedure is 0.015 Bq/l. This is based on a one liter aliquot of sample, a 100 min couting period, and a 3 hour decay interval between the end of²²⁸Ac ingrowth and midpoint of counting. Decontamination factor studies were performed to determine the extent of the carry-over of²³⁸U,²²⁶Ra,²¹⁰Po, and⁹⁰Sr into the final fraction.     

Comparative plant uptake and environmental behavior of U-series radionuclides at a uranium mine-mill

Concentrations of U, Th, Ra, Pb, and Po were determined in native vegetation and underlying substrate (soil and tailings) at various sites around a conventional open pit, acid leach uranium production operation in the Western United States. Radionuclide concentrations in substrate and vegetation were generally elevated above background at all sites disturbed by mining and milling activities. Observed plant/soil CR values for vegetation growing on exposed, weathered tailings were ordered as follows:²³⁸U>²³⁰Th>²¹⁰Po,²²⁶Ra>²¹⁰Pb. We suspect that in the case of sulfuric acid leached tailings, Ra and Pb are sequestered as sulfates, which are highly insoluble relative to U and Th sulfates, resulting in reduced availability for plant uptake. Soil acidity and the saturation condition at the tailings impoundment edge tend to enhance radionuclide availability for plant uptake. The transport of radionuclides to foliage and subsequent retention and absorption may play a role in plant contamination.     

Comprehensive survey of radionuclides in contemporary smokeless tobacco products

There is considerable interest in the chemical composition of smokeless tobacco products (STPs), owing to health concerns associated with their use. Previous studies have documented levels of ²¹⁰Po, ²¹⁰Pb and uranium in STP samples. Here, the levels of 13 α-particle and 15 β-radiation emitting radionuclides have been measured in a broad and representative range of contemporary STPs commercially available in the United States and Sweden. For each radionuclide, the level of radioactivity and calculated mass per gram of STP are reported. The results indicate that, among 34 Swedish snus and 44 US STPs, a more complex radionuclide content exists than previously reported for these products. Of the 28 radionuclides examined, 13 were detected and quantified in one or more STPs. The most frequently identified radionuclides in these STPs were ⁴⁰K, ¹⁴C, ²¹⁰Po and ²²⁶Ra. Over half the STPs also contained ²²⁸Th, and an additional 8 radionuclides were identified in a small number of STPs. The presence of ¹⁴C, ³H and ²³⁰Th are reported in tobacco for the first time. The activity of β-emitters was much greater than those of α-emitters, and the β-emitter ⁴⁰K was present in the STPs with both the greatest radioactivity and mass concentrations. Since the three radionuclides included in the FDA’s HPHC list were either not detected (²³⁵U), identified in only three of 78 samples (²³⁸U), and/or had activity levels over fifty times lower than that of ⁴⁰K (²¹⁰Po, ²³⁸U), there may be a rationale for reconsidering the radionuclides currently included in the FDA HPHC list, particularly with respect to ⁴⁰K. Using a model of the physical and biological compartments which must be considered to estimate the exposure of STP users to radionuclides, we conclude that exposure from α-emitters may be minimal to STP users, but ⁴⁰K in particular may expose the oral cavities of STP users to β-radiation. Although a more comprehensive picture of the radioisotope content of STPs has emerged from this study, epidemiological evidence suggests that the levels of radionuclides measured in this study appear unlikely to present significant risks to STP users.     

Natural radioactivity in bottled natural spring,mineral and therapeutic waters in Poland

Activities of ²³⁸U, ²³⁴U, ²²⁸Ra, ²²⁶Ra, and ²²⁴Ra as well as total α- and β-activities of 23 bottled spring, mineral and therapeutic waters produced and distributed in southern and central Poland are presented. The activities vary from a few tenth to a few mBq·L⁻¹ for uranium and to several hundred mBq·L⁻¹ for radium isotopes. The activities of ⁴⁰K were calculated from chemical analyses of potassium and checked for several mineral waters by gamma-spectrometer coupled with an HPGe detector. Positive correlation between water mineralization and activities of ⁴⁰K, ²²⁶Ra, as well as total alpha- and total beta-activities were observed. The radiological annual doses were calculated for all investigated waters and for different human age groups assuming the consumption of 1 liter of water per day. The calculated committed effective dose rate from uranium and radium isotopes resulting from consumption of the investigated waters exceeds the recommended value of 0.1 mSv per year in seventeen cases for infants and in one case for adults.