Radiological characterization of phosphate fertilizers: Comparison between alpha and gamma spectrometry

The natural radioactivity in phosphate fertilizers used in central Italy has been measured by alpha and gamma spectrometry. The results show that the specific activities of ²³⁸U, ²³⁴U and ²³⁵U ranged within interval from < 0.5 to 2628.8, from < 0.5 to 2826.3 and from < 0.9 to 138.0 Bq kg^{− 1} respectively and those of ²¹⁰Pb and ²¹⁰Po ranged within interval from < 15.0 to 401.5 and < 0.5 to 351.6 Bq kg^{− 1} respectively. The ²²⁸Th, ²³⁰Th and ²³²Th concentrations found by alpha spectrometry ranged from < 0.5 to 50.2, from 0.9 to 2727.2 and from < 0.5 to 60.8 Bq kg^{− 1} respectively. ²²⁶Ra and ²²⁸Ra activity concentrations ranged from < 14.3 to 290.9 and from < 2.9 to 24.9 respectively. ⁴⁰K specific activities ranged from 39.2 to 8263.7 Bq kg^{− 1}. A very good correlation exists between the activity concentrations found by alpha spectrometry and those found by gamma spectrometry.     

Advantages of low-background liquid scintillation alpha-spectrometry and pulse shape analysis in measuring222Rn, uranium and226Ra in groundwater samples

Liquid scintillation counting (LSC) and pulse shape analysis (PSA) was used in measuring radon and gross alpha- and beta-activities in groundwater. We used conventional LSC counters for the measurement of radon in water, but low-background LSC spectrometers for the gross activity measurements. The lower limit of detection (LLD) for radon in water is 0.6 Bq/l for a 60 min count with a conventional counter, but 0.1 or 0.2 Bq/l, with the two types of low-background LSC spectrometers equipped with a pulse shape analyser (PSA). The gross alpha and beta activity measurements are made using a simple sample preparation method, PSA of a low background LSC and spectrum analysis. The LLD recorded for gross alpha and beta with the two spectrometers are 0.02 and 0.03 Bq/l and 0.2 and 0.4 Bq/l, respectively, for a 180 minutes count and a 38 ml sample volume. The method also enable the calculation of the U and²²⁶Ra contents in water and indicates the presence of some other long-lived radionuclides (²¹⁰Pb,²²⁸Ra or⁴⁰K). The LLD for U recorded with both spectrometers is 0.02 Bq^–1 and for²²⁶Ra 0.01 Bq·1^–1. The LLDs attained by this LSC method are two orders of magnitude lower than the maximum permissible concentrations set for U and²²⁶Ra.     

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).     

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.     

226Ra, 228Ra and 228Ra/226Ra in surface marine sediment of Malaysia

Surface sediment samples were collected at the West (east coast and west coast of Peninsular Malaysia) and East (Sabah and Sarawak) Malaysia in several expeditions within August 2003 until June 2008 for determining the level of natural radium isotopes. Activity concentrations of ²²⁶Ra and ²²⁸Ra in surface marine sediment at 176 sampling stations were measured. The activity concentrations of both radionuclides in Malaysia (East and West Malaysia) display varied with the range from 9 to 158 Bq/kg dry wt. and 13 to 104 Bq/kg dry wt., respectively. Meanwhile, the ratio distributions of ²²⁸Ra/²²⁶Ra were ranged from 0.62 to 3.75. This indicated that the ratios were slightly high at west coast of Peninsular Malaysia compared to other regions (east coast of Peninsular Malaysia, Sabah and Sarawak). The variation of activity concentrations of ²²⁶Ra and ²²⁸Ra and its ratios were also supported by the statistical analyses of one-way ANOVA and t test at 95 % confidence level, whereby there were proved that the measured values were different between the regions. These different were strictly related to their half-life, potential input sources (included their parents, ²³⁸U and ²³²Th), parent’s characteristic, the geological setting/formation of the study area, environment origin and behavior.     

Determination of226Ra and uranium in fish samples from waters of the Grand Canyon by alpha spectroscopy without electrodeposition

A previous paper reported the application of a method for determining²²⁶Ra by -spectroscopy. This paper presents important improvements which permit the determination of²²⁶Ra in the presence of large amounts of Ca. The method was applied to the analysis of²²⁶Ra and U isotopes in fish samples from the waters of the Grand Canyon.²²⁶Ra ranged from 0.05 Bq kg^–1 /1.4 pCi kg^–1/ to 0.17 Bq k^–1 /4.7 pCi kg^–1/.²³⁸U values ranged from 0.13 Bq kg^–1 /3.5 pCi kg^–1/ to 0.52 Bq kg^–1 /14 pCi kg^–1/ and²³⁴U values were between 0.23 Bq kg^–1 /6.2 pCi kg^–1/ and 12 Bq kg^–1/ /326. pCi kg^–1/.     

Radiological characterization of drinking waters in Central Italy

Due to the importance of water in human life, its quality must be strictly controlled; for this purpose, simple and reliable analytical methods must be available. In this study, a monitoring of radioactivity content was performed in tap waters collected in a region of Central Italy to check the compliance with recent European and Italian regulations. Gross alpha and beta activities, ²³⁸U, ²³⁴U, ²²⁶Ra, ²²²Rn, and ³H concentrations were measured. Gross alpha and beta activities were determined by standard ISO 9696 and ISO 9697; for ²²⁶Ra, ²²²Rn and ³H determination, liquid scintillation was used. ²³⁸U and ²³⁴U concentrations were determined by alpha spectrometry after separation from the matrix by extraction chromatography and electroplating. The results revealed that the tritium concentration was always lower than 6.75 Bq l^− 1. The concentrations (mBq l^− 1) of ²²⁶Ra, ²²²Rn, ²³⁸U, and ²³⁴U ranged from < 1.70 to 15.31, from 0.69 to 20.3, from 0.65 to 48.77, and from 0.78 to 51.50, respectively.²³⁴U/²³⁸U ratios were higher than 1 in most cases. The results obtained revealed that, in most samples, gross alpha and gross beta were lower than the parameter value indicated in the international regulations. An attempt was also made to find a correlation between these results and the chemical parameters of waters.     

Natural radionuclides in Austrian bottled mineral waters

All commercially available mineral waters of Austrian origin were investigated with regard to the natural radionuclides ²²⁸Ra, ²²⁶Ra, ²¹⁰Pb, ²¹⁰Po, ²³⁸U and ²³⁴U. From 1 to 1.5 L of sample the nuclides were extracted and measured sequentially: the radium isotopes as well as ²¹⁰Pb were measured by liquid scintillation counting after separation on a membrane loaded with element-selective particles (Empore Radium Disks), ²¹⁰Po was determined by α-particle spectroscopy after spontaneous deposition onto a copper planchette and uranium was determined also by α-particle spectroscopy after anion separation and microprecipitation with NdF₃. The calculated committed effective doses for adults, teens and babies were compared to the total indicative dose of 0.1 mSv/year given in the EC Drinking Water Directive. The dominant portion of the committed effective dose was due to ²²⁸Ra. Highly mineralised waters showed also higher ²²⁶Ra and ²²⁸Ra levels.     

Radionuclides analysis in hot spring waters in Korea by liquid scintillation counting

Tritium and ¹⁴C concentration in hot spring water in Korea were determined. Tritium in the most hot spring samples could not detected and concentration range was <0.5?C1.31?TU. And ¹⁴C contents were ranged 1.7?C78.6?pMC. From the ³H and ¹⁴C analysis, we found some hot springs are mixed with recent groundwater and hot spring water ages were estimated from 1,940 to 32,800?years. And also, ²²⁶Ra and ²²⁸Ra were determined simultaneously in hot spring water, and some other radionuclides were also analyzed. Content distribution of ²²²Rn was 50?C3,760?pCi/L, ²²⁶Ra was <0.003?C0.15?Bq/L and ²²⁸Ra was below the detection limit.     

Natural radioactivity levels in mineral,therapeutic and spring waters in Tunisia

Radioactivity measurements were carried out in 26 groundwater samples from Tunisia. Activity concentrations of uranium were studied by radiochemical separation procedures followed by alpha spectrometry and that for radium isotopes by gamma-ray spectrometry.The results show that, the concentrations in water samples range from 1.2 to 69 mBq/L.1, 1.3 to 153.4 mBq/L, 2.0 to 1630.0 mBq/L and 2.0 to 1032.0 mBq/L for ²³⁸U, ²³⁴U, ²²⁶Ra and ²²⁸Ra, respectively. The U and Ra activity concentrations are low and similar to those published for other regions in the world. The natural radioactivity levels in the investigated samples are generally increased from mineral waters through therapeutic to the spring waters.The results show that a correlation between total dissolved solids (TDS) values and the ²²⁶Ra concentrations was found to be high indicating that ²⁶⁶Ra has a high affinity towards the majority of mineral elements dissolved in these waters. High correlation coefficients were also observed between ²²⁶Ra content and chloride ions for Cl^?–Na⁺ water types. This can be explained by the fact that radium forms a complex with chloride and in this form is more soluble.The isotopic ratio of ²³⁴U/²³⁸U and ²²⁶Ra/²³⁴U varies in the range from 0.8 to 2.6 and 0.6 to 360.8, respectively, in all investigated waters, which means that there is no radioactive equilibrium between the two members of the ²³⁸U series. The fractionation of isotopes of a given element may occur because of preferential leaching of one, or by the direct action of recoil during radioactive decay.The annual effective doses due to ingestion of the mineral waters have been estimated to be well below the 0.1 mSv/y reference dose level.     

Natural and Artificial Radionuclides in Selected Lignites from Istanbul

The radioactivity levels of Istanbul environs lignites were determined. The gamma-spectrometric technique has been used for the determination of activity levels of naturally occurring radionuclides ^235+238U, ^228+232Th, ⁴⁰K, ²²⁶Ra and fallout radionuclides ¹³⁷Cs in lignites taken from 7 different parts of Istanbul. Concentration of ²³⁸U, ^228+232Th, ⁴⁰K, ²²⁶Ra ¹³⁷Cs and ²³⁵U were found up to 1.6 ppm, 1.7 ppm, 4.9 ppm, 56.8 Bq/kg, 34 Bq/kg, 1.8 Bq/kg, 1.6 Bq/kg, respectively. In addition total alpha- and beta-activity levels in lignite samples were found to be 7.6 and 15 eps, respectively.     

Comparison of analytical methods used to determine <Superscript>235</Superscript>U, <Superscript>238</Superscript>U and <Superscript>210</Superscript>Pb from sediment samples by alpha,beta and gamma spectrometry

An intercomparison of the methodology (alpha, beta and gamma spectrometry) used for ²³⁸U, ²³⁵U and ²¹⁰Pb determination was carried out based on 38 sediment samples. The activity range of the samples varied from 10–700 Bq/kg for ²¹⁰Pb, 1–35 Bq/kg for ²³⁵U and 10–800 Bq/kg for ²³⁸U. Results obtained using the three methods were not statistically different at high activity levels, but agreement between the results decreased at lower sample activity levels. For ²¹⁰Pb, the smallest difference was found between alpha and gamma spectrometry. A good correlation between results from alpha and gamma spectrometry was observed over the whole activity range. In beta spectrometry, the results were slightly higher than those obtained by alpha or gamma spectrometry due to the impurity of ²²⁸Ra. In ²³⁸U analysis, good correspondence was observed between ²³⁸U determined by gamma and alpha spectrometry, particularly at higher ²³⁸U activity concentrations over 100 Bq/kg. In ²³⁵U analysis, attention needs to be paid to interference from ²²⁶Ra and its reduction.     

234U and 238U in mineral water: reference value and uncertainty evaluation in the frame of an interlaboratory comparison

In 2007/2008 the Institute for Reference Materials and Measurements (IRMM) organised an interlaboratory comparison (ILC) on the determination of ²²⁶Ra, ²²⁸Ra, ²³⁴U and ²³⁸U activity concentrations in mineral water. This paper describes the determination of the reference values for the activity concentrations of ²³⁴U and ²³⁸U by radiochemical separation and α-particle spectrometry performed at two independent laboratories. The experimental uncertainty of the reference values is discussed in detail.     

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%.     

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.     

Radioactive Contamination of Lichens and Mosses Collected in South Shetlands and Antarctic Peninsula

Samples belonging to two species of lichen and one of moss collected on the Antarctic seashore (King George Island, Deception, Antarctic Peninsula) were analysed for gamma-emitters using HPGe gamma-spectrometry, and for alpha-emitters using alpha-spectrometry with silicon detectors. Observed ¹³⁷Cs activities show large variations: from 4.1±0.4 to 74±3 Bq/kg. Total activity of ²¹⁰Pb changed from <2 to 125±35 Bq/kg. The ^2391240Pu activity ranged from 0.07±0.02 to 2.95±0.16 Bq/kg. The activity of ²³⁸Pu ranged from <0.02 to 0.64±0.04 Bq/kg. Maximum ²³⁸U and ²³⁴U activity was 7 Bq/kg, respectively, and 0.3 Bq/kg for ²³⁵U, whereas minimum activities were below 0.5 Bq/kg for ²³⁴U and ²³⁸U and about 0.02 Bq/kg for ²³⁵U. The ²³⁵U to ²³⁸U activity ratio for most of the samples was natural. Thorium activities were about two times lower than those for uranium. The activities of ¹⁴⁷Sm ranged from 0.014±0.002 to 1.0±0.2 Bq/kg. One sample had relatively high activity of ²⁴¹Am: 3.38±0.11 Bq/kg, another did not exceeded 1 Bq/kg. Observed activity ratios confirmed differences between mosses and lichen accumulation properties for radionuclides. Lichens are more selective for plutonium accumulation. Some radiocesium and probably also americium can be leached from them.     

Using the 186-keV peak for 226Ra activity concentration determination in Hungarian coal-slag samples by gamma-ray spectroscopy

The uranium isotopic abundance and the ²³⁸U–²²⁶Ra secular equilibrium were determined in nine Hungarian coal slag samples. The ²²⁶Ra activity concentration was measured based on the radon decay products and also the ²²⁶Ra peak at 186 keV. Secular equilibrium existed in eight samples, whereas one sample showed a slight disequilibrium. The direct and fast measurement using only the 186 keV peak was validated which can be used after measuring the uranium isotopic ratio and verifying the ²³⁸U–²²⁶Ra secular equilibrium. This method can be used to measure the ²²⁶Ra content of high number of samples from the same geochemical background.     

Background levels of238U and226Ra in atmospheric aerosols

The²³⁸U and²²⁶Ra contents of small-volume aerosols are determined by a chemical analysis technique. Mean activity concentrations of²³⁸U and²²⁶Ra in aerosols over approximately ten years are 0.29·10^–5 and 0.93·10^–5 Bq/m³, respectively. The yearly variation of²³⁸U and²²⁶Ra in aerosols is small. The concentrations of²²⁶Ra are always larger than those of²³⁸U in the same sampling time. The correlation of²³⁸U and²²⁶Ra cannot be recogonized (r=0.18). The concentrations of summer samples are greater than those of winter samples for²³⁸U. One of the causes of seasonal difference may be due to the fact that the components of aerosols are different according to soil size, soil components, weathering states, etc.     

Distribution of 238U, 226Ra, 232Th and 40K in soil samples around Tarapur,India

The radioactivity concentrations of ²³⁸U, ²²⁶Ra, ²³²Th and ⁴⁰K in soil samples around Tarapur vary from 11.5 ± 2.6 to 50.3 ± 6.6, 14.9 ± 0.6 to 40.5 ± 1.2, 18.1 ± 0.4 to 75.0 ± 1.5 and 130.1 ± 1.6 to 295.1 ± 2.6 Bq/Kg respectively. The measured activity concentrations for ²³⁸U and ²²⁶Ra were compared and found in good agreement with the Indian as well as world average. The average ²³²Th and ⁴⁰K concentrations in Tarapur were lower than the Indian average value.     

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.