Ra-isotopes around a phosphate fertilizer complex in an estuarine system at the Southwest of Spain

The presence of²²⁴Ra and²²⁶Ra in waters from an estuarine system which surrounds a phosphate fertilizer complex (southwest Spain) has been studied. The high activities obtained confirm that an important radiological impact from such industrial complex on its close environment is being produced. The influence of tidal oscillations and seasonal conditions on activity concentration has also been investigated.     

Studies on226Ra and210Pb activities and the concentration factors of226Ra in the surface organic layers of the estuarine sediments of Mindola and Purna rivers in India

The sediment samples have been collected from estuarine regions of Mindola and Purna of Gujarat State. These samples are found to contain less than 3% of organic matter which scavange and carry most of the activity of²²⁶Ra, etc., to the sediment floor. The activities of²²⁶Ra are found to vary from 0.1 to 0.5 pCi/g, while²¹⁰Pb activities lie in the range of 3 to 8 pCi/g. These activities find their way into the organisms present in sea water and then into fish which is finally consumed by humans. This paper gives in detail the sampling techniques, experimental procedures and the distribution of the isotopes of²²⁶Ra and²¹⁰Pb in the estuarine regions and the concentration factors of²²⁶Ra in the region.     

Direct determination of 226Ra in environmental matrices using collision cell inductively coupled plasma mass-spectrometry

Direct determination of ²²⁶Ra in complex environmental matrices (biological and uranium ore samples) by collision-cell inductively coupled plasma mass-spectrometry was investigated. Possible polyatomic interferences were studied and their effects on ²²⁶Ra measurements were determined. The instrumental conditions for optimal signal-to-noise ratio for ²²⁶Ra were found. Concentrations of ²²⁶Ra in certified reference samples were measured using both external calibration and standard addition approaches. The best precision was obtained by applying standard additions. The absolute detection limit for ²²⁶Ra was 1 fg with optimal gas flow rates for the collision cell of 7 ml^.min^-1 for helium and 4 ml^.min^-1 for hydrogen.     

Chemometry of the distribution and origin of 226Ra, 228Ra, 40K and 137Cs in the soil near the lignite fired plants of West Macedonia (Greece)

The distribution and origin of natural ⁴⁰K,²²⁶Ra and²²⁸Ra and artificial ¹³⁷Cs have been investigated in the surface soil of a West Macedonia basin at four lignite fired power plants. No significant increase in specific activity of soil due to natural radionuclides of coal has been found. The specific activities of ²²⁶Ra, ²²⁸Ra and ⁴⁰K are equal to those of Greek soils. Radiocesium activity is slightly higher in the first 10 cm layer. The application of chemometrical methods confirmed that the radionulides ²²⁶Ra, ²²⁸Ra and ⁴⁰K are natural components of the soil and they do not originate from fly ash. This revised version was published online in July 2006 with corrections to the Cover Date.     

Application of a Liquid Scintillation Technique to the Measurement of 226Ra and 224Ra in Samples Affected by Non-Nuclear Industry Wastes

Experiment procedures have been developed for the determination of ²²⁶Ra and ²²⁴Ra activity concentration in solid and liquid samples collected around a non-nuclear industrial area, by liquid scintillation counting. The different radiochemical procedures developed in this work, have been adaptations of a radiochemical procedure previously used, for ²²⁶Ra and ²²⁴Ra determinations by LSC in drinking water, which was improved, refined up and adapted to the type of sample to be applied. These improved radiochemical methods have been applied to waste samples (phosphogypsum) produced by two factories which are engaged in phosphoric acid production, and to waters collected from the Odiel river, where during the sampling period a fraction of these wastes were released. ²²⁶Ra activity concentrations in the phosphogypsum ranged from 673 to 1178 Bq/kg dry weight, indicating that the wastes are particularly enriched in this radionuclide. Consequently, high ²²⁶Ra levels were easily found in the river waters analysed, especially in the neighbouring zones of the waste discharges.     

Rapid sequential separation of actinides using Eichrom's extraction chromatographic material

The presence of ²²⁶ Ra in an estuary formerly affected by direct discharges of waste from a phosphate fertilizer complex has been investigated. Specific activities ranging from 3.6 to 45.2 mBq/l have been detected. In general, activity levels are lower than those detected when direct discharges were carried out. However, there is still a clear contamination due to the disposal of phosphogypsum in open air piles by the river. Moreover, it seems that ²²⁶ Ra is being redissolved from the contaminated bed sediments, which also contributes to an enhancement in the activity levels of the estuary waters.     

Distribution of some natural and anthropogenic radionuclides in Sudanese harbour sediments

The distribution of some natural and anthropogenic radionuclides (²²⁶Ra,²²⁸Ra,²¹⁰Po,⁴⁰K,¹³⁷Cs) in surface marine sediments from the harbours at Port Sudan and Sawakin on the Sudanese coast of the Red Sea has been investigated using α-spectrometry and direct high-resolution γ-spectrometry. The prime ams were to assess the levels of radioactivity and the influence of factors such as dredging and the organic matter content of the sediments on the distribution pattern of the radionuclides. The results have been evaluated and the leves indicate the absence of any possible enhancement by anthropogenic influx from the hinterland. The spatial distribution pattern is more heterogeneous in Sawakin harbour where some parts have recently been dredged and the sludge is removed to maintain the required depth. The data also show an insignificant relationship between the activity concentrations of all the radionuclides and the content of organic matter in the sediments.     

Determination of radium isotopes in mineral and environmental water samples by alpha-spectrometry

Summary A method for the determination of low-level radium isotopes in mineral and environmental water samples by alpha-spectrometry has been developed. Radium-225, which is in equilibrium with its mother ²²⁹Th, was used as a yield tracer. Radium were preconcentrated from water samples by coprecipitation with BaSO₄and iron (III) hydroxide at pH 8-9 using ammonia solution, then isolated from uranium, thorium and iron using a Microthene-TOPO chromatography column at 8M HCl, separated from barium in a cation-exchange resin column using 0.05M 1,2-cyclohexylenedinitrilotetraacetic acid monohydrate at pH 8.5 as an eluant, and finally electrodeposited on a stainless steel disc in a medium of 0.17M (NH₄)₂C₂O₄at pH 2.6 and current density of 400 mA^. cm^-2, and counted bya-spectrometry. Optimum experimental conditions for radium separation, purification and electrodeposition have been studied and discussed in the paper. The lower limits of detection of the method are 0.11 mBq^. l^-1for ²²⁶Ra, ²²⁸Ra and ²²⁴Ra, respectively, if 2 l of water are analyzed. The method has been checked with a certified reference material IAEA-Soil-6 supplied by the International Atomic Energy Agency and reliable results were obtained. Eighteen water samples collected in Italy have been analyzed with the method, the mean radiochemical yields for radium were 86.2±6.5%. The obtained radium concentrations were in the range of 0.50-60.8 mBq^. l^-1for ²²⁶Ra, of 0.10-25.7 mBq^. l^-1for ²²⁸Ra, and of￡LLD-7.97 mBq^. l^-1for ²²⁴Ra. The ²²⁸Ra/²²⁶Ra and ²²⁴Ra/²²⁶Ra ratios were in the range of 0.189-4.45 and￡LLD-0.941, respectively.     

Radium-226 in uranium mill tailings

A study of the physical state of²²⁶Ra in uranium mill tailings was undertaken by Chemex Laboratories Ltd. under contract to NUTP. A test portion of a leached uranium ore was collected just prior to neutralization with lime and subjected to repetitive batch water leaching. The leachates were analyzed for barium, lead,²²⁶Ra, iron and sulphate. The experimental results suggest that²²⁶Ra is co-precipitated with lead sulphate during uranium leaching of the ore with sulphuric acid. The attainment of equilibrium conditions in the pore water of the leached ore then allows a re-proportioning of²²⁶Ra between solid lead and barium sulphates resulting in a depletion of²²⁶Ra in the outer layers of the crystals of solid lead sulphate and an enrichment in²²⁶Ra in the outer layers of solid barium sulphate.     

A simple method for the determination of natural uranium and226Ra in waters and soils

A procedure for the determination of natural uranium and²²⁶Ra in waters and soils has been carried out and applied to the analysis of samples for environmental radiological monitoring.²²⁶Ra determination consists of co-precipitation with BaSO₄,²²²Rn emanation in toluene and finally liquid scintillation counting. Natural uranium is then determined by a fluorometric technique. This paper describes the method and the conditions that were tested to optimize it. The technique was found to be suitable for the analysis of surface and ground waters, samples from rivers, streams and lakes and soil samples, because of its few steps, short processing time, high recovery percentages and suitable detection limits.     

Activity concentration of226Ra and238U in various soils

The distribution of²²⁶Ra and²³⁸U in various soils has been studied. Supposing that radioactive equilibrium were in existence, the average activities of²²⁶Ra and²³⁸U would show a nearly 11 correlation. As weathering affects radioactive equilibrium in surface soil, radioactive equilibrium was not in existence. Therefore, four kinds of soil were selected from different weathering conditions, viz. river bed soil, paddy field soil, field soil and uncropped soil. The²²⁶Ra/²³⁸U ratio of various soils lies in the range of 1.63 to 2.41. The activity concentrations of²²⁶Ra were greater than²³⁸U in various soils. The ratio²²⁶Ra/²³⁸U can be shown to be a quantitative index of weathering. Phosphatic manure contains²³⁸U and its daughter isotopes in concentrations far exceeding the average abundance in the earth's crust. But the cultivated soils (paddy field soil, field soil) are not affected by fertilizers in Kamisaibara.     

222Rn and 226Ra activity concentrations in groundwaters of southern Poland: new data and selected genetic relations

Since 2008, the authors have been conducting research into ²²²Rn and ²²⁶Ra activity concentrations in shallow circulation groundwaters in southern Poland. Measurements have been performed with a liquid-scintillation method and ultra low-level liquid-scintillation spectrometers α/β Quantulus 1220. The research carried out so far has demonstrated that in the Sudetes groundwaters with high activity concentrations of ²²²Rn and ²²⁶Ra are common. In other studied areas in southern Poland no shallow circulation groundwaters with high radon or radium concentrations have been found yet. The conducted research has demonstrated that the activity concentration of ²²²Rn dissolved in shallow circulation groundwaters in the Sudetes depends chiefly on the amount of radon, which after being released as gas from reservoir rocks is dissolved in waters flowing through these rocks. At the same time, the concentration of ²²²Rn dissolved in some shallow circulation groundwaters in the Carpathians is influenced significantly by the amount of radon produced from the decay of its parent ion ²²⁶Ra²⁺ dissolved in these waters.     

<Superscript>226</Superscript>Ra and <Superscript>228</Superscript>Ra determination in environmental samples by alpha-particle spectrometry

A complete methodology for ²²⁶Ra and ²²⁸Ra determination by alpha-particle spectrometry in environmental samples is being applied in our laboratory using ²²⁵Ra as an isotopic tracer. This methodology can be considered highly suitable for the determination of these nuclides when very low absolute limits of detection need to be achieved. The ²²⁶Ra determination can be performed at any time after the isolation of the radium isotopes from the analyzed samples while the ²²⁸Ra determination needs to be carried out at least six months later through the measurement of one of its grand-daughters. The method has been validated by its application to samples with known concentrations of these Ra nuclides, and by comparison with other radiometric methods.     

Rapid determination of 226Ra in drinking water samples using dispersive liquid-liquid microextraction coupled with liquid scintillation counting

A new radioanalytical method was developed for rapid determination of ²²⁶Ra in drinking water samples. The method is based on extraction and preconcentration of ²²⁶Ra from a water sample to an organic solvent using a dispersive liquid-liquid microextraction (DLLME) technique followed by radiometric measurement using liquid scintillation counting. In DLLME for ²²⁶Ra, a mixture of an organic extractant (toluene doped with dibenzo-21-crown-7 and 2-theonyltrifluoroacetone) and a disperser solvent (acetonitrile) is rapidly injected into the water sample resulting in the formation of an emulsion. Within the emulsion, ²²⁶Ra reacts with dibenzo-21-crown-7 and 2-theonyltrifluoroacetone and partitions into the fine droplets of toluene. The water/toluene phases were separated by addition of acetonitrile as a de-emulsifier solvent. The toluene phase containing ²²⁶Ra was then measured by liquid scintillation counting. Several parameters were studied to optimize the extraction efficiency of ²²⁶Ra, including water immiscible organic solvent, disperser and de-emulsifier solvent type and their volume, chelating ligands for ²²⁶Ra and their concentrations, inorganic salt additive and its concentration, and equilibrium pH. With the optimized DLLME conditions, the accuracy (expressed as relative bias, B _r ) and method repeatability (expressed as relative precision, S _B ) were determined by spiking ²²⁶Ra at the maximum acceptable concentration level (0.5 Bq L⁻¹) according to the Guidelines for Canadian Drinking Water Quality. Accuracy and repeatability were found to be less than −5% (B _r ) and less than 6% (S _B ), respectively, for both tap water and bottled natural spring water samples. The minimum detectable activity and sample turnaround time for determination of ²²⁶Ra was 33 mBq L⁻¹ and less than 3 h, respectively. The DLLME technique is selective for extraction of ²²⁶Ra from its decay progenies.     

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.     

Rapid determination of 226Ra in emergency urine samples

A new method has been developed at the Savannah River National Laboratory (SRNL) that can be used for the rapid determination of ²²⁶Ra in emergency urine samples following a radiological incident. If a radiological dispersive device event or a nuclear accident occurs, there will be an urgent need for rapid analyses of radionuclides in urine samples to ensure the safety of the public. Large numbers of urine samples will have to be analyzed very quickly. This new SRNL method was applied to 100 mL urine aliquots, however this method can be applied to smaller or larger sample aliquots as needed. The method was optimized for rapid turnaround times; urine samples may be prepared for counting in <3 h. A rapid calcium phosphate precipitation method was used to pre-concentrate ²²⁶Ra from the urine sample matrix, followed by removal of calcium by cation exchange separation. A stacked elution method using DGA Resin was used to purify the ²²⁶Ra during the cation exchange elution step. This approach combines the cation resin elution step with the simultaneous purification of ²²⁶Ra with DGA Resin, saving time. ¹³³Ba was used instead of ²²⁵Ra as tracer to allow immediate counting; however, ²²⁵Ra can still be used as an option. The rapid purification of ²²⁶Ra to remove interferences using DGA Resin was compared with a slightly longer Ln Resin approach. A final barium sulfate micro-precipitation step was used with isopropanol present to reduce solubility; producing alpha spectrometry sources with peaks typically <40 keV FWHM (full width half max). This new rapid method is fast, has very high tracer yield (>90 %), and removes interferences effectively. The sample preparation method can also be adapted to ICP-MS measurement of ²²⁶Ra, with rapid removal of isobaric interferences.     

Contribution to the simultaneous determination of228Ra and226Ra by using 3M's EMPORETM radium rad disks

New method for simultaneous determination of²²⁸Ra and²²⁶Ra by using 3M's EMPORE^TM Radium Rad Disks in water has been developed. Both radionuclides²²⁶Ra and²²⁸Ra were counted through their daughter products,²²⁶Ra by conventional radon emanation techniques and²²⁸Ra through its daughter²²⁸Ac by using a proportional counter. Different molarity of diammonium hydrogen citrate were used for elution of²²⁸Ac and²²⁶Ra from EMPORE^TM Radium Rad Disks. 79% of²²⁸Ac was eluted in 10 ml of 0.0003M diammonium hydrogen citrate. The recovery of²²⁶Ra was 99% by using 40 ml of 0.2M diammonium hydrogen citrate adjusted by ammonium to pH 7.8.     

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.     

Gamma-Ray Emission Probabilities in the Decay of 226Ra and Its Daughters

Relative gamma-ray emission probabilities in the decay of ²²⁶Ra and its decay products have been measured using a HPGe detector. The resulting data have been evaluated together with five previously published sets of ²²⁶Ra gamma-ray emission probabilities.     

Chemometrics of the distribution and origin of <Superscript>226</Superscript>Ra, <Superscript>228</Superscript>Ra, <Superscript>40</Superscript>K and <Superscript>137</Superscript>Cs in plants near the West Macedonia Lignite Center (Greece)

Summary The distribution and origin of ⁴⁰K, ²²⁶Ra, ²²⁸Ra and ¹³⁷Cs has been investigated in trees, mosses and lichens in the basin of the West Macedonia Lignite Centre. In tree leaves ¹³⁷Cs is negligible, while the ²²⁶Ra and ²²⁸Ra concentrations are affected by the fly ash particles. Concerning ²²⁶Ra and ²²⁸Ra values of mosses and lichens, which are systematically larger than those of unpolluted areas, the application of chemometrics proved that they originate mainly from the lignite fly ash.