Radiological characterization of the tailings of an abandoned copper mine using a neural network and geostatistical analysis through the Co-Kriging method.

The radiological characterization of soil contaminated with natural radionuclides enables the classification of the area under investigation, the optimization of laboratory measurements, and informed decision-making on potential site remediation. Neural networks (NN) are emerging as a new candidate for performing these tasks as an alternative to conventional geostatistical tools such as Co-Kriging. This study demonstrates the implementation of a NN for estimating radiological values such as ambient dose equivalent (H*(10)), surface activity and activity concentrations of natural radionuclides present in a waste dump of a Cu mine with a high level of natural radionuclides. The results obtained using a NN were compared with those estimated by Co-Kriging. Both models reproduced field measurements equivalently as a function of spatial coordinates. Similarly, the deviations from the reference concentration values obtained in the output layer of the NN were smaller than the deviations obtained from the multiple regression analysis (MRA), as indicated by the results of the root mean square error. Finally, the method validation showed that the estimation of radiological parameters based on their spatial coordinates faithfully reproduced the affected area. The estimation of the activity concentrations was less accurate for both the NN and MRA; however, both methods gave statistically comparable results for activity concentrations obtained by gamma spectrometry (Student's t-test and Fisher's F-test).

Influence of soil chemical composition on U, 226Ra and 210Pb uptake in leaves and fruits of Quercus ilex L.

To determine their transfer factors, activity concentrations of natural radionuclides were measured in the leaves and acorns of holm oak (Quercus ilex L.) trees collected from seven locations with different soil properties and radionuclide activity concentrations. The chemical and mineralogical compositions of the soils were also analysed to investigate the effect these had on radionuclide absorption by the trees. Soil chemistry showed significant effects on radionuclide incorporation into Quercus ilex L. tissues. A significant relationship was established between activity concentrations and soil content of Ca and P with 238U and 226Ra in the leaves and acorns of Quercus ilex L. Differentiated transfer was found for 40K, which showed greater transfer to the leaves than the other radionuclides. The activity concentration of U and 226Ra was higher in the fruits than in the leaves, with the opposite effect being observed for 40K. The risk of U and 226Ra transfer into the food chain through acorn consumption by livestock is predicted to increase in soils poor in Ca and rich in P.

Increasing the recovery and selectivity of 238U, 235U, and 234U extraction with tri-n-butyl phosphate in mine tailing samples with a high copper content.

Abandoned Cu mine tailings may be associated high concentrations of U. However, the presence of stable cations such as Cu, Fe, Al, Ca, or Mg, etc. in high concentrations can reduce the chemical efficiency of the liquid-liquid extraction method with tri-n-butyl phosphate (TBP); it can also inhibit the electrodeposition of U on the stainless steel planchet where the sample is measured. In this work we studied an initial stage of complexation with ethylenediaminetetraacetic acid (EDTA) and a back extraction with different solutions: H2O, Na2CO3, and (NH4)2CO3 at room temperature and at 80 °C. The sensitivity of the method was 4.9·10-4 Bq for 238U and 234U, and 2.3·10-5 Bq for 235U. The validation of the method achieved 95% of the results when using a |ζ-score| ≤ ± 2.0 and a relative bias (RB[%]) ≤ ± 20% as the acceptance criteria. The recoveries obtained with the proposed method were higher than those achieved with the extraction method without initial complexation and re-extraction with H2O for water samples. Finally, this method was applied in practice to study the tailing of an abandoned Cu mine and the activity concentrations of 238U and 235U were compared with those obtained by gamma spectrometry for 234Th and 235U. The means and variances of both methods showed no significant differences between these two isotopes.

Improvements in the radiochemical method for separating 226Ra in solid samples through coprecipitation with BaSO4.

The aim of this work was to improve the commonly used method for 226Ra determination in water and to establish its application in solid samples. This method is based on the coprecipitation of Ra with BaSO4 and gross alpha counting of the precipitate. An exhaustive study of the coprecipitation behaviour of the most abundant cations present in solid samples was performed to avoid incorrect radiochemical yields. As a result, it was considered necessary to introduce two new purification steps into the conventional method. Likewise, two nuclides, 241Am and 226Ra, were compared to obtain the mass efficiency curve given their different behaviour in the coprecipitation process. While Ra behaves similarly to Ba, Am coprecipitates, forming mixed crystals that may behave differently in the self-absorption process. The influence of the cations on the chemical yield with no precipitate purification was: Sr2+≫Fe3+>Mg2+≈Ca2+>K+≈Na+. The method was successfully applied to soil, sediment, and plant ash samples.

Development of a reference material for analysing naturally occurring radioactive material from the steel industry.

Accurate measurement of naturally occurring radionuclides in blast furnace slag, a by-product of the steel industry, is required for compliance with building regulations where it is often used as an ingredient in cement. A matrix reference blast furnace slag material has been developed to support traceability in these measurements. Raw material provided by a commercial producer underwent stability and homogeneity testing, as well as characterisation of matrix constituents, to provide a final candidate reference material. The radionuclide content was then determined during a comparison exercise that included 23 laboratories from 14 countries. Participants determined the activity per unit mass for 226Ra, 232Th and 40K using a range of techniques. The consensus values obtained from the power-moderated mean of the reported participant results were used as indicative activity per unit mass values for the three radionuclides: A0(226Ra) = 106.3 (34) Bq·kg-1, A0(232Th) = 130.0 (48) Bq·kg-1 and A0(40K) = 161 (11) Bq·kg-1 (where the number in parentheses is the numerical value of the combined standard uncertainty referred to the corresponding last digits of the quoted result). This exercise helps to address the current shortage of NORM industry reference materials, putting in place infrastructure for production of further reference materials.

Factors that influence the absorption of uranium by indigenous plants on the spoil tip of an abandoned mine in western Spain.

The purpose of this work was to study the factors affecting the absorption of U by plants growing on the spoil tip of an abandoned mine in western Spain. The plant species were selected based on how palatable they were to livestock and were sampled for four consecutive years during which, we also recorded rainfall data. The factors related to the plants studied were the leaf size and the percentage and characteristics of the arbuscular mycorrhizae (AM) fungi present in their roots. Our results showed a correlation between the annual rainfall and the U concentration in the plants. The percentage of mycorrhization and AM vesicles is a predominant factor in the uptake of U by plants. Spergularia rubra (L.) J.Presl & C.Presl, which is resistant to mycorrhization, contained higher U concentrations relative to the plants that grew with AM mycorrhization. The absorption curves of the different plants studied indicated that these plants were tolerant to 238U from 875 Bq kg-1 (70 mg kg-1), with a hormesis effect below that concentration. The annual U removal was 0.068%, suggesting that AM are responsible for limiting the incorporation of U into the food chain, favouring its retention in the soil and preventing its dispersion.

Data on natural radionuclide's activity concentration of cement-based materials.

Cement based materials may contain varying levels of radionuclides, mainly 226Ra (from the 238U series), 232Th and 40K, which are used to determine the Activity Concentration Index ("ACI"). According to the European directive Euratom 2013/59 in these materials, the "ACI" must be < 1 to be suitable for their use in construction. In this paper, data on the activity concentration of natural radionuclides in cement-based materials (i.e. cements, additions, pigments and aggregates) as well as their chemical composition are presented. Radioactivity measurements have been determined by using gamma spectroscopy the chemical compositions have been determined by X-Ray Fluorescence. Data for cements measured shown that white cements present a lower concentration of activity than conventional CEM I. In addition, the CAC (Calcium aluminate cements) present high activity concentration in the 232Th series. Regarding additions, FA (Fly Ash) are those that present the highest concentration of activity in the 238U and 232Th series, while olive biomass ashes are those supplementary cementitious materials that show the highest concentration of activity for 40K. Some pigments used in mortar and concrete technology were also characterized. Granitic and volcanic rocks, potentially used as aggregates present much higher activity concentration than the siliceous aggregate.

Characteristic limits of 230Th in alpha spectrometry with 229Th as tracer, calculated by simulating interfering tails and overlapping peaks.

This study explores the effect of 229Th tracer tail interference on the determination of the sensitivity of 230Th alpha spectrometry of samples with environmental levels of radioactivity. Tracer peak tail interference was calculated with Suma-Alpha, whilst Visual Basic for Applications (VBA in Excel©) software was used to study the variation in sensitivity in terms of the amount of tracer added. Unnecessary increases in the amount of tracer or extended sample measuring times were observed to have adverse effects on method sensitivity (Detection Limit- Ld).

A radiological index for evaluating the impact of an abandoned uranium mining area in Salamanca, Western Spain.

The establishment of a screening index would be a powerful tool to decide whether abandoned uranium mining areas should be rehabilitated or decommissioned. Thus, in this work we established a radiological index which uses the activity concentrations of different groups of gamma emitters from the natural radioactive series of 238U, 235U, and 232Th, as well as 40K and 137Cs. These activity concentrations were calculated by using the absorbed gamma radiation dose value of 175 nGy h-1 specified in the U.S. Code of Federal Regulations. We studied our index in an abandoned uranium mining area in Salamanca, Western Spain, and found that the most influential factors in this area were the presence of organic matter in the soil and the possible effect that plants and fungi may have on the retention of these aforementioned radionuclides. In addition, the results showed that contaminants are migrating in an easterly direction in line with the prevailing wind direction and we were able to identify areas in which the radiological risk is likely high. The mean effective dose rate was 2.51 ± 0.98 mSv y-1 which was equivalent to the levels obtained in previous works.

Use of Genie 2000 and Excel VBA to correct for γ-ray interference in the determination of NORM building material activity concentrations.

The γ-radiation emitted by building materials is calculated from the activity indices for 232Th, 226Ra and 40K and expressed as the activity concentration index (ACI). Gamma spectroscopy is a non-destructive technique frequently used to simultaneously determine the indices for several radionuclides. Spectral interpretation poses a number of challenges, including identification of γ-lines subject to summing-in effects, interference from other γ-ray emitting radionuclides and the time required to reach secular equilibrium. These challenges are not fully addressed by Canberra Industries' Genie 2000, the software used by many laboratories to analyse samples. This article describes a Microsoft Excel workbook that exploits Genie 2000 flexibility to program applications with Visual Basic using Canberra's Nuclear Data Access Library and batch procedure tools. The workbook determines 40K activity concentration after correcting for 228Ac interference and 226Ra activity directly from the γ-peak at 186.5 keV. The method proposed was tested by participating in 13 national and international scale inter-comparison exercises. The results were statistically indistinguishable from the reference values at a coverage factor of k = 3 and no statistically significant differences were identified between the respective means by a Student's t pairwise comparison.

Determination of specific alpha-emitting radionuclides (uranium, plutonium, thorium and polonium) in water using [Ba+Fe]-coprecipitation method.

The indicative dose (ID) is one of the parameters established in the current European directive for water intended for human consumption. To determine the ID, it is necessary to know the activity concentration of: 238U, 234U, 226Ra, 210Po, 239,240Pu and 241Am. The existing methods to determine these radionuclides involve complex radiochemical separations (ionic exchange columns, extraction chromatography, etc.), followed by measurements with a semiconductor detector, laboratory procedures that are time-consuming and costly. As a lower cost alternative that reduces measuring and preparation times, avoids the need for a self-absorption correction and the use of tracers, and above all that can be used in any laboratory, methods based on liquid-liquid extraction and selective co-precipitation were developed. These methodologies offer high separation recovery and selectivity, and the measurements are made using a gas proportional counter or a solid ZnS(Ag) scintillation counter. The separation factor ranged between 91.4% and 100.0% for all alpha-emitting radionuclides across the different methods. The activity concentration for each method was computed through linear equations that represent the relationship between the activity and selectivity of the different alpha-emitting radionuclides. This mathematical procedure simplifies the radiochemical separations and provides more accurate activity concentrations. The results of the internal and external validation studies proved that the proposed method is suitable for determining 241Am, 226Ra, uranium, plutonium, thorium and 210Po in water samples.

Sample pretreatment in the determination of specific alpha emitters in drinking water using [Ba+Fe]-coprecipitation method.

The [Ba+Fe]-coprecipitation method is applied to measure gross alpha activity for radiological examination of drinking water in the laboratory. This method collects all the alpha-emitting radionuclides of interest (natural alpha emitters and transuranium elements) in a precipitate on a filter. This paper describes an investigation of sample pretreatment of the precipitate collected by the [Ba+Fe]-coprecipitation method for gross alpha activity determination. The aim of this preliminary work is to be a starting point to develop simple and rapid radiochemical procedures for specific alpha emitters (polonium, radium, thorium, uranium, plutonium and americium), in contrast to the sophisticated, expensive and time-consuming alpha spectrometry method. The sample pretreatment aspects considered include quantitative [Ba+Fe]-coprecipitation, two methods for precipitate treatment (leaching and complete destruction of the filter), and the determination of the alpha-emitting proportions present in the barium sulfate precipitate and acid solution obtained after precipitate treatment. Furthermore, a radiochemical procedure for (226)Ra determination was performed and finally, the sample pretreatment proposed in this work was summarized.

Self-absorption correction for beta radioactivity measurements in water samples.

Two methods were used to apply self-absorption corrections for the determination of beta radioactivity in water samples (either for an identified radionuclide or for monitoring trends). One method was performed by estimating the absorption coefficient by assuming an exponential behaviour of absorption using external absorbers, while the other method was performed by preparing empirical curves using standards of different mass. In the first method, a relationship between absorption coefficient and maximum beta energy was also derived. In the second method, self-absorption curves for 90Sr/90Y standard were prepared with several sodium salts (carbonate, nitrate and sulphate salts) and, for 40K standard using a potassium salt. Both beta emitters are usually necessary to calibrate detectors for beta radioactivity measurements. This study showed that, for 90Sr/90Y, results using standards of different mass were more accurate than using external absorbers. Furthermore, it is highly recommended to melt sodium nitrate salts in order to perform a self-absorption curve for 90Sr/90Y because standards were stable in time and homogeneously distributed. For 40K, a self-absorption curve may be easily derived using paper absorbers of different thickness, instead of performing a time consuming self-absorption curve using a set of varying thickness of 40K standards. In order to test the two methods, the gross beta activity of several environmental water samples was analysed.

A method for the selection of the optimum counting conditions in a ZnS(Ag) scintillation detector.

The well-known criteria for the selection of the optimum counting conditions in a ZnS(Ag) scintillation detector seem to restrict its applicability. These do not consider simultaneously operating voltage and electronic threshold variation to reach the best counting conditions. Therefore, a more general method for the determination of the optimum counting conditions in ZnS(Ag) scintillation detectors is proposed. In this method, a relationship between voltage and electronic threshold is derived for counting efficiency. In order to test the method, quality control procedures have been carried out as well as the determination of gross alpha activity in environmental samples.