Radiological assessment of natural and fallout radioactivity in the soil of Chamba and Dharamshala areas of Himachal Pradesh,India

This paper presents the results of measurement of natural and fallout radioactivity in soil samples of Chamba and Dharamshala areas in Himachal Pradesh, India. Spatial distribution of ²³⁸U, ²²⁶Ra, ²³²Th, ⁴⁰K, ¹³⁷Cs was determined using High resolution gamma-ray spectrometry. The mean activity concentration in Chamba region due to ²³⁸U, ²³²Th, ⁴⁰K and ¹³⁷Cs was 32.3, 58.4, 588.3, and 10.9 Bq kg⁻¹, respectively, whereas in Dharamshala it was 35.7, 61.3, 594.9, 10.0 Bq kg⁻¹, respectively. Absorbed gamma dose rate (D) in air was calculated using appropriate dose conversion factors, which was varying from 45 to 103 nGy h⁻¹. To control the radiation exposure due to natural radioactivity in soil, if it is used as building materials, radium equivalent activity (Ra_eq) and activity index were also evaluated. Radium equivalent activity calculated for the soil ranged from 95.5 to 234.2 Bq kg⁻¹ with average of 171.0 Bq kg⁻¹.The calculated Activity concentration index was ranged from 0.34 to 0.85 with an average value of 0.64. The natural and fallout radioactivity in soil of this region is comparable with Indian average and other parts of the world. The percentage contribution of ²³⁸U, ²³²Th and ⁴⁰K and ¹³⁷Cs to the average external gamma dose rate was 22, 46, 32, 2%, respectively. This shows that the dose contribution due to fallout radioactivity is negligible as compared to the natural radioactivity.     

Assessment of natural radioactivity in silt samples from Moticher lake near Kakrapar Atomic Power Station,India

The naturally occurring radioisotopes such as ²³⁸U, ²³²Th and ⁴⁰K in the silt samples collected from Moticher lake, Gujarat were evaluated. The activity of ²³⁸U, ²³²Th and ⁴⁰K was found to be 4.4-9.7 Bq kg⁻¹ with a mean 6.4 ± 1.3 Bq kg⁻¹, 10.5–21.2 Bq kg⁻¹ with a mean 15.6 ± 2.5 Bq kg⁻¹ and 102–231 Bq kg⁻¹ with a mean 160 ± 40 Bq kg⁻¹, respectively. The depth profile study could not reveal any significant vertical correlation on radioactivity levels of ²³⁸U, ²³²Th and ⁴⁰K. Radium equivalent activity (Ra_eq), external hazard index (H _ex) and internal hazard index (H _int) were calculated by using the activity of ²³⁸U or ²²⁶Ra, ²³²Th and ⁴⁰K in silt samples. Annual Effective Dose Equivalent (AEDE) level in Moticher silt was found to be 24.8 ± 5.0 μSv year⁻¹, which is much lower than the worldwide average value. The relative contribution to dose due to ²³⁸U and ²³²Th series were found to be 14% and 53%, followed by the contribution of 33% due to ⁴⁰K.     

Determination of uranium isotopic composition and 236U content of soil samples and hot particles using inductively coupled plasma mass spectrometry

As a result of the accident at the Chernobyl nuclear power plant (NPP) the environment was contaminated with spent nuclear fuel. The ²³⁶U isotope was used in this study to monitor the spent uranium from nuclear fallout in soil samples collected in the vicinity of the Chernobyl NPP. Nuclear track radiography was applied for the identification and extraction of hot radioactive particles from soil samples. A rapid and sensitive analytical procedure was developed for uranium isotopic ratio measurement in environmental samples based on double-focusing inductively coupled plasma mass spectrometry (DF–ICP–MS) with a MicroMist nebulizer and a direct injection high-efficiency nebulizer (DIHEN). The performance of the DF–ICP–MS with a quartz DIHEN and plasma shielded torch was studied. Overall detection efficiencies of 4×10^–4 and 10^–3 counts per atom were achieved for ²³⁸U in DF–ICP–QMS with the MicroMist nebulizer and DIHEN, respectively. The rate of formation of uranium hydride ions UH⁺/U⁺ was 1.2×10^–4 and 1.4×10^–4, respectively. The precision of short-term measurements of uranium isotopic ratios (n = 5) in 1 μg L^–1 NBS U-020 standard solution was 0.11% (²³⁸U/²³⁵U) and 1.4% (²³⁶U/²³⁸U) using a MicroMist nebulizer and 0.25% (²³⁵U/²³⁸U) and 1.9% (²³⁶U/²³⁸U) using a DIHEN. The isotopic composition of all investigated Chernobyl soil samples differed from those of natural uranium; i.e. in these samples the ²³⁶U/²³⁸U ratio ranged from 10^–5 to 10^–3. Results obtained with ICP–MS, α- and γ-spectrometry showed differences in the migration properties of spent uranium, plutonium, and americium. The isotopic ratio of uranium was also measured in hot particles extracted from soil samples.     

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.     

Determination of plutonium and americium in environmental samples by inductively coupled plasma sector field mass spectrometry and alpha spectrometry

Application of inductively coupled plasma sector field mass spectrometry (ICP-SFMS) for the determination of americium and plutonium in environmental samples is described in comparison with alpha spectrometry. A sequential sample preparation method was employed using a co-precipitation step for pre-concentration and a separation step applying extraction chromatographic resins. The average recovery of sample preparation calculated from the concentration of the tracer before and after sample treatment was better than 80%. The method development focused on the elimination of possible interferences in mass spectrometric analysis caused by molecular ions (e.g. ²⁰⁰Hg⁴⁰Ar⁺, ²⁰⁴Pb³⁶Ar⁺, ²⁰⁸Pb¹⁶O₂⁺or ²³⁸U¹H⁺) employing matrix separation and desolvation prior to ICP-SFMS analysis. The effect of N₂ gas on signal intensity and oxide ratio was investigated. A two-fold signal improvement was obtained by adding 5 ml min^− 1 N₂ to the sample gas after the desolvation system. For ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu and ²⁴¹Am limit of detection (LOD) of 15, 9.2, 14 and 104 fg g^− 1 was achieved, respectively. Calculation of LOD was based on three times standard deviation of the method blank solution. Absolute detection limit was calculated to be 10-25 fg. For all investigated actinides the precision of the analysis was in the range 0.8-3% relative standard deviation. Results from the analysis of certified reference materials (IAEA-384 and IAEA-385) showed good agreement with recommended values and data available in the literature. The method was applied for analysis of environmental samples originated from Chernobyl and from Mayak region. The possibility of the determination of the origin and date of pollution was demonstrated using isotopic data obtained by ICP-SFMS and alpha spectrometry.     

Distribution of <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K, <Superscript>232</Superscript>Th and <Superscript>238</Superscript>U in coastal marine sediments of Margarita Island,Venezuela

This work presents the results of ¹³⁷Cs, ⁴⁰K, ²³²Th and ²³⁸U concentration (Bq kg⁻¹) values in coastal marine sediments collected from 38 sites along the coastline of the island of Margarita, Venezuela. The purpose was to determine baseline values for these radionuclides in surface marine sediments and to detect if there were any anomalously high concentration values. Only three of the 38 sediments analyzed had measurable values above the detection limit of 0.9 Bq kg⁻¹ for ¹³⁷Cs and the highest only being 1.4 Bq kg⁻¹. While, the concentration (Bq kg⁻¹) ranges for the primordial radionuclides, ⁴⁰K, ²³²Th and ²³⁸U were as follows: 12.2–211.7, <1.5–9.8 and <4.4–20.7, respectively. These concentration ranges for the primordial radionuclides can be considered as baseline values for surface marine sediments for areas that are considered not polluted by man or contaminated by nature. Finally, the concentration range of ¹³⁷Cs can also be employed as baseline values, which only seem to have been the result of the atmospheric testing of nuclear weapons in the past.     

Determination of naturally occurring radionuclides in selected rocks from Hetaunda area,central Nepal

The specific activities of the naturally occurring radionuclides ²³⁸U, ²³²Th, and ⁴⁰K were measured in rock samples from the Hetaunda area, central Nepal, using gamma spectrometry. The specific activities were found to be in the range of 17–95 Bq kg⁻¹ for ²³⁸U, 24–260 Bq kg⁻¹ for ²³²Th and 32–541 Bq kg⁻¹ for ⁴⁰K. From these data absorbed dose rates in air and annual effective doses were calculated and compared with respective data from the UNSCEAR compilation. The results from our study open the door to the safe applicability of most of the investigated materials as a cheep building material.     

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.     

Long-Lived Radionuclides in Sea Sediments Around Kashiwazaki-Kariwa Nuclear Power Station

Natural and artificial radionuclide concentrations in sea sediments around Kashiwazaki-Kariwa nuclear power station have been investigated with respect to the particle size distributions and the ignition losses during assay. Plutonium concentrations around the south and north discharge area, ranged from 0.054 to 0.24 Bq·kg^-1 (average 0.145) and 0.15 to 0.25 Bq·kg^-1 (average 0.213), respectively. Plutonium concentrations were significantly related to erosion and accumulation processes of sediments in both south and north discharges. Additionally, the ratios of ²³⁹Pu to ²⁴⁰Pu were evaluated with ICP-MS to determine the origin of the Pu-isotopes. Uranium-238, ²³²Th and ⁴⁰K were found in concentration range of 7.3–67, 12–100 and 260–560 Bq·kg^-1 with mean concentrations of 20, 29 and 390 Bq·kg^-1, respectively. It is assumed that the relatively high concentrations of the natural radionuclides such as U and Th are due to the presence of minerals (the south discharge regions). On the basis of these results, the origin of the Pu-isotopes was assumed to be derived from fallout of the past atmospheric nuclear tests.     

Estimation of daily uranium ingestion by urban residents in Japan

125 types of food were collected mainly from Yokohama City which is one of the typical urban cities in Japan. The samples, were divided into the 18 food categories in the report of the National Nutrition Survey (NNS),¹ were analysed for uranium by -spectrometry after chemical separation. Concentrations of²³⁸U in individual types of food ranged from 9.85·10^–5 Bq·kg^–1 in grain vinegar to 5.90 Bq·kg^–1 in boiled and dried hijiki. The median value of²³⁸U was found to be 4.83·10^–3 Bq·kg^–1 on a raw weight basis. The daily intake of²³⁸U per person by ingestion was estimated to be approximately 14 mBq with more than 50% of it coming from marine products.     

Determination of U/U atom ratio in uranium samples using liquid scintillation counting (LSC)

A correlation has been developed for the determination of ²³⁵U/²³⁸U atom ratio in uranium samples using liquid scintillation counting (LSC). The ²³⁵U/²³⁸U atom ratio determined by thermal ionization mass spectrometry (TIMS) was correlated to the ratio of (i) α-count rate and (ii) Cerenkov count rate due to ^234mPa in the sample; both measured by LSC. This correlation is linear over the range of ²³⁵U/²³⁸U atom ratio encountered in the nuclear fuel samples, i.e. the low enriched uranium (LEU) samples with ²³⁵U < 20 atom%. The methodology based on this correlation will be useful for the quick determination and verification of ²³⁵U/²³⁸U atom ratios in fuel samples using cost effective technique of LSC.     

Recombination of HCO and DCO ions with electrons

Recombination of HCO⁺ and DCO⁺ ions with electrons was studied in afterglow plasma. The flowing afterglow with Langmuir probe (FALP) apparatus was used to measure the recombination rate coefficients and their temperature dependencies in the range 150–270 K. To obtain a recombination rate coefficient for a particular ion, the dependencies on partial pressures of gases used in the ion formation were measured. The variations of α_HCO⁺(T) and α_DCO⁺(T) seem to obey the power law: α_HCO⁺(T) = (2.0 ± 0.6) × 10⁻⁷ (T/300)^−1.3 cm³ s⁻¹ and α_DCO⁺(T) = (1.7 ± 0.5) × 10⁻⁷ (T/300)^−1.1 cm³ s⁻¹ over the studied temperature range.     

An ultra-sensitive and colorimetric sensor for copper and iron based on glutathione-functionalized gold nanoclusters

Here, we report an ultra-sensitive and colorimetric sensor for the detection of Fe³⁺ or Cu²⁺ successively using glutathione-functionalized Au nanoclusters (GSH-AuNCs). For GSH-AuNCs can catalytically oxidize peroxidase substrates, such as 3, 3′, 5, 5′-tetramethylbenzidine (TMB), colored products are formed in the presence of H₂O₂. While upon the addition of Fe³⁺ or Cu²⁺ into the GSH-AuNCs-TMB-H₂O₂ system, diverse color and absorbance of the system was obtained due to the self oxidation of Fe³⁺ and the inhibition of peroxidase-like activity of GSH-AuNCs. With the introduction of ethylene diamine tetraacetic acid (EDTA) or ammonium fluoride (NH₄F) to GSH-AuNCs-TMB-H₂O₂+Cu²⁺ system or GSH-AuNCs-TMB-H₂O₂+Fe³⁺ system respectively, a restoration of color and absorbance of system was realized. On the basis of above phenomenon, a colorimetric and quantitative approach for detecting Fe³⁺ and Cu²⁺ was developed with detection limit of 1.25 × 10⁻⁹ M and 1.25 × 10⁻¹⁰ M respectively. Moreover, the concentration of Fe³⁺ and Cu²⁺ in human serums was also accurate quantified by this method. So this design strategy realized the simple and simultaneous detection of Fe³⁺ and Cu²⁺, suggesting significant potential in clinical diagnosis.     

Transfer of uranium and thorium from soil to different parts of medicinal plants using SSNTD

The uptake of ²³⁸U and ²³²Th in different parts of some selected plants used in traditional treatment of hypertension and diabetes in south-eastern Morocco (Errachidia area) has been studied using two different types of solid state nuclear track detectors (SSNTDs) LR-115 type II and CR-39. Plant uptake of radionuclides is one of many vectors for introduction of contaminants into the human food chain. Thus, it is critical to understand soil–plant relationships that control nuclide bioavailability. Soil concentrations of uranium ranged from 6.10 to 11.62 ppm, with a mean of 7.90 ppm. Soil concentrations of thorium ranged from 2.70 to 4.80 ppm, with a mean of 3.41 ppm. Mean uranium specific activities were 8.38 Bq kg⁻¹ in root tissue, 5 Bq kg⁻¹ in stem tissue and 6.02 Bq kg⁻¹ in leaf tissue. Mean thorium specific activities were 2.53 Bq kg⁻¹ in root tissue, 1.64 Bq kg⁻¹ in stem tissue and 1.96 Bq kg⁻¹ in leaf tissue. The transfer factors of ²³⁸U and ²³²Th from soil to different parts (root, stem, leaf, seed and fruit) of studied plant samples have been investigated. The transfer factors obtained for root plants were markedly higher than those for leaf, stem, fruit and seed plants. Soil-to-plant transfer factor (TF) is one of the most important parameters to be used in transfer models for predicting the concentration of radionuclides in agricultural crops and for estimating dose impacts to man. This study of uranium and thorium uptake in plants used in traditional medicine is also significant as far as the health hazard effects of uranium and thorium in human being are concerned.     

A dual-response fluorescent probe for Zn and Al detection in aqueous media: pH-dependent selectivity and practical application

A Schiff base-type fluorescent probe (1) consist of 2-hydroxynaphthaldehyde and glutamide moieties has been designed and synthesized for detection Zn²⁺ and Al³⁺. The probe shows pH dependent dual-selectivity for Zn²⁺ and Al³⁺ in Tris-HCl buffer, viz. that can selectively recognized Zn²⁺ at pH 7.4 and Al³⁺ at pH 6.0, respectively. From Job's plots and MS data, the stoichiometric ratios of the probe with Zn²⁺ and Al³⁺ appeared to be 1:1 and 2:1, respectively. The probe can detect as low as 5.5 × 10⁻⁸ M⁻¹ Zn²⁺ and 1.27 × 10⁻⁷ M⁻¹ Al³⁺, whereas respective association constants are 4.27 × 10⁴ M⁻¹ and 3.50 × 10⁹ M⁻¹. Furthermore, it is also confirmed that the probe has good cell-permeability and could thus be used to selectively sense intracellular Zn²⁺ and Al³⁺ by bioimaging in different pH environment. Finally the probe has been used successfully for determination of the analytes in real drug samples.     

Determination of Hg on poly(vinylferrocenium) (PVF)-modified platinum electrode

A new surface based on poly(vinylferrocenium) (PVF⁺)-modified platinum electrode was developed for determination of Hg²⁺ ions in aqueous solutions. The polymer was electrodeposited on platinum electrode by constant potential electrolysis as PVF⁺ClO₄⁻. Cl⁻ ions were then attached to the polymer matrix by anion exchange and the modified electrode was dipped into Hg²⁺ solution. Hg²⁺ was preconcentrated at the polymer matrix by adsorption and also complexation reaction with Cl⁻. Detection of Hg²⁺ was carried out by differential pulse anodic stripping voltammetry (DPASV) after reduction of Hg²⁺. Mercury ions as low as 5 × 10⁻¹⁰ M could be detected with the prepared electrode and the relative standard deviation was calculated as 6.35% at 1 × 10⁻⁶ M concentration (n = 6). Interferences of Ag⁺, Pb²⁺ and Fe³⁺ ions were also studied at two different concentration ratios with respect to Hg²⁺. The developed electrode was applied to the determination of Hg²⁺ in water samples.     

Construction of a new Cu2+ coated wire ion selective electrode based on 2-((2-(2-(2-(2-hydroxy-5-methoxybenzylidene amino)phenyl)disufanyl)phenylimino)methyl)-4-methoxyphenol Schiff base

In this article a new coated platinum Cu²⁺ ion selective electrode based on 2-((2-(2-(2-(2-hydroxy-5-methoxybenzylideneamino)phenyl)disufanyl)phenylimino) methyl)-4-methoxyphenol Schiff base (L₁) as a new ionophore is described. This sensor has a wide linear range of concentration (1.2 × 10⁻⁷-1.0 × 10⁻¹ mol L⁻¹) and a low detection limit of 9.8 × 10⁻⁸ mol L⁻¹of Cu(NO₃)₂. It has a Nernstian response with slope of 29.54 ± 1.62 mV decade⁻¹ and it is applicable in the pH range of 4.0-6.0 without any divergence in potentioal. The coated electrode has a short response time of approximately 9 s and is stable at least for 3.5 months. The electrode shows a good selectivity for Cu²⁺ ion toward a wide variety of metal ions. The proposed sensor was successfully applied for the determination of Cu²⁺ ion in different real and environmental samples and as indicator electrode for potentiometric titration of Cu²⁺ ion with EDTA.     

A new plastic scintillation resin for single-step separation,concentration and measurement of technetium-99

Technetium is a synthetic element with no stable isotopes, produced as waste in nuclear power plants and in cyclotrons used for nuclear medicine. The element has high mobility, in the form of TcO₄⁻; its determination is therefore important for environmental protection. Technetium is found in low concentrations and therefore common methods for its analysis include long treatments in several steps and require large amounts of reagents for its purification and preconcentration. Plastic scintillation resins (PSresin) are novel materials used to separate, preconcentrate and measure radionuclides in a single step. The objective of this study is to prepare and characterise a PSresin for the preconcentration and measurement of ⁹⁹Tc. The study first evaluates the reproducibility of the production of PSresins between batches and over time; showing good reproducibility and storage stability. Next, we studied the effect of some common non-radioactive interferences, showing small influences on measurement, and radioactive interferences (³⁶Cl and ²³⁸U/²³⁴U). ³⁶Cl can be removed by a simple treatment with 0.5 M HCl and ²³⁸U/²³⁴U can be removed from the column by cleaning with a mixture of 0.1 M HNO₃ and 0.1 M HF. In the latter case, a slight change in the morphology of the PSresin caused an increase in detection efficiency. Finally, the PSresin was applied to the measurement of real spiked samples (sea water and urine) with deviations lower than 10% in all cases.     

A study on 210Po activity concentration in soil at different depths along coastal Kerala

The paper presents systematic studies on the vertical profiles of ²¹⁰Po, an important decay product of ²³⁸U, in soils along coastal Kerala. Soil samples collected from different depth intervals 0–10, 10–20, 20–30 cm were analyzed for ²¹⁰Po activity concentration by radiochemical methods. The activity ²¹⁰Po in soil samples were counted using a ZnS(Ag) alpha scintillation counting system. The mean values of activity concentrations of ²¹⁰Po in soil of various depths were found to be 8.66, 5.63 and 4.95 Bq kg⁻¹ for depth intervals of 0–10, 10–20 and 20–30 cm, respectively. The overall activity concentration of ²¹⁰Po in soil was found to vary from 2.26 ± 0.19 to 14.02 ± 0.12 Bq kg⁻¹ with a mean value of 6.43 Bq kg⁻¹. Maximum activity concentration was found in soil samples of Kollam region with the mean value of 10.08 ± 0.92 Bq kg⁻¹. The activity of ²¹⁰Po was found to be comparatively high in surface soil. The variation of ²¹⁰Po activity concentration with organic matter contents was studied. ²¹⁰Polonium activity concentration was found to increase with increasing organic matter content.     

Deconvolution of liquid scintillation alpha spectra of mixtures of uranium and radium isotopes

A method for the determination of uranium and radium isotopes in water samples is proposed. Liquid scintillation techniques were used for collecting alpha spectra, which were then analyzed by fitting the alpha peaks with overlapping Gaussians. The analysis can quantify the observed isotopes with accuracy depending on the activity of each isotope.In order to simulate the peaks with Gaussian normal distribution functions, the centroid of each peak as well as the full width at half maximum (FWHM) are required, as they depend on the quenching of the sample. For this purpose, samples with known activities of ²²⁶Ra and its decay products and also of the uranium isotopes ²³⁸U and ²³⁴U, at various quenching levels, were used to establish the correlation of the peaks’ shift with the quench effect. In addition, the correlation of the FWHM with the centroid of a peak was determined, using the same procedure.Following the above analysis technique, an average of 97 ± 2% of detection efficiency and a lower limit of detection of 8.2 mBq kg⁻¹ for alpha isotopes were achieved.