Vertical inventories and fluxes of <Superscript>210</Superscript>Pb, <Superscript>228</Superscript>Ra and <Superscript>226</Superscript>Ra at southern South China Sea and Malacca Straits

Inventories and fluxes of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were determined in sediment cores collected at nine stations covering of the southern South China Sea and Malacca Straits with the thickness of water column between 42 and 83 m depth. The inventories of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were calculated range from 0.15–2.55 Bq cm⁻², 0.05–0.40 Bq cm⁻² and 6.83–83.63 Bq cm⁻², meanwhile the fluxes ranged from 0.005–0.079 Bq cm⁻² yr⁻¹, 0.009–0.048 Bq cm⁻² yr⁻¹ and 0.003–0.037 Bq cm⁻² yr⁻¹, respectively. The results show that the highest inventories and fluxes for ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra were found at station WC 01 and EC 05. Because there are additional sources of ²¹⁰Pb, ²²⁸Ra and ²²⁶Ra, where water transport will brings more dissolved isotopes, influence of the transportation and deposition of suspended particles, fast rate of regeneration and greater production of those radionuclides and others.     

Application of ICP-QMS for the determination of ultratrace-levels of <Superscript>226</Superscript>Ra in geothermal water and sediment samples

A rapid, accurate and less labor intensive approach to determining ²²⁶Ra in environmental samples was examined; this utilized quadrupole-based inductively coupled plasma mass spectrometry (ICP-QMS). The procedure used chemical separation by ion exchange chromatography to remove most of the matrices after coprecipitation with BaSO₄. The average chemical recovery of the NIST SRM preparation method ranged from 60.5 to 85.9% using ¹³³Ba as internal tracer by gamma counting. This technique was capable of completing a ²²⁶Ra measurement within 3 min. It did not require an in-growth period to allow radon and its progeny to achieve secular equilibrium with the parent ²²⁶Ra as is needed for liquid scintillation analyzer (LSA). The method detection limits for the determination of ²²⁶Ra in geothermal water and sediment samples were 0.02 mBq L⁻¹ (0.558 fg L⁻¹) and 0.10 Bq kg⁻¹ (2.79 fg g⁻¹), respectively. The results obtained with various natural samples and the suitability of the method when applied to various environmental matrices such as geothermal water and sediment are discussed. When ICP-QMS was compared to double-focusing magnetic sector field inductively coupled plasma mass spectrometry (ICP-SFMS), good agreement was obtained with a correlation coefficient, r ² = 0.982.     

<Superscript>224</Superscript>Ra and its implications in the East China Sea

The activities of ²²⁴Ra in the East China Sea (ECS) were measured by the Mn-fiber adsorption—emanation method. The horizontal and vertical distributions of ²²⁴Ra in the ECS in summer and winter were studied. The ranges of ²²⁴Ra activities were < lowest limit of detection (LLD)–5.88 Bq/m³ in summer with an average of 0.85 Bq/m³, and < LLD-7.50 Bq/m³ in winter with an average of 0.72 Bq/m³. And the distributions of ²²⁴Ra in the surface water were similar in these two seasons, decreasing rapidly with the increasing distance from the coast. The high ²²⁴Ra area was located within 30–100 km offshore and the lowest activities appeared in the Kuroshio Current. The vertical distributions of ²²⁴Ra showed two different characteristics. The horizontal and vertical eddy diffusion coefficients calculated by the one-dimensional state model of ²²⁴Ra were (7.1–88.9) × 10⁶cm²/s and 2.18–163 cm²/s, respectively. The upwelling rates off Zhejiang Province were calculated from ²²⁴Ra vertical distribution, which varied from 8.4 × 10⁻³cm/s to 13.3 × 10⁻³cm/s in summer and 16.3 × 10⁻³cm/s to 16.8 × 10⁻³cm/s in winter.     

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.     

Vertical distribution of <Superscript>210</Superscript>Pb and <Superscript>226</Superscript>Ra and their activity ratio in marine sediment core of the East Malaysia coastal waters

Marine sediment cores were collected from two stations at East Malaysia coastal waters on June 2004. Activity concentrations of ²¹⁰Pb in sediment core were ranged from 11 Bqkg⁻¹ to 84 Bqkg⁻¹ dry wt. for SR 01 and 4 Bqkg⁻¹ to 66 Bqkg⁻¹ dry wt. for SB 03. Meanwhile, activity concentrations of ²²⁶Ra in sediment core were varied significantly depending on the sampling location of SR 01 and SB 03 with ranged 17–26 Bqkg⁻¹ dry wt. and 8–11 Bqkg⁻¹ dry wt., respectively. The activity ratios of ²¹⁰Pb/²²⁶Ra were no significantly different at all sampling stations with an average of 1.78. Refer to the entire results; the activities of ²¹⁰Pb and ²²⁶Ra were higher at station SR 01 than station SB 03, but contrast with ratio of ²¹⁰Pb/²²⁶Ra. The reasons of different ²¹⁰Pb and ²²⁶Ra activity concentration and distribution of their ratios were strictly related to their half lives, environment origin, potential sources and behavior.     

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.     

Low level detection of <Superscript>135</Superscript>Cs and <Superscript>137</Superscript>Cs in environmental samples by ICP-MS

The measurement of fission product cesium isotopes ¹³⁵Cs and ¹³⁷Cs at low femtogram (fg) 10⁻¹⁵ levels in ground water by Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) is reported. To eliminate the natural barium isobaric interference on the cesium isotopes, in-line chromatographic separation of the cesium from barium was performed followed by high sensitivity ICP-MS analysis. A high efficiency desolvating nebulizer system was employed to maximize ICP-MS sensitivity ~10 cps/fg. The three sigma detection limit for ¹³⁵Cs was 2 fg/mL (0.1 μBq/mL) and for ¹³⁷Cs 0.9 fg/mL (0.0027 Bq/mL) measured from the standard with analysis time of less than 30 min/sample. Cesium detection and 135/137 isotope ratio measurement at very low femtogram levels using this method in a spiked ground water matrix is also demonstrated.     

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.     

Measurement of <Superscript>228</Superscript>Ra in the Yellow Sea and East China Sea using the radon emanation method

²²⁸Ra levels in the Yellow Sea and East China Sea were determined using the emanation method. The seawater radium was concentrated using an Mn-fiber and the ²²⁴Ra ingrowth was measured after about half a year when the initial ²²⁴Ra in the sample would have decayed. The ²²⁴Ra activity in the sample was evaluated using the decay dynamics relationship between parent ²²⁸Ra and daughter ²²⁸Th. The concentration and distribution feature of ²²⁸Ra in the Yellow Sea and East China Sea were studied and the ²²⁸Ra concentrations in the surface seawater of the Yellow Sea and the East China Sea were in the range 0.09–15.0 Bq/m³ with an average of 6.84 Bq/m³ during the summer cruise, and in the range 0.09–16.9 Bq/m³ with an average of 6.37 Bq/m³ during the winter cruise. The ²²⁸Ra distribution in the northern Yellow Sea was different from the southern Yellow Sea and East China Sea. The highest ²²⁸Ra activity of surface water was located in the middle of the northern Yellow Sea, but for the southern Yellow Sea and East China Sea, it decreased with increasing distance from China continent.     

Influence of the physico-chemical properties of Selangor soil series on the distribution coefficient (<Emphasis Type="Italic">K</Emphasis><Subscript>d</Subscript>-value) of <Superscript>226</Superscript>Ra

²²⁶Ra is a member of the ²³⁸U natural decay series and is one of the most important isotope to be determined among the naturally occurring nuclides in environmental samples. In order to evaluate the radiation dose from ²²⁶Ra, it is important to know its mobility in different types of soils. The aim of the present study is to quantify the influence of physico-chemical soil properties on ²²⁶Ra adsorption. The distribution coefficients (K _d-value) of ²²⁶Ra in Selangor soil series samples were measured in one core, at three depth levels to evaluate the adsorbability of ²²⁶Ra. The soil samples were spiked with ²²⁶Ra tracer and the activities of ²²⁶Ra in the separated phase from batch sorption test were measured by a low background but high efficiency well-type HPGe detector. Several physico-chemical soil properties were also characterised for each soil samples. Pearson’s correlation and stepwise multiple regression test were applied at the 0.05 level of significance throughout all analysis to determine the relationships and influences between distribution coefficients (K _d-value) of ²²⁶Ra with physicochemical soil properties for the Selangor soil series. The observed K _d value was in the range of 50.55–172.28 mL g⁻¹ (mean: 93.20 ± 46.99 mL g⁻¹). The regression showed that the highest positive correlations were observed for organic matter (OM) and cation exchange capacity (CEC) (r = 0.96**, 0.81**, respectively) with K _d-values. The results indicate that the stepwise multiple regression model incorporating the soil’s OM and CEC accounts for 98% of the variability in distribution coefficients of ²²⁶Ra.     

<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.     

Radium isotopes and <Superscript>222</Superscript>Rn in Austrian drinking waters

The activity concentrations of the Ra isotopes, ²²⁶Ra and ²²⁸Ra, as well as of ²²²Rn were measured in Austrian tap waters. Rn was extracted into a mineral oil cocktail not miscible with water and measured by liquid scintillation counting using pulse-shape analysis for α/β-separation. Ra isotopes were co-precipitated with BaSO₄ or concentrated by filtration through an element specific filter. EDTA solution was used to redissolve the precipitate as well as to release the Ra from the filter. After mixing with a cocktail, the EDTA solution was measured by liquid scintillation counting, too. From our results the effective ingestion doses for adults and 3 months old babies were calculated.     

The concentration of <Superscript>238</Superscript>U and the levels of gross radioactivity in surface waters of the Van Lake (Turkey)

Gross α and gross β activities and ²³⁸U concentrations were determined in 18 surface water samples collected from Van Lake. The instrumentations used to count the gross α and gross β activities and to determine the ²³⁸U concentrations were α/β counter of the multi-detector low background system (PIC-MPC-9604) and Inductively Coupled Plasma-Mass Spectrometry (Thermo Scientific Element 2), respectively. Concentrations ranging from 0.001 to 0.021 Bq L⁻¹ and from 0.111 to 2.794 Bq L⁻¹ were observed for the gross α and β activities in surface waters, respectively. For all samples the gross β activities were higher than the corresponding gross α activities. The results indicated that the gross α radioactive contamination in water samples was lower than recommended values for the guideline of drinking waters and most of the gross β activities in water samples were higher than those in the same procedure. The ²³⁸U concentrations ranged from 74.49 to 113.2 μg L⁻¹ in surface waters. The obtained results have showed that ²³⁸U concentrations are higher than guideline values for uranium.     

Effects of La<Superscript>3+</Superscript> and Eu<Superscript>3+</Superscript> on outward potassium channels in Vicia guard cells

Effects of La³⁺ and Eu³⁺ on outward potassium channels (K_out⁺) in Vicia guard cells have been studied by patch clamping technique. Extracellular La³⁺ inhibited K_out⁺ currents with a half-inhibition concentration (IC₅₀) of 81 μmol·L⁻¹. Interestingly, intracellular La³⁺ activated K_out⁺ currents at a free concentration of 1.13 × 10⁻¹⁴ mol·L⁻¹, and inhibited K_out⁺ currents at a free concentration of 5.86 × 10⁻¹⁴ mol·L⁻¹. Extracellular Eu³⁺ also activated K_out⁺ currents at concentrations of 10 μmol·L⁻¹ and 50 μmol·L⁻¹, and inhibited K_out⁺ currents at concentrations of more than 1 mmol·L⁻¹. The effects of La³⁺ and Eu³⁺ on K_out⁺ currents may contribute to regulation of the plant water status, which may be one of the mechanisms of the biological effect of rare earth elements.     

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.     

Separation of strontium from calcium by the use of sodium hydroxide and its application for the determination of long-term background activity concentrations of <Superscript>90</Superscript>Sr in 100 km area around Kozloduy Nuclear Power Plant (Bulgaria)

The method for the determination of ⁹⁰Sr which employs sodium hydroxide for the separation of strontium from calcium was further improved introducing the use of elevated temperatures. The results from 11-year study of background activity concentrations of ⁹⁰Sr in different environmental objects in 100 km zone around Kozloduy Nuclear Power Plant (Bulgaria) are presented as an application of the analytical method. The measured mean values are as follows: air precipitation − 0.0015±0.0009 Bq(m^2.d), tap water − 0.0017±0.0012 Bq/L, soil − 1.90±1.26 Bq/kg, grass − 1.54±0.80 Bq/kg, milk − 0.023±0.012 Bq/L and for the Danube river: water − 0.0046±0.0026 Bq/L, bottom sediments − 0.64±0.60 Bq/kg, algae − 1.99±1.56 Bq/kg. The calculated transfer coefficients (soil-grass) are in the range of 0.33–0.84. Between 2 and 5 times reduction in actual background activities of ⁹⁰Sr is observed compared to 1972–1974.     

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.     

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.     

Levels of <Superscript>232</Superscript>Th activity in the South Adriatic Sea marine environment of Montenegro

²³²Th activities in the South Adriatic Sea-water, surface sediment, mud with detritus, seagrass (Posidonia oceanica) samples, and the mullet (Mugilidae) species Mugil cephalus, as well as soil and sand from the Montenegrin Coast, were measured using the six-crystal spectrometer PRIPYAT-2M, which has relatively high detection efficiency and a good sensitivity, and allows a short acquisition time, and measuring samples of any shape, without preliminary preparation and calibration measurements for different sample geometries. An average ²³²Th activity concentration in surface soil layer is found to be 40.33 Bq kg⁻¹, while in sand—4.7 Bq kg⁻¹. The absorbed dose rate in air due to ²³²Th gamma radiation from surface soil layer ranged from 11.76 to 63.39 nGy h⁻¹, with a mean of 24.06 nGy h⁻¹. Corresponding average annual effective dose rate has been found to be 0.03 mSv y⁻¹. The absorbed dose rates due to the thorium gamma radiation in air at 1 m above sand surface on the Montenegrin beaches have been found to be from 0.41 to 9.08 nGy h⁻¹, while annual effective dose rates ranged from 0.0005 to 0.011 mSv y⁻¹. ²³²Th activity concentration in seawater ranged from 0.06 to 0.22 Bq L⁻¹, as in the mullet (Mugil cephalus) whole individuals from 0.63 to 1.67 Bq kg⁻¹. Annual intake of ²³²Th by human consumers of this fish species has been estimated to provide an effective dose of about 0.003 mSv y⁻¹.     

An accurate method for the determination of <Superscript>226</Superscript>Ra activity concentrations in soil

A quantitative method to determine the activity concentration of ²²⁶Ra in soil samples was established using high performance environmental gamma-ray spectrometry. In this method, a semi-empirical calibration procedure was developed for full energy peak efficiency calculation utilizing the elemental composition of the soil sample. Aatami software was used to deconvolute the ²³⁵U and ²²⁶Ra doublet at 185.7 keV and 186.2 keV, respectively, and to fit the baseline of the soil gamma-spectrum for the determination of ²²⁶Ra activity. The results indicated that the Aatami doublet deconvolution procedure provides a rapid and accurate analysis of a complicated spectrum in comparison with other cumbersome spectral interference correction methods. The study also compared the results with those obtained by radon progeny (²¹⁴Pb, or ²¹⁴Bi) measurements and found that the deconvolution method provided a more accurate ²²⁶Ra activity as it is independent of the error caused by radon diffusion. This error can be quite large since the amount of escaped radon gas through the sample container walls and sealing cannot be accurately quantified.