<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.     

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.     

Analysing of <Superscript>228</Superscript>Th, <Superscript>232</Superscript>Th, <Superscript>228</Superscript>Ra in human bone tissues for the purpose of determining the post mortal interval

The adsorption of Cs on clayey materials such as bentonite and Na-montmorillonite was studied in various electrolytic conditions (concentration and composition), various solid to liquid ratios and various pH conditions. The results obtained for these different conditions were modeled considering an exchange model associated to the surface complexation concept. Then, the same approach was considered to model the sorption of Rb, which have the same chemical behavior than Cs. Experiments were carried out for various electrolyte, pH, and Rb concentrations. The stoichiometries corresponding to the sorption of Rb on bentonite and montmorillonite were then deduced from the experimental results.     

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.     

Determination and differentiation of <Superscript>226</Superscript>Ra and <Superscript>222</Superscript>Rn by gamma-ray spectrometry in drinking water

The analysis of ²²⁶Ra in natural waters can be tedious and time-consuming. For the determination and differentiation of activities of ²²⁶Ra and ²²²Rn in drinking water by γ-ray spectrometry a simple and fast method is presented. Activities of ²²⁶Ra > 0.5 Bq L⁻¹ can be determined according to stabilization of the sample without further procedures. For a more sensitive detection sample volumes of up to 5 litres are applicable by a rapid precipitation procedure without large expenditure. Further laborious enrichment methods are not necessary. Thus, detection limits of 0.1 Bq L⁻¹ can be obtained when using sample volumes of 5 litres. Therefore the method is suitable for the monitoring of radioactivity in drinking water samples in accordance with the legal guidance of the European Union.     

Determination of <Superscript>228</Superscript>Ra in human bone ash containing significant quantities of <Superscript>40</Superscript>K and Ca<Superscript>2+</Superscript>

The determination of ²²⁸Ra by means of γ-spectrometry, in material containing significant quantities of ⁴⁰K and Ca²⁺ such as bone ash results in increased values of counting uncertainty and lower limit of detection (LLD) because of a significant contribution from the Compton continuum of ⁴⁰K. However, ⁴⁰K is widely removed from bone ash if ²²⁸Ra is coprecipitated with barium sulfate. As a result, the counting uncertainty and LLD are significantly reduced. A method is presented for determination of very low activity concentrations of ²²⁸Ra. Impurities introduced by precipitation are negligible when applying high resolution γ-spectrometry.     

Determination of <Superscript>40</Superscript>K, <Superscript>226</Superscript>Ra and <Superscript>232</Superscript>Th concentration and radiation dose assessment in titanium enamel frits use in polishing household utensils in Ghana

As part of monitoring the exposure of the Ghanaian public to natural radioactivity, radioactivity concentrations in titanium enamel frits use for coating, spraying and decorating steel bowls were investigated. Samples collected from Ghana Utensil Manufacturing Company in Ghana were analyzed using γ-ray spectrometry with a high purity germanium detector. The samples were found to contain an average absorbed dose rate of 509.38 nGy h⁻¹, while an average annual effective dose was calculated to be 2.50 mSv.     

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.     

Measuring <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K and decay products of <Superscript>226</Superscript>Ra and <Superscript>232</Superscript>Th in samples of different nature by a multidetector spectrometer

A coincidence method for measuring ¹³⁷Cs, ⁴⁰K, ²²⁶Ra and ²³²Th decay products activity in soil, vegetation and fish samples, was applied to the six-crystal gamma-coincidence spectrometer PRIPYAT-2M. In this way, some problems appeared in simultaneous measurement of ¹³⁷Cs, ²²⁶Ra and ²³²Th by NaI(Tl) detectors and the PRIPYAT-2M spectrometer were solved. The obtained results were agreeable with the HPGe spectrometer ones.     

The apparent change of activity with temperature in a <Superscript>226</Superscript>Ra decay chain

Radioactive decay rates are to a large extent believed to be independent of the chemical environment. This is the physics basis implicitly assumed in applications such as radioisotope dating. While this statement is a good approximation for most radioactive decays, there are cases where a slight variation of 0.5% or more can be observed, as in the electron capture type of decay. There are renewed interests in possible decay-rate changes with external parameters such as temperature, with controversy as to the phenomenon’s authenticity. In this paper, we study the variation of radioactivity counts that significantly change (up to 50% or more) with temperature. We carefully studied the characteristics of the change and found that the presence of a gaseous decay daughter can pose a serious challenge to a bona fide account of the intrinsic nuclear decay rate. After a careful solution to rate equations of the relevant isotopes under our experimental conditions, we found that most of the radioactivity change could be accounted for by the diffusion and loss of gaseous daughters under the heat, without a supposed change in the intrinsic nuclear decay rate. We hence demonstrate that an accurate determination of the decay constant has to consider the possible diffusion of volatile components in the decay chain. This is especially important in cases involving significant temperature change.     

Distribution of <Superscript>14</Superscript>C, <Superscript>90</Superscript>Sr and <Superscript>228</Superscript>Th in an elephant tusk

The period of date of death of an elephant can be assessed by analyzing four different radionuclides, ¹⁴C, ⁹⁰Sr, ²²⁸Th and ²³²Th in its ivory. These nuclides are supposed to have variing concentrations at different parts of a tusk. The reason is the procedure of growth which takes place at the butt-site of a tusk. Therefore the site of sampling could have a big influence on the assessed date of death. However, to find out if the position of sampling is important a complete tusk was analyzed regarding the distribution of these nuclides. Results show that the concentration activity of ¹⁴C and ²²⁸Th varies in different parts of a tusk. The activity concentration of ⁹⁰Sr is very similar in all analyzed parts. The conclusion is that sampling at the butt of a tusk is recommended for age assessment.     

Sequential radioanalytical method for the determination of U and Th isotopes, <Superscript>226</Superscript>Ra and <Superscript>210</Superscript>Po using alpha spectrometry in samples of the Brazilian phosphate industry

The phosphate rocks used for the production of phosphate fertilizers present in their composition radionuclides of the U and Th series. During the chemical attack, the radionuclides are distributed to final products and phosphogypsum. A sequential radiochemical procedure was implemented to determine the content of radionuclides alpha emitters in samples of fertilizers and phosphogypsum produced in Brazil. The results obtained show that the levels of radioactivity present in the fertilizers are of the same order of magnitude on those found in the phosphogypsum, reaching values up to 1158 and 457 Bq kg⁻¹, for the U and Th series, respectively.     

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.     

Determination of <Superscript>226</Superscript>Ra in sediments by ICP-MS: A comparative study of three sample preparation approaches

Three protocols (Method I: ion chromatography (IC) and extraction chromatography (EC), Method II: precipitation followed by IC, and Method III: adsorption onto MnO₂ followed by IC-EC) were investigated to determine their applicability for the separation and pre-concentration of ²²⁶Ra in sediments. ²²⁶Ra recoveries, measured using the isotope dilution method with ²²⁸Ra as yield tracer, and the removal of spectral and non-spectral interferences were evaluated. The formation of polyatomic interferences at m/z = 226 from elements found in the matrix of sediments was also investigated to assess the level of separation required. Methods I and III were found to be the most effective with respect to recoveries and interference removal. The efficiency of a rapid microwave based protocol for the complete digestion of 1 g of sediment is also described. The method was tested and ²²⁶Ra concentrations in the millibecquerel range (fg) were determined in a standard reference material and sediment cores collected from Lake Baikal.     

Modeling of <Superscript>226</Superscript>Ra behavior in a Spanish estuary affected by the phosphate industry

The Odiel and Tinto rivers, southwest Spain, form a fully mixed estuary. An industrial area that includes a complex dedicated to the production of phosphate fertilizers is located by the Odiel River. This complex released phosphogypsum wastes directly to the Odiel River and also disposed them on open air piles located by the Tinto River. Due to new EU regulations, wastes are not directly released to the Odiel from 1998 on, although they are still disposed on the open air piles. The behavior of ²²⁶Ra in a system like this estuary is complex, since radionuclides are affected by tidal actions and interactions with sediments through adsorption/desorption reactions and erosion/deposition processes. A numerical 2D depth-averaged model of the estuary has been developed, including processes mentioned above. It has been applied to reproduce experimental data measured after a release from the industrial complex in the Odiel River and after an accidental release in the Tinto River from the gypsum piles. The model has also been applied to simulate the self-cleaning process observed in the estuary after the direct releases from the fertilizer complex were stopped.     

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.     

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.     

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.