Preparation of <Superscript>26</Superscript>Al, <Superscript>59</Superscript>Ni, <Superscript>44</Superscript>Ti, <Superscript>53</Superscript>Mn and <Superscript>60</Superscript>Fe from a proton irradiated copper beam dump

The station for pions cancer therapy was operated at PSI from 1980 to 1992. After a cooling time of 12 years it’s made of copper beam dump was cut and samples were taken for analytical purposes. The sampling collected about 500 g of high active copper chips that can be used for separation of exotic radionuclides. The analyses by gamma spectrometry, LSC and AMS showed main nuclides present to be ⁶⁰Co, ⁵⁴Mn, ²²Na, ⁶⁵Zn, ²⁶Al, ⁵³Mn, ⁵⁹Ni, ⁶³Ni, ⁵⁵Fe and ⁶⁰Fe and ⁴⁴Ti with a daughter nuclide ⁴⁴Sc. In the frame of ERAWAST project a procedure combining selective precipitation and ion exchange for the separation of the rare radionuclides from the copper beam dump was developed. The proposed separation procedure is easy for remote controlled implementation in a hot cell. The ion exchange separation of Ni, Al, Mg, Ti and Fe was complete and high decontamination factors for copper and cobalt were achieved. Based on the developed procedure a remotely controlled system for separation of exotic radionuclides from the copper chips was set up. The full scale system was installed in a hot cell where high activity levels can be handled. In order to evaluate the reliability and functionality of the system extensive tests have been done. During the test period 13.86 g in total of the proton irradiated copper beam dump were processed for separation of ²⁶Al, ⁵⁹Ni, ⁵³Mn, ⁴⁴Ti and ⁶⁰Fe. The results showed that the system was operational and the radionuclide separation was selective with high chemical yield. The procedure manages as well the generated liquid wastes containing high level of ⁶⁰Co activity.     

Sequential separation of <Superscript>99</Superscript>Tc, <Superscript>94</Superscript>Nb, <Superscript>55</Superscript>Fe, <Superscript>90</Superscript>Sr and <Superscript>59/63</Superscript>Ni from radioactive wastes

A sequential separation procedure has been developed for the determination of ⁹⁹Tc, ⁹⁴Nb, ⁵⁵Fe, ⁹⁰Sr and ^59/63Ni in various radioactive wastes generated from nuclear power plants. Ion exchange and extraction chromatography were adopted for individual separation of the radionuclides. Precipitation was supplementarily utilized for both purification of the individual radionuclides and preparation of the radionuclide sources for use in a radioactivity measurement. The chromatographic separation behavior of the radionuclides both from the sample matrix metals and from one another was investigated using stable metals, Re (as a surrogate of ⁹⁹Tc), Nb, Fe, Sr and Ni. The validity of the procedure for reliability and applicability was evaluated by measuring the recovery of the metal carriers added to synthetic radioactive waste solutions. The recoveries by the chromatographic separation were in the range of 84.8 to 102.2% with 2s of less than 8.6%, the recoveries by the precipitation being in the range of 84.3 to 97.3% with 2s of less than 10.9%.     

Modeling β-γ coincidence spectra of <Superscript>131m</Superscript>Xe, <Superscript>133</Superscript>Xe, <Superscript>133m</Superscript>Xe,and <Superscript>135</Superscript>Xe

In support of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), improvements have been made to the model of the Automated Radioxenon Sampler/Analyzer (ARSA) β-γ coincidence detector for radioxenon monitoring. MCNPX is used to simulate the detector response for all the electrons and photons emitted from ^131mXe, ¹³³Xe, ^133mXe, ¹³⁵Xe, and ¹³⁷Cs signals. A MatLab code was written to incorporate the MCNPX results in the calculation of β-γ coincidence spectra. These will aid in the development of the Spectral Deconvolution Analysis Tool (SDAT)¹ and to calibrate β-γ coincidence systems. The models developed for this work include improvements over previous models in their ability to address Compton scattering in the β-cell, and the β-distribution offset in the 31 keV γ-ray region for ¹³³Xe.     

Determination of activity ratios of <Superscript>238,239+240,241</Superscript>Pu, <Superscript>241</Superscript>Am, <Superscript>134,137</Superscript>Cs,and <Superscript>90</Superscript>Sr in Bulgarian soils

The origins of different artificial radionuclides found in soils from Northern and Southern Bulgaria was determined by measurements of their actual concentrations and respective ratios. On the basis of the measured mobility and concentrations of the investigated radionuclides in soils, it was estimated that after the Chernobyl accident the mean depositions of fresh ¹³⁷Cs were 3.0 ± 2.5 kBq/m² for Northern Bulgaria and 15 ± 7 kBq/m² for Southern Bulgaria. As a result of global fallout following atmospheric nuclear weapon tests in the 1950s, mean depositions (corrected to 1965) were calculated for Northern and Southern Bulgaria as follows: for ⁹⁰Sr—1.0 ± 0.5 and 2.3 ± 1.3 kBq/m², ²³⁸Pu—1.3 ± 0.8 and 2.8 ± 1.6 Bq/m², ^239+240Pu—15 ± 14 and 47 ± 38 Bq/m², and ²⁴¹Pu—520 ± 200 and 760 ± 260 Bq/m².     

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.     

Behavior of <Superscript>134</Superscript>Cs, <Superscript>90</Superscript>Sr,and <Superscript>238</Superscript>Pu in different Syrian soils

The experiment aimed to evaluate the vertical migration of ¹³⁴Cs, ⁹⁰Sr and ²³⁸Pu in the main types of Syrian soils; entisol, inceptisol, alluvial (rock outcrops) and gypsiferous soils, using soil columns through which the aqueous solution of the radionuclides percolated. The results show that the vertical migration of the studied radionuclides through the soil profile depend on the radionuclide and the soil type. More than 97% of ¹³⁴Cs and ²³⁸Pu concentrated in the upper 2 cm of the entisol, inceptisol, and alluvial soils, whereas only 46.2% to 68.6% of the ⁹⁰Sr was retained in the upper 2 cm of these soils. The vertical migration of the studied radionuclides in the gypsiferous soil was different from the other soils. The distribution of the radionuclides in the gypsiferous soil was irregular through the soil profile and reached the deeper layer of the soil. This may be due to its physical characteristics; poor structure stability, high permeability and low retention capacity.     

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.     

Atmospheric deposition fluxes of <Superscript>7</Superscript>Be, <Superscript>210</Superscript>Pb and <Superscript>210</Superscript>Po at Xiamen,China

The atmospheric deposition fluxes of ⁷Be, ²¹⁰Pb and ²¹⁰Po at Xiamen were measured. The samples were collected from March 2004 to April 2005 and the sampling period was one month. The ⁷Be and ²¹⁰Pb activity were measured using HPGe γ-spectrometer after concentration using Fe(OH)₃ co-precipitation method. The ²¹⁰Po was counted with an α-spectrometer after the sample was digested and spontaneous plated onto a silver planchet. At Xiamen, the atmospheric deposition fluxes of ⁷Be varied between 0.11 and 2.93 Bq·m⁻²·d⁻¹ and the average was 1.64 Bq·m⁻²·d⁻¹; ²¹⁰Pb fluxes varied between 0.04 and 0.85 Bq·m⁻²·d⁻¹, and the average was 0.51 Bq·m⁻²·d⁻¹; ²¹⁰Po fluxes varied between 0.002 and 0.133 Bq·m⁻²·d⁻¹, and the average was 0.061 Bq·m⁻²·d⁻¹. There were positive correlations between the deposition fluxes of ⁷Be, ²¹⁰Pb or ²¹⁰Po and the amount of precipitation. The residence time of aerosols varied between 6.0 and 54.0 days with a mean of 27.1 days, which were calculated by ²¹⁰Po/²¹⁰Pb fluxes ratios.     

Systematic radiochemical separation for the determination of <Superscript>99</Superscript>Tc, <Superscript>90</Superscript>Sr, <Superscript>94</Superscript>Nb, <Superscript>55</Superscript>Fe and <Superscript>59,63</Superscript>Ni in low and intermediate radioactive waste samples

A simple and rapid separation procedure was systemized for the determination of ⁹⁹Tc, ⁹⁰Sr, ⁹⁴Nb, ⁵⁵Fe and ^59,63Ni in low and intermediate level radioactive wastes. The integrated procedure involves precipitation, anion exchange and extraction chromatography for the separation and purification of individual radionuclide from sample matrix elements and from other radionuclides. After separating Re (as a surrogate of ⁹⁹Tc) on an anion change resin column, Sr, Nb, Fe and Ni were sequentially separated as follows; Sr was separated as Sr (Ca-oxalate) co-precipitates from Nb, Fe and Ni followed by purification using Sr-Spec extraction chromatographic resin. Nb was separated from Fe and Ni by anion exchange chromatography. Fe was separated from Ni by anion exchange chromatography. Ni was separated as Ni-dimethylglyoxime precipitates after the removal of ^134,137Cs and ^110mAg by Cs-phosphotungstate and AgCl precipitation, respectively. Finally, the radionuclide sources were prepared by precipitation for their radioactivity measurements. The reliability of the procedure was evaluated by measuring the recovery of chemical carriers added to a synthetic radioactive waste solution.     

Synthesis,Structure, and Keto-Enol Tautomerism of 3-R<Superscript>1</Superscript>-5,5-R<Superscript>2</Superscript>,R<Superscript>2</Superscript>-6-R<Superscript>3</Superscript>-2,3,5,6-Tetrahydropyran-2,4-diones

Ethyl esters of 2,4-dibromo-2-R¹-4-R²-3-oxopentanoic and -hexanoic acids react with zinc and aliphatic or aromatic aldehydes under the conditions of the Reformatskii reaction to give 3-R¹-5,5-R², R²-6-R³-2,3,5,6-tetrahydropyran-2,4-diones, which are obtained in three forms: keto, enol with enolization of the keto group, and enol with enolization of the ester group. The keto form is isolated by crystallization from a mixture of CCl₄ and petroleum ether; the first enol form, from MeOH, EtOH, and polar aprotic solvents; and the second enol form, from CHCl₃. The second enol form is oxidized in DMSO to form a keto compound containing a hydroxy group at the 3-position of the heteroring.     

Separation of <Superscript>133</Superscript>Xe from <Superscript>99</Superscript>Mo, <Superscript>131</Superscript>I and uranium,and removal of impurities using gas chromatography

Summary Separation and purification of ¹³³Xe from acidic solution containing uranium, ⁹⁹Mo and ¹³¹I has been developed. In the first step of this work, uranium pellets were dissolved under pressure (8-15 bar) in 8M nitric acid solution. Then¹³³ Xe and other gases were conducted to activated charcoal cold trap. Final purification of ¹³³Xe from impurities such as NO_x, radioiodine and krypton was performed by passing through a molecular sieve preparative chromatographic column using helium as mobile phase. The final recovery of ¹³³Xe from the separation-purification process was higher than 98%. Adsorption-desorption behavior of radioxenon on the charcoal and molecular sieves have also been studied and discussed.     

Study of <Superscript>239</Superscript>Pu, <Superscript>144</Superscript>Ce,and <Superscript>90</Superscript>Sr Behavior During Radioactive Wastes Treatment by Thermal Plasma Technology

A computer model is used to study the volatility of some radioelements (Cerium, Plutonium and Strontium) during radioactive wastes treatment by thermal plasma technology. This model is based on the calculation of system composition using the free enthalpy minimization method, coupled with the equation of mass transfer at the reactional interface. The model enables the determination of the effects of various parameters (e.g., temperature, plasma current, and presence of oxygen in the carrier gas) on the radioelement volatility. The obtained results indicate that any increase in molten bath temperature causes an increase in the radioelement volatility. It is also found that the oxygen flux in the carrier gas strengthens the radioelement incorporation in the containment matrix. For electrolyses effects, an increase in the plasma current increases both the vaporization speed and the vaporized quantities of ²³⁹Pu, ¹⁴⁴Ce, and ⁹⁰Sr.     

Diffusion mobility of alkali metals in perfluorinated sulfocationic and carboxylic membranes as probed by <Superscript>1</Superscript>H, <Superscript>7</Superscript>Li, <Superscript>23</Superscript>Na,and <Superscript>133</Superscript>Cs NMR spectroscopy

Water self-diffusion and ion mobilities in various ionic forms (H⁺, Li⁺, Na⁺, Rb⁺, Cs⁺, and Ba²⁺) of perfluorinated sulfocationic membranes MF-4SK were studied by NMR and impedance spectroscopy. When degrees of hydration are low, the self-diffusion coefficients of water and ionic conductivities are considerably affected by the water content of the membrane. The self-diffusion coefficients decrease in the order H⁺ > Ba²⁺ > Cs⁺ > Rb⁺ > Na⁺ > Li⁺, whereas the ion mobility decreases in the order H⁺ > Li⁺ > Na⁺ > Cs⁺ > Ba²⁺.     

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.     

European measurement comparison of <Superscript>137</Superscript>Cs, <Superscript>40</Superscript>K and <Superscript>90</Superscript>Sr in milk powder

Recently, the Institute for Reference Materials and Measurements (IRMM) has assumed responsibility for organizing regular measurement comparisons among those laboratories which provide radioactivity monitoring data from their country to authorities of the European Commission (EC) under various EC legislation articles. The most recent exercise under this International Comparison Scheme for Radioactivity Environmental Monitoring (ICS-REM) in measuring the ¹³⁷Cs, ⁴⁰K and the ⁹⁰Sr activity concentration in milk powder is presented here. The complete cycle of the comparison is described, including the establishment of reference values traceable to SI units, the demonstration of the homogeneity of the distributed samples, the treatment and measurement of samples in the participating laboratories, and the evaluation of the results.     

Structural features of acidic fluorophosphatozirconates (hafnates) from the <Superscript>19</Superscript>F, <Superscript>31</Superscript>P, <Superscript>1</Superscript>H NMR data

Fluorophosphatometallates with the composition K₃H₃Zr₃F₃(PO₄)₅, Rb₃H₃Zr₃F₃(PO₄)₅, Rb₃H₃Hf₃F₃(PO₄)₅, CsH₂Hf₂F₂(PO₄)₃?2H₂O are studied by ³¹P, ¹⁹F, and ¹H NMR. It is found that protons enter in the composition of hydrophosphate groups and fluorine atoms occupy the terminal sites in the tetravalent metal environment. Schemes of the crystal structure of fluorophosphatometallates are proposed. It is established that in CsH₂Hf₂F₂(PO₄)₃?2H₂O water molecules are bonded to the phosphate group proton via a strong hydrogen bond and are characterized by a low energy barrier of molecular motions.     

Half-life of <Superscript>97</Superscript>Zr,re-measured

Summary The half-life of ⁹⁷Zr, used for the calculation of thermal/epithermal neutron flux ratio in k₀-NAA, is re-determined using three measurement systems with different pulse processing principles. The result of 16.755±0.013 hours clarifies the discrepancy between two widely used literature values, 16.744±0.011 and 16.90±0.05 hours. Different dead-time correction methods used on various measurement systems are evaluated. Factors influencing precise measurement of relative peak counting rates are discussed in time-series measurements over a dynamic range of 1000-fold radioactive intensities (10 half-lives).