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.     

Isotopic fractionation during pretreatment for accelerator mass spetrometer measurement of (D<Subscript>3</Subscript>C)<Subscript>2</Subscript>O containing <Superscript>14</Superscript>C produced by nuclear reaction

A (D₃C)₂O (d₆-acetone) target was irradiated with semi-monoenergetic neutrons generated from ⁹Be(p,n)⁹B reaction with 20 MeV protons to convert ¹³C and oxygen nuclides in the target into ¹⁴C. With both liquid scintillation counting (LSC) and accelerator mass spectrometry (AMS) we measured the (D₃C)₂O (d₆-acetone) liquid targets, which were combustible and easy to afford CO₂ for the AMS measurements. The ¹⁴C yield measured by the LSC method turned out to be 80 times larger than that by the AMS method. This large discrepancy may be attributed to the loss of ¹⁴C atoms during the sample pretreatment in the AMS method such as combustion and cryogenic trapping of CO₂. It means that ¹⁴C newly produced by nuclear reactions can exist in various chemical forms, i.e., C₃D₆O, CO, CO₂, hydrocarbons, etc., and a simple sample pretreatment right after production can cause serious isotopic fractionation. Therefore, using the AMS method, extreme caution in sample pretreatment should be exercised when the ¹⁴C yield produced immediately by nuclear reaction is measured.     

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.     

Field measurement of the <Superscript>218</Superscript>Po, <Superscript>214</Superscript>Pb and <Superscript>214</Superscript>Bi concentrations in typical indoor and outdoor environments in Beijing

The activity concentrations of ²¹⁸Po, ²¹⁴Pb and ²¹⁴Bi [i.e. C(²¹⁸Po), C(²¹⁴Pb), and C(²¹⁴Bi)] and the calculated concentration ratios [i.e. 1:C(²¹⁴Pb)/C(²¹⁸Po):C(²¹⁴Bi)/C(²¹⁸Po)] are necessary for assessing radon and its progenies exposure. In this study, a measurement method of radon progenies concentrations with both high sensitivity and low uncertainty, was developed based on the Kerr method. The field measurement results of radon progeny concentrations and calculated concentration ratios in both typical indoor and outdoor environments in Beijing, China, were reported. The effects of air exchange rate on concentration ratios of radon progenies in indoor environments were discussed.     

A facile preparation of ammonium [<Superscript>14</Superscript>C]thiocyanate

Summary An attractive and simple method has been developed for the preparation of ammonium [¹⁴C]thiocyanate from [¹⁴C]thiourea which eliminates the necessity of handling highly hazardous potassium [¹⁴C] cyanide. [¹⁴C]thiourea was isomerized to ammonium [¹⁴C]thiocyanate by heating the aqueous solution of thiourea (12%) in a sealed tube at 160 °C for 24 hours. The product formed was purified by silica-gel column chromatography. A radiochemical yield of 92.7% was obtained based on [¹⁴C]thiourea. The specific activity of the product obtained was 53.3 mCi/mmol (1.97 GBq/mmol) and the radiochemical purity was greater than 99%. This method has not been reported so far for the production of this labeled compound.     

Global fallout levels of <Superscript>99</Superscript>Tc and activity ratio of <Superscript>99</Superscript>Tc/<Superscript>137</Superscript>Cs in the Pacific Ocean

Summary Global fallout levels of ⁹⁹Tc and ¹³⁷Cs of surface seawater in the Pacific Ocean were measured. The ⁹⁹Tc concentrations ranged from 0.62 to 3.33 mBq^. m^-3and 5 of 6 samples showed less than 1 mBq^. m^-3except one sample taken in the Great Barrier Reef, Australia. The ¹³⁷Cs concentrations ranged from 2.13 to 3.14 Bq^. m^-3, showing a gradual decrease in the North Pacific toward the equator and a constant level in the South Pacific. The ⁹⁹Tc/¹³⁷Cs activity ratios ranged from 2.5^. 10^-4to 2.9^. 10^-4, which is very close to that calculated theoretically from the fission yield.     

Distribution characteristics of <Superscript>14</Superscript>C and <Superscript>3</Superscript>H in spent resins from the Canada deuterium uranium-pressurized heavy water reactors (CANDU-PHWRs) of Korea

It is regarded that the spent resins from the water purification systems of moderator (MOD) and the primary coolant of the Canada deuterium uranium-pressurized heavy water reactor (CANDU-PHWR) are a unique waste, owing to their high ¹⁴C and gamma-emitting nuclides. In this work, ¹⁴C and ³H contents, anion and cation fractions and the predominant gamma-emitting nuclides of the spent resins from 4 units of CANDUPHWRs, were investigated. Also the chemical species of ¹⁴C of the spent resins were determined. For a simultaneous separation of ¹⁴C and ³H from the spent resins, the wet oxidation-16 wt% H₂SO₄ stripping process was utilized. The ¹⁴C and ³H activity concentration range of the spent resins of the nuclear power plant (NPP), 4 units of all CANDU-PHWR types, was 2.48E5 Bq/g ∼5.33E6 Bq/g, 1.29E5 Bq/g and ∼2.33E5 Bq/g, respectively. Among the analyzed spent resins, the highest ¹⁴C and ³H activity concentration was detected in units 4 and 3, respectively. It was found that more than 92% of the ¹⁴C activity concentration was retained on the anion resin and the predominant chemical species was inorganic ¹⁴C. It was revealed that the anion resin fraction of the spent resins from unit 1 and unit 2, was about 40% and that of unit 3 and unit 4 was around 60%. More than 80% of the total gamma-radioactivity concentration was associated with the cation fraction of the spent resin. The predominant gamma-emitting nuclide of the spent resin for unit 2 was ¹³⁷Cs, a fission product, and that for unit 4 was ⁶⁰Co, a corrosion product.     

Measurements of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb in total diet samples: Estimate of dietary intakes of <Superscript>210</Superscript>Po and <Superscript>210</Superscript>Pb for Japanese

To estimate the dietary intakes of ²¹⁰Pb and ²¹⁰Po for the Japanese adults and their annual effective doses, ²¹⁰Pb and ²¹⁰Po were measured for 240 daily diet samples collected at two locations of Ishikawa Prefecture in Japan over three years by duplicate portion studies. No appreciable differences in intake rates of ²¹⁰Pb and ²¹⁰Po and their ²¹⁰Po/²¹⁰Pb ratios were seen among the years in each district, and between the two districts. The intake rates evaluated using 240 diet samples were 0.20 Bq/d/p for ²¹⁰Pb and 0.61 Bq/d/p for ²¹⁰Po as a median, respectively. Annual effective doses of ²¹⁰Pb and ²¹⁰Po for Japanese adults were estimated to be 0.050 and 0.053 mSv/y, respectively.     

Magnesium-Potassium Phosphate Matrix for Immobilization of <Superscript>14</Superscript>C

Possibility of using a low-temperature magnesium-potassium phosphate matrix to solve the problem of immobilizing the radioactive wastes containing radioactive carbon (¹⁴C) in the form of calcium carbonate was examined. The physicochemical characteristics of the compounds obtained were determined. Large values of the ultimate compression strength (22 ± 5 MPa), which satisfy the technical requirements for cemented radioactive wastes (no less than 4.9 MPa), were obtained. The minimum carryover of carbon dioxide into the atmosphere in the course of synthesis and in keeping of samples for 14 days was noted: not more than 3 wt % relative to the starting CaCO₃. The leaching rate of carbonate ions from magnesium-potassium compounds by 28th day of contact with air does not exceed 10?9 g cm^?2 day^?1, with this value for the rest of the compound components not exceeding 10^?4 g cm^?2 day^?1. Thus, it was found that the magnesium?potassium phosphate matrix is an alternative to the cementation for solidification of radioactive wastes containing ¹⁴C.     

Application of an experimental design to optimize a segregation method of <Superscript>129</Superscript>I and <Superscript>14</Superscript>C

In this work, the optimization of a segregation method of ¹²⁹I and ¹⁴C, two long-living radionuclides, main constituents of nuclear radioactive waste, has been developed. To be able to carry out this project, a fractional factorial experimental design was applied using 5 factors and 2 levels by factor (2^5–2). Only 8 experiments were necessary to identify the variables affecting the process, and very good recoveries of both radionuclides were obtained: (94?±?2)% for ¹²⁹I, and (99?±?1)% for ¹⁴C. The segregation of ¹²⁹I was influenced by flow (Q), volume of H₂SO₄ (V_H+), and carriers (CR), while V_H+ and time (t) played a major role in the segregation of ¹⁴C.     

Simultaneous measurements of cosmogenic radionuclides <Superscript>32</Superscript>P, <Superscript>33</Superscript>P and <Superscript>7</Superscript>Be in dissolved and particulate forms in the upper ocean

A technique to determine concentrations of ³²P, ³³P and ⁷Be in dissolved and particulate forms, in the upper ocean was developed. By using a large volume in situ filtration and concentration system (LV-FiCS), several tons of seawater at different depths were filtered concurrently through two kinds of filters. The dissolved radionuclides were concentrated onto adsorbents in the LV-FiCS. The radionuclides obtained were further purified by precipitation and ion-exchange chromatography, and quantified by gamma-spectrometry and ultra-low level liquid scintillation counter measurements. The technique was used with good results in a coastal area of Ibaraki, Japan.     

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.     

Direct low-energy measurement of <Superscript>37</Superscript>Ar and <Superscript>127</Superscript>Xe in a radiotracer gas using low-background proportional counters

A radiotracer gas with a blend of ³⁷Ar and ¹²⁷Xe was created for a gas migration experiment and was characterized at Pacific Northwest National Laboratory using ultra-low-background proportional counters. This paper describes the direct low-energy measurement of ³⁷Ar and ¹²⁷Xe in a dual-isotope sample. Using this low-energy technique, the dual-isotope radiotracer gas was determined to have activity concentrations of 483 Bq/cc and 1435 Bq/cc for ³⁷Ar and ¹²⁷Xe, respectively, and a ratio of 1:3 on the reference date of 7/11/2016.     

<Superscript>237</Superscript>Np in peat and lichen in Finland

Activity concentrations of ²³⁷Np in peat and lichen samples in Finland were determined and contributions from nuclear weapons testing in 1950–1960s and the Chernobyl accident were estimated. ²³⁷Np was determined with ICP-MS using ²³⁵Np as a tracer. Activity concentrations of ²³⁷Np in peat samples varied between 1.98 ± 0.05 and 14.1 ± 0.3 mBq/m². The contribution from the Chernobyl accident to the total ²³⁷Np deposition in peat was 0.1–13%, the Chernobyl-derived fraction of total ²³⁷Np in peat being much lower than the previously determined corresponding Chernobyl-derived fractions of ^239+240Pu, ²⁴¹Pu, ²⁴¹Am and ²⁴⁴Cm.     

Gasification characteristics to <Superscript>14</Superscript>CO<Subscript>2</Subscript> of <Superscript>14</Superscript>C radionuclide desorbed from spent resin by phosphate solutions

The removal characteristics of H¹⁴CO₃ ⁻ ions from IRN-150 mixed resin contaminated with ¹⁴C radionuclide and the gasification effects of ¹⁴C radionuclide on ¹⁴CO₂ are investigated in this study. The stripping solutions used for the removal of ¹⁴C from spent resin are NaNO₃, Na₃PO₄, NH₄H₂PO₄, and H₃PO₄. The influence of the stripping solution concentration on the desorption characteristics of an inactive HCO₃ ion into a stripping solution from IRN-150 mixed resin and the gasification of this ion to CO₂ is analyzed. The gasification behavior to CO₂ using NaOH, HNO₃, and HCl was also compared to that of phosphate solution. Spent resin stored in Wolsong nuclear power plant is used to evaluate the gasification characteristics of ¹⁴C radionuclide to ¹⁴CO₂. Gamma radionuclides such as ¹³⁷Cs and ⁶⁰Co in residual striping solutions after desorption experiments are analyzed.     

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%.     

<Superscript>1</Superscript>H and <Superscript>31</Superscript>P nuclear spin-lattice relaxation in C-phosphorylated oximes

The ¹H spin-lattice relaxation times of the proton-bearing groups and the ³¹P spin-lattice relaxation times in C-phosphorylated oximes R¹C(=NOH)P(=O)R²R³ (R¹ = Ph, R² = R³ = OMe; R¹ = Ph, R² = OMe, R³ = OCH²CH²Br; R¹ = PhCH², R² = R³ = OCHMe²) and dioxime R²P(=O)C(=NOH)(CH₂)₄C(=NOH)P(=O)R² (R = OMe) in DMSO-d₆ were measured. The characteristic reorientation times of the whole molecules were estimated using the measured values of the ¹H relaxation times and the results of semiempirical PM3 quantum chemical calculations of the molecular geometries. The reorientation times were used to identify the contributions of different relaxation mechanisms to the rate of ³¹P spin-lattice relaxation. The anisotropy of the chemical shielding of ³¹P nuclei was evaluated from the difference between the ³¹P relaxation rates measured at 101.27 and 161.92 MHz.     

<Superscript>234</Superscript>U/<Superscript>238</Superscript>U and <Superscript>235</Superscript>U/<Superscript>238</Superscript>U ratios in domestic water from the environs of Obuasi mine in Ghana

Activity concentrations of ²³⁸U, ²³⁵U and ²³⁴U were determined in different sources of drinking water at the Obuasi gold mines and its surrounding areas in Ghana. Water samples collected from the mines and its surrounding areas were analyzed using direct gamma-ray spectrometry and neutron activation analysis. The ²³⁴U/²³⁸U and ²³⁵U/²³⁸U ratios were calculated and the mean values range from 1.27 to 1.38 and from 0.044 to 0.045 respectively. The average ²³⁴U/²³⁸U ratio was from 1.27 for groundwater to 1.38 for treated water, demonstrating the lack of equilibrium. The average ²³⁵U/²³⁸U activity ratio is 0.045, indicating that only natural uranium was detected in the samples investigated.     

<Superscript>13</Superscript>C NMR and mass spectrometry of soil organic matter

Liquid state, high resolution ¹³C NMR spectroscopy and mass spectrometry were used to study the composition and structure of soil organic matter (SOM) using soil extracts from two long-term experiments at the Rothamsted Experimental Station. Both one- and two-dimensional NMR techniques were applied. ¹³C NMR sub-spectra of the CH _n (n=0...3) groups, obtained by the Distortionless Enhancement by Polarisation Transfer (DEPT) technique, were used for the elucidation of the qualitative and quantitative composition of humic and fulvic acids in the soils. The chemical structure of SOM was further analysed at the molecular level through Fast Atom Bombardment Mass Spectrometry (FABMS) and Gas Chromatography-Mass Spectrometry (GC/MS). Humic and fulvic extract results were not only compared to each other, but also to the solid state ¹³C NMR results for the complete soil sample.     

Ultra-sensitive measurements of <Superscript>233</Superscript>U by accelerator mass spectrometry for national security applications

By making modifications to our previously established measurement setup, we increased our abundance sensitivity for ²³³U by three orders of magnitude and can now measure ²³³U/²³⁸U ratios as low as 10⁻¹³. Because ²³³U has separate production pathways than ²³⁶U, it can provide valuable information on the particular source of anthropogenic uranium in a sample. We demonstrated the utility of our improved capability by using ²³³U to distinguish separate sources of anthropogenic uranium in a set of samples collected from a contaminated site. In the future, we plan to apply our new capability to characterizing ²³³U in a wide range of uranium materials.