Urine radiobioassay intercomparison results from the Intercomparison Studies Program at Oak Ridge National Laboratory

The concentrations of As(III) and As(V) in natural hot spring and river waters collected in the Kusatsu-Shirane volcano area, Gunma, Japan, were determined by neutron activation analysis (NAA) preceded by the pyrrolidinedithiocarbamate (PDC) coprecipitation. The PDC coprecipitation technique using Pb(PDC)₂ as a collector of As(III) was applicable to the determination of As(III) at μg/L to mg/L levels. It was found important that the sufficient amount of PDC must be added to sample waters to accomplish the quantitative coprecipitation of As(III), taking the amounts of coexisting metal ions into consideration.     

Further development of accelerator mass spectrometry for the measurement of <Superscript>90</Superscript>Sr at Lawrence Livermore National Laboratory

Based on the encouraging results of our initial efforts to develop a ⁹⁰Sr accelerator mass spectrometry capability, we have undertaken efforts to enhance our system. By changing some key operating parameters and constructing an optimized detector we were able to improve the discrimination of ⁹⁰Sr from the isobaric interference ⁹⁰Zr and reduce our instrumental background by nearly two orders of magnitude. Our current background (4 × 10⁶ atoms, 3 mBq) is comparable to that achievable by decay counting, but is still a factor of ten higher than what is theoretically predicted based on the efficiency of our system. Therefore, future plans include implementation of a time-of-flight system to improve the rejection of ⁹⁰Zr.     

Simultaneous determination of <Superscript>89</Superscript>Sr and <Superscript>90</Superscript>Sr: comparison of methods and calculation techniques

The presence of ⁸⁹Sr and ⁹⁰Sr in the biosphere constitutes a biological hazard. There are several analytical methods for the determination of ⁸⁹Sr and ⁹⁰Sr. Three analytical methods of various application fields using selective Sr resin for Sr separation and DGA resin for Y separation and measuring techniques, i.e. liquid scintillation spectrometry and Cerenkov counting are discussed in the paper. The calculation techniques are compared in the aspects such as trueness and accuracy of the results and the limit of detection. Uncertainties and detection limits are calculated using the spreadsheet method.     

Polymer-coated magnetic nanoparticles for rapid bioassay of <Superscript>90</Superscript>Sr in human urine samples

A rapid bioassay for ⁹⁰Sr was developed involving preconcentration of ⁹⁰Sr/⁹⁰Y from human urine samples with a cation exchange polymer (poly–acrylamido–methyl–propanesulfonic acid) coated onto magnetic nanoparticles, followed by selective elution of ⁹⁰Sr (over ⁹⁰Y) with phosphate for determination by liquid scintillation analysis. The minimum detectable activity for this method (4.9 ± 0.5 Bq/L) is lower than the required sensitivity of 19 Bq/L for ⁹⁰Sr in human urine samples, as defined in the requirements for radiation emergency bioassay techniques for the public and first responders based on the dose threshold for possible medical attention recommended by the International Commission on Radiological Protection. The relative bias was 9.2%, the relative precision was 3.2%, and the linear dynamic range covered 12–600 Bq/L. This simple and rapid bioassay method is found to be in compliance with the HPS ANSI N13.30 performance criteria for radiobioassay.     

Quinolinephosphomolybdate as ion exchanger: synthesis,characterization, and application in separation of <Superscript>90</Superscript>Y from <Superscript>90</Superscript>Sr

An inorganic ion exchanger, quinolinephosphomolybdate has been synthesized and characterized by elemental analysis, infrared (IR) and X-ray diffraction (XRD) spectroscopy. This compound is highly stable toward thermal, chemical and radiation dose. This has been employed in the separation of carrier-free ⁹⁰Y from its parent ⁹⁰Sr from an equilibrium mixture. The absorbed daughter was recovered by using 0.0284 mol L⁻¹ ascorbic acid solutions at pH 5.0 as eluting agent.     

Determination of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in the bottom sediments from the Barents Sea

The aim of this paper was to determine the extent of contamination by anthropogeneous radionuclides ¹³⁷Cs and ⁹⁰Sr in the bottom sediments from the Barents Sea based on the radioactive activity of the samples taken up in August 1991, among others, from the area close to New Land Island and Francis Joseph Archipelago. The results are based on the phenomenon of vertical migration, in the bottom sediments which is of significant importance from the natural environment point of view.     

Methodology for determination of <Superscript>89</Superscript>Sr and <Superscript>90</Superscript>Sr in radiological emergency: II. Method development and evaluation

In this work a method for the determination of both ⁸⁹Sr and ⁹⁰Sr is presented. The method can potentially be used in radiological emergency and deliver results shortly after an incident. The method development was based on theoretical calculations of potential interferences from other fission products and how these could be discriminated when applying different chemical separation schemes. Validation was done on reactor coolant water containing short-lived fission products, and on a reference material. The results indicate that correct results of ⁸⁹Sr and ⁹⁰Sr can be obtained 4 and 9 days, respectively, after an incident.     

Estimation of <Superscript>90</Superscript>Sr activity in reprocessed uranium from the PUREX process

⁹⁰Sr estimation in reprocessed uranium was carried out by a series of solvent extraction and carrier precipitation techniques using strontium and lanthanum carriers. Fuming with HClO₄ was used to remove ¹⁰⁶Ru as RuO₄. Three step solvent extraction with 50% tri-n-butyl phosphate in xylene in presence of small amounts of dibutyl phosphate and thenoyl trifluoro acetone was carried out to eliminate uranium, plutonium, thorium and protactinium impurities. Lanthanum oxalate precipitation in acid medium was employed to scavenge the remaining multivalent ions. Strontium was precipitated as strontium oxalate in alkaline pH and ¹³⁷ Cs was removed by washing the precipitate with water. A strontium recovery well above 70% was obtained. Final estimation was carried out by radiometry using end window GM counter after drying the precipitate under an infra red lamp. The same procedure was extended to the estimation of ⁹⁰Sr in a diluted sample of the actual spent fuel solution. An additional lanthanum oxalate precipitation step was required to remove the entire ¹⁴⁴Ce impurity from this sample. This modified procedure was employed in the determination of ⁹⁰Sr in a number of reprocessed uranium samples and the over all precision of the method was found to be well within ±10%. An additional barium chromate precipitation step was necessary for the analysis of reprocessed uranium samples from high bumup fuels to eliminate trace amounts of short lived ²²⁴Ra produced during the decay of ²³²U and its daughters as they interfere in the estimation of ⁹⁰Sr.     

Analytical investigation of energy spectrums of beta rays emitted from <Superscript>90</Superscript>Sr and <Superscript>204</Superscript>Tl radioisotopes

The energy spectra of beta rays emitted from ⁹⁰Sr and ²⁰⁴Tl radioisotopes were obtained by using a silicon surface barrier detector with a 1000 μm depleted layer and 50 mm² effective area. The detector response function is interpreted by making use of range distributions of mono-energetic electrons in matter and by assuming a linear energy loss along the range in the depleted layer of the detector. An analytical expression is given for pulse height distribution obtained in the surface barrier detector. A good agreement is observed between the experimental results and theoretical interpretation.     

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%.     

Production of high specific activity <Superscript>68</Superscript>Ge at Brookhaven National Laboratory

Summary Germanium-68 is produced at the Brookhaven Linac Isotope Producer (BLIP) by irradiating ^natGa targets with ~45 MeV protons. Typical irradiation yields are 17.4 GBq (470 mCi) from a 4 week irradiation (0.52 MBq/µAh). Germanium-68 is recovered from the target by extraction into 4N HCl and 30% H₂O₂. Further purification is achieved by extraction into carbon tetrachloride and back-extraction into H₂O. Recovery yields are greater than 85%, with greater than 99% radiopurity, and activity concentrations are greater than 3.15 GBq/ml (85 mCi/ml). The final pH of the product solution, which is 0.03M diethylenetriaminepentaacetate (DTPA), can now be adjusted to user specifications.     

Determination of <Superscript>90</Superscript>Sr in preparedness: Optimization of total analysis time for multiple samples

In radiological emergency, rapid determination of radiostrontium will be necessary. The required quantification levels will be relatively high which offers smaller sample sizes and shorter ingrowth and counting times. In this paper a rapid method for the determination of ⁹⁰Sr in fresh milk in emergency preparedness is presented. The method is based on microwave digestion, chemical separation of Sr, ingrowth of ⁹⁰Y and Cherenkov measurements. In order to minimize the total analysis time, a mathematical model was developed. For a given number of samples the model minimizes the analysis time by optimizing the ingrowth and counting time in order to reach a detection limit fit-for-purpose.     

An ion chromatographic separation method for the sequential determination of <Superscript>90</Superscript>Sr, <Superscript>241</Superscript>Am and Pu isotopes in a urine sample

A radiobioassay method has been developed for the sequential determination of ⁹⁰Sr, ²⁴¹Am and Pu isotopes in a urine sample. Unlike the existing methods using multiple extraction chromatographic cartridges, this work demonstrates an application of an automated ion chromatographic (IC) system for the separation of these radionuclides on a single IC column. The method meets the bioassay performance criteria for relative bias and relative precision as recommended by ANSI/HPS N13.30-2011. The detection limits for the radionuclides are found to be satisfactory for medical intervention in case of an accidental exposure scenario. Sample preparation time is less than 11 h.     

Radioactivity in the Baltic Sea: inventories and temporal trends of <Superscript>137</Superscript>Cs and <Superscript>90</Superscript>Sr in water and sediments

The Baltic Sea is ecologically unique as one of the world’s largest brackish water basins. It was significantly contaminated by radioactivity following the Chernobyl accident in 1986, the major contaminant being long-lived ¹³⁷Cs. Due to the slow exchange of water between the Baltic Sea and the North Sea and the relatively rapid sedimentation rates, radionuclides have prolonged residence times in the Baltic Sea. ¹³⁷Cs levels are consequently still clearly higher than in other water bodies around the world. In addition to the Chernobyl accident, artificial radionuclides in the Baltic Sea originate from the global fallout following nuclear weapons testing in the 1950s and 1960s, while discharges into the Baltic Sea from nuclear power plants and other facilities are of minor importance. Here, inventories and the temporal evolution of radionuclides both in seawater and sediments of the Baltic Sea are presented and discussed.     

Distribution of uranium,plutonium, and <Superscript>241</Superscript>Am in soil samples from Idaho National Laboratory

Soil materials used were collected in the early 1970s at Idaho National Laboratory near the Subsurface Disposal Area (SDA). Samples from a depth of 0–4 and 4–8 cm at two different sites located on the northeast corner of the SDA perimeter were analyzed. The concentration of ²³⁴U, ²³⁵U, ²³⁶U, and ²³⁸U in soil digests were measured by mass spectrometry. Uranium isotopic composition of the soil at the two sample sites and depths is compared to previously measured concentrations of ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu, and ²⁴¹Am. Implications for remediation of contaminated soils surrounding the SDA are discussed.     

Radiometric analysis of <Superscript>90</Superscript>Sr in fish bone ash samples by liquid scintillation counting after separation by extraction chromatographic resin

Studies on the extraction behavior and immobilization of cadmium by greener reagents have important bearings in today’s science. No-carrier-added (NCA), ¹⁰⁹Cd radionuclide is a potential candidate towards radiopharmaceutical studies for both in vivo and in vitro applications and is also used in industrial and environmental studies. Herein, we have studied the adsorption and desorption characteristics of cadmium in both NCA and bulk concentrations into calcium alginate using radiochemical method. Various isotherms like Langmuir, Freundlich, Temkin and Dubinin–Radushkevich have been studied and compared to match the adsorption phenomenon. A spontaneous endothermic physisorption process is expected from thermodynamic parameters.     

Pattern recognition analysis for <Superscript>1</Superscript>H NMR spectra of plasma from hemodialysis patients

¹H NMR spectroscopic and pattern recognition-based methods (NMR-PR) were applied to the metabolic profiling studies on hemodialysis (HD). Plasma samples were collected from 37 patients before and after HD and measured by 600 MHz NMR spectroscopy. Each spectrum was data-processed and subjected to principal component analysis for pattern recognition. Spectral patterns of plasma between pre- and post-dialyses were clearly discriminated, together with significant fluctuations in the levels of creatinine, trimethylamine-N-oxide, glucose, lactate, and acetate, which were quantitated. We have first observed the significant elevation of lactate levels in post-dialysis plasma. The present study has demonstrated the high feasibility of NMR-PR method for monitoring the dialysis condition and comprehensive profiling of the change of low-molecular-weight metabolites in HD. Figure PCA for 1H NMR spectra of plasma from HD patients     

Photoacoustic and photoluminescence studies on ThO<Subscript>2</Subscript>:Sm<Superscript>3+</Superscript>

Nanocrystalline ThO₂:Sm³⁺ was synthesized using wet-chemical route and characterized using X-ray diffraction (XRD), photoacoustic (PA) and photoluminescence (PL) spectroscopy. PA absorptions of Sm³⁺ doped samples are found to be quite weak as compared to Nd³⁺, while PL of Sm³⁺ was intense. As the energy gap between lowest luminescent levels and highest non-luminescent level in samarium ion is around 7000 cm^?1; it is highly fluorescing compared to Nd³⁺ which has close by levels. Through photoacoustic data it was pointed out that large covalent character exists in ThO₂:Nd³⁺ compared to ThO₂:Sm³⁺.     

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.     

Niobium(V) oxide doped with Mg<Superscript>2+</Superscript> and Gd<Superscript>3+</Superscript> cations: Synthesis and structural studies

Methods for direct doping of niobium pentoxide with photovoltaically inactive Mg²⁺ and Gd³⁺ cations were developed for subsequent use in the synthesis of a stock for growing single crystals of lithium niobate with improved optical characteristics. The Raman spectra of doped pentoxides Nb₂O₅: Mg and Nb₂O₅: Gd revealed their island structures.