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.     

SDAT: analysis of <Superscript>131m</Superscript>Xe with <Superscript>133</Superscript>Xe interference

The Spectral Deconvolution Analysis Tool (SDAT) software was developed at The University of Texas at Austin. SDAT utilizes a standard spectrum technique for the analysis of β–γ coincidence spectra. Testing was performed on the software to compare the standard spectrum analysis technique with a region of interest (ROI) analysis technique. Experimentally produced standard spectra and sample data were produced at the Nuclear Engineering Teaching Laboratory (NETL) TRIGA reactor. The results of the testing showed that the standard spectrum technique had lower errors than the ROI analysis technique for samples with low counting statistics. In contrast, the ROI analysis technique outperformed the standard spectrum technique in high counting statistics samples. It was also shown that the standard spectrum technique benefitted from a compression of the number of channels within the spectra.     

A simple method for self-attenuation correction in <Superscript>210</Superscript>Pb activity measurement in a well-type HPGe detector

A simple method for ²¹⁰Pb determination in a well-type detector for matrix with apparent densities ranging from ρ = 0.430 g cm^?3 to ρ = 2.037 g cm^?3 is presented. Ten spiked samples of ²¹⁰Pb were prepared to obtain the detector efficiency as a quadratic function of the matrix density. Then this equation was validated and successfully used to measure ²¹⁰Pb concentration activity in other samples. The equation proposed in this work is specific for each germanium detector; however it is proposed an extrapolation of the method to other well-type germanium detector by preparing a spiked sample and determining the efficiency for ²¹⁰Pb.     

Production of <Superscript>41</Superscript>Ar and <Superscript>79</Superscript>Kr gaseous radiotracers for industrial applications

Radiotracers are extensively used in many industries for trouble shooting and optimization of process parameters leading to considerable savings in time and huge economic benefits. In chemical and petrochemical industries different gases and vapours flowing in the conversion reactors play a major role in the final production. Gaseous radiotracers are ideal to study hydrodynamics of gas phases in process vessels. ⁴¹Ar and ⁷⁹Kr are the preferred gaseous radiotracers for such studies. Owing to the increase in demand from Indian industries for gas phase radiotracers, efforts have been made to produce ⁴¹Ar and ⁷⁹Kr indigenously by irradiation of ⁴⁰Ar and enriched ⁷⁸Kr gaseous targets in research reactors. Prequalification of the containers used, safety aspects concerning accidental rupture and mandatory tests necessary for irradiation of gaseous targets in the reactors have been studied. The paper describes some of the important safety aspects involved and the results of trial irradiations on the production of ⁴¹Ar and ⁷⁹Kr radiotracers. Standardization of suitable assay protocols for their regular production and supply for applications in industries is also described.     

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.     

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.     

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.     

Adsorption of <Superscript>85</Superscript>Kr radioactive inert gas into hardening mixtures

Changes in volumetric activity of ⁸⁵Kr radioactive inert gas take place in the atmosphere: it has increased by around 50% during the past 15 years. The main source of such gas is the operation of nuclear power plants and spent nuclear fuel reprocessing plants. ⁸⁵Kr as an inert gas spreads throughout the entire atmosphere and its ionizing radiation may result in changes of atmospheric electric phenomena. Therefore it is necessary to control ⁸⁵Kr emission into the atmosphere. However, there is no effective method for this as inert gases, under normal conditions, can hardly be adsorbed in different adsorbents and stored in special containers for a long period of time. This paper tries to show the possibility of keeping ⁸⁵Kr longer within the adsorbent by changing its aggregate state: gas is adsorbed into liquid adsorbent and desorption takes place from solid adsorbent. For this purpose, an epoxy resin is used which, after adding a special hardener at room temperature, turns into a solid material with density of around 1.2 × 10³ kg m⁻³. As a result of sample blending with substances which contribute to better solubility of ⁸⁵Kr, diffusion coefficient of this gas (i.e. desorption speed) changes within the adsorbent in the solid state.     

A semi-empirical formula for HPGe detector efficiency calibration

The precision obtainable by instrumental neutron activation analysisdepends strongly on the quality of the calibration of the gamma-ray spectrometerused for measuring the irradiated samples. Even when relative standardizationis employed, practical experience has shown the importance of detector calibration.This is especially relevant when radionuclides of varying activities are involved.The problems often encountered are those of intolerable high dead time andthe occurrence of summed peaks in the gamma-ray spectra. A simple but accuratesemi-empirical formula is presented that could effectively predict the efficiencyof a detector at any source-to-detector distance. Experimental data obtainedat 0, 50, 100, 200 mm source-to-detector distances are used to demonstratethe usefulness of this formulation. In addition, nine elements were analyzedin the NIST Orchard Leaves using absolute standardization including four elementsSm, Ta, Au, and La for which no certified values could be obtained.     

Preparation of <Superscript>166</Superscript>Dy/<Superscript>166</Superscript>Ho-chitosan as an in vivo generator for radiosynovectomy

¹⁶⁶Ho is one of the most effective radionuclides used for radiosynovectomy. One method to deliver this radioisotope to target tissue is via the ¹⁶⁶Dy/¹⁶⁶Ho in vivo generator system. The aim of this work was to prepare ¹⁶⁶Dy/¹⁶⁶Ho-chitosan (¹⁶⁶Dy/¹⁶⁶Ho-CHIT) in vivo generator for radiosynovectomy applications. ¹⁶⁶Dy obtained by the irradiation of natural ¹⁶⁴Dy target. ¹⁶⁶Dy was separated from ¹⁶⁶Ho by extraction chromatographic method (separation yield; 93% and separation factor;1.7). Chitosan labeling was performed in acetic acid with 99.3 ± 0.6% radiochemical purity. Biodistribution studies on intraarticular injected rats demonstrated high retention in the knee joint even 7 days showing no radioactivity leakage from the injection site into other organs as well as any translocation of the daughter nucleus after β^? decay of ¹⁶⁶Dy.     

Preparation of a one-curie <Superscript>171</Superscript>Tm target for the detector for advanced neutron capture experiments (DANCE)

Approximately one curie of ¹⁷¹Tm (T _1/2 = 1.92a) has been produced and purified for the purpose of making a nuclear target for the first measurements of its neutron capture cross section. Target preparation consisted of three key steps: (1) material production; (2) separation and purification; and (3) electrodeposition onto a suitable backing material. Approximately 1.5 mg of the target material (at the time of separation) was produced by irradiating ca. 250 mg of its stable enriched ¹⁷⁰Er lanthanide neighbour with neutrons at the ILL reactor in France. This production method resulted in a “difficult-to-separate” 1:167 mixture of near-neighboring lanthanides, Tm and Er. Separation and purification was accomplished using high-performance liquid chromatography (HPLC), with a proprietary cation-exchange column (Dionex, CS-3) and alpha-hydroxyisobutyric acid (α-HIB) eluent. This technique yielded a final product of ∼95% purity with respect to Tm. A portion (20 μg) of the Tm was electrodeposited onto thin Be foil and delivered to the Los Alamos Neutron Science Center (LANSCE) for preliminary analysis of its neutron capture cross section using the Detector for Advanced Neutron Capture Experiments (DANCE). This paper discusses the major hurdles associated with the separation and purification step, including scale-up issues related to the use of HPLC for material separation and purification of the target material from α-HIB and 4-(2-pyridylazo)resorcinol (PAR) colorant.     

Preparation and analysis of <Superscript>226</Superscript>Ra-<Superscript>222</Superscript>Rn emanation standards for calibrating passive radon detectors

Summary In order to calibrate vials containing charcoal for measurement of radon, emanation sources of radon were produced in-house using ²²⁶Ra salts. Calibrated emanation standards containing solution of ²²⁶Ra(NO₃)₂ absorbed into inorganic compounds were prepared. The emanation coefficient of ²²²Rn for these standards vary from 0.23-0.25. The emanation sources were found to be suitable for calibrating radon monitors.     

Radionuclide purity assessment and calibration of <Superscript>90</Superscript>Y(<Superscript>177</Superscript>Lu) glass particles using gamma-ray spectrometry

Intra-hepatic administration of radioactive glass microspheres is a treatment for patients with primary liver cancer and hepatic metastases. The purpose of this study was radionuclide purity assessment of new glass particles containing two radionuclide, ⁹⁰Y as a therapeutic source and also ¹⁷⁷Lu as a source of diagnostic gamma. For the mixed source, activity measurement using a dose calibrator cannot be used and we need new calibration methods. YAS (Yb) and YAS compositions were sol–gel derived glass particles and production of ⁹⁰Y (¹⁷⁷Lu) and ⁹⁰Y particles was performed using the Tehran Research Reactor. The radionuclide purity was carried out using γ-spectrometry with HPGe detector. A non-destructive spectroscopic assay was employed due to a newly updated low uncertainty positron branching ratio of ⁹⁰Y that emit 511 keV annihilation radiations. In another method, a new calibration of ⁹⁰Y using a non-destructive spectroscopic assay of ⁸⁸Y were investigated. Potential radionuclide impurity include: ⁸⁸Y, ¹⁵²Eu, ⁶⁰Co with activity 100, 50 and 5 Bq per 1 mg of that are not harmful for patients due to delivering radioactive particles about 20–50 mg in ⁹⁰Y(¹⁷⁷Lu) glass microspheres. Among of radionuclide impurity, ¹⁵²Er with a half life of 13.54 years and ⁸⁸Y with a half life of 106.65 days was important in the residual delivery device. For calibration of ⁹⁰Y with monitoring of 511 keV, errors were12.2–21%. In calibration of ⁹⁰Y using gamma spectroscopic assay of ⁸⁸Y, there was an error less than 14%. Spectroscopic assay of ⁸⁸Y can be performed easily and has more repeat for our purpose.     

Preparation and preliminary evaluation of <Superscript>211</Superscript>At-labeled amidobisphophonates

In this paper, 3-amino-1-hydroxypropylidene-1,1-bisphosphonate(APB), a amidobisphophonate was synthesized and labeled with the α-emitter ²¹¹At by an indirect method using N-succinimidyl 5-(tributylstannyl)-3-pyridinecarboxylate (SPC) as a bi-functional linker, and the conjugated amidobisphophonate (²¹¹At-SAPC-APB) was preliminarily evaluated in vitro and in vivo by comparison with free astatide (²¹¹At⁻) and ^99mTc-MDP. 3-amino-1-hydroxypropylidene-1,1-bisphosphonate(APB) was prepared using β-alanine as the starting material. With SPC bi-functional linker, APB was conjugated with ²¹¹At in a labeling yield of 80–90% with radiochemical purity of more than 99%. The conjugated amidobisphophonate (²¹¹At-SAPC-APB) exhibited considerable stability in vitro, in that the radiochemical purity of ²¹¹At-SAPC-APB was still more than 98% in 0.1 mol/L PBS (pH 7.6) or in fetal calf serum, even stayed for 24 h at room temperature (RT). Biodistribution of ²¹¹At-SAPC-APB was investigated in NIH strain mice by I.V injection. The results showed that ²¹¹At-SAPC-APB could rapidly locate in shank, with the maximum uptake of 23.70 ± 2.29% I.D/g at 6 h, earlier than that of ^99mTc-MDP at 12 h, and stayed in the bone for long time. Moreover, ²¹¹At-SAPC-APB uptake in some key organs or tissues, especially in thyriod, stomach, lung and spleen, was much less than that of free astatide (²¹¹At⁻), implying that ²¹¹At-SAPC-APB was constantly stable in vivo as well as in vitro. These results indicated that ²¹¹At-SAPC-APB will be a suitable candidate for the targeted radiotherapy of bone metastases and should be further investigated.     

Scalar-relativistic 5f-in-core pseudopotentials and core-polarization potentials for trivalent actinides: calibration calculations for Ac<Superscript>3+</Superscript>, Cm<Superscript>3+</Superscript> and Lr<Superscript>3+</Superscript> complexes

The performance of recently proposed 5f-in-core pseudopotentials for the trivalent actinides was investigated in calculations for model complexes An³⁺L ⁿ⁻ for three selected actinides (An³⁺ = Ac³⁺, Cm³⁺, Lr³⁺) and eight simple ligands with atoms from the first three periods of the table of elements (L ⁿ⁻ = F⁻, Cl⁻, OH⁻, SH⁻, CO, NH₂⁻, H₂O, H₂S, NH₃). Results of Hartree-Fock and Coupled Cluster with singles, doubles and perturbative triples calculations using basis sets of quadruple-zeta quality are compared to corresponding reference data obtained with scalar-relativistic energy-adjusted 5f-in-valence small-core pseudopotentials. The inclusion of core-polarization potentials in the 5f-in-core pseudopotential calculations and corrections of the basis set superposition error by the counterpoise correction leads to very good agreement between the 5f-in-valence and 5f-in-core pseudopotential results for bond lengths, bond angles and binding energies. Results from 5f-in-core pseudopotential calculations using different density functionals also show reasonable agreement with the more rigorous Coupled Cluster results. It is argued that the An 5f rather than the An f population is a useful criterion for the applicability of a specific An 5f-in-core pseudopotential.     

Full energy peak efficiency calibration of HPGe detector for point and extended sources using Monte Carlo code

Monte Carlo simulation is important to get efficiencies for cases where the experimental efficiencies are difficult to get such as for samples with nonstandard geometries and for large samples. In this paper, efficiency of the HPGe detector, routinely used in our lab for a variety of samples, has been computed for point source geometry and its parameters has been optimized to match MCNP and experimental efficiencies within 5% at different sample to detector distances. This optimized geometry was then validated by efficiency transfer to other geometries.     

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%.     

Disequilibrium of dissolved <Superscript>234</Superscript>U/<Superscript>238</Superscript>U and <Superscript>210</Superscript>Po/<Superscript>210</Superscript>Pb in Greek rivers

For the first time, a radiological study for the dissolved ²³⁸U, ²³⁴U, ²¹⁰Pb and ²¹⁰Po was held in major Greek rivers across the country. ²³⁴U/²³⁸U activity ratios are above one in all samples and ²¹⁰Po/²¹⁰Pb activity ratios are respectively below the unit indicating the disequilibrium in the samples. Quite satisfactory correlations were observed among ²³⁴U and ²³⁸U as well as among ²¹⁰Po and ²¹⁰Pb values. Uranium isotopes were separated by ion exchange and electroplated on stainless steel plates. ²¹⁰Po was spontaneously deposited on nickel plates, while ²¹⁰Pb was indirectly determined through the ingrowth of ²¹⁰Po. The sources were measured by a-spectrometry.     

<Superscript>129</Superscript>Xe NMR spectroscopy of adsorbed xenon: Possibilites for exploration of microporous carbon materials

Despite the extensive use of ¹²⁹Xe NMR for characterization of high surface-to-volume porous solids, particularly zeolites, this method has not been widely used to explore the properties of microporous carbon materials. In this study, commercial amorphous carbons of different origin (produced from different precursors) and a series of activated carbons obtained by successive cyclic air oxidation/pyrolysis treatments of a single precursor were examined. Models of ¹²⁹Xe chemical shift as a function of local Xe density, mean pore size, and temperature are discussed. The virial coefficient arising from binary xenon collisions, σ_Xe-Xe, varied linearly with the mean pore size given by N₂ adsorption analysis; σ_Xe-Xe appeared to be a better probe of the mean pore size than the chemical shift extrapolated to zero pressure, σ_S.