Radiochemical determination of the yields of transuranium nuclides produced from natural uranium irradiated in a reactor

Transuranium nuclides were produced by irradiating a pellet of natural uranium sulfide in the Japan Material Testing Reactor (JMTR). After irradiation, a successive separation of uranium, plutonium, americium and curium was carried out. The fractional concentrations of the nuclides²³⁸Pu,²³⁹Pu,²⁴⁰Pu,²⁴¹Am,²⁴³Am,²⁴²Cm and²⁴⁴Cm were determined by α-ray spectrometry, and those of²⁴¹Pu and^242mAm were estimated from the build-up of α-emitting daughters,²⁴¹Am and²⁴²Cm, respectively. As the yield of²⁴²Pu was too slight to be detected by α-counting, the neutron activation analysis of the plutonium fraction based on the²⁴²Pu(n, γ)²⁴³Pu reaction was carried out by γ-ray spectrometry, and it was shown that a few pg of²⁴²Pu could be determined. A burn-up of²³⁵U was also estimated by neutron activation analysis. The experimental results are compared with the calculated ones.     

Low level Pu and Am estimation in liquid waste from nuclear reactor

Estimation of very low amount up to pico-gram of Am and Pu in the liquid waste of U–Pu fuel cycle of the irradiated U fuel from the nuclear reactor has been carried out using combined method of α- and γ-ray spectrometric techniques. ²⁴¹Am was estimated by γ-ray spectrometry from a plancheted source. In spite of the same α energy of 5.49 MeV for ²⁴¹Am and ²³⁸Pu, the amount ²³⁸Pu was estimated by α spectrometry from the same plancheted source after subtracting amount of the ²⁴¹Am obtained from γ-ray spectrometry. The amount of Am and Pu obtained by this technique is found to be superior compared to other techniques even in the presence of Th, U and fission products.     

Application of instrumental radioanalytical techniques to nuclear waste testing and characterization

This paper describes the validation of a multi-technique analytical methodology that uses inductively coupled plasma-mass spectrometry, α-spectrometry, and γ-spectrometry for the routine analysis of samples containing transuranic radionuclides. This methodology is capable of the determination of concentrations of both²³⁸Pu and²⁴¹Pu in the presence of²³⁸U and²⁴¹Am without the need for chemical separations. The relative merits of these three techniques were evaluated as they are applied in a nuclear waste material and spent nuclear fuel testing program by analytical (1) standards and (2) solutions prepared from the dissolution of glasses doped with²³⁷Np,²³⁹Pu, and²⁴¹Am. The uncertainty associated with technique was within ±4% for standards and ±10% for doped nuclear waste glasses. The methodology was then used to analyze three fully radioactive waste glasses.     

γ-Ray spectroscopic reinvestigation of the long lived166Hom decay

The decay of¹⁶⁶Ho^m has been reinvestigated on radiochemically separated sources with the aid of high efficiency HPGe detector. Energies and intensities of 54 γ-lines, of which 10 are new, were carefully measured. All γ-rays can be interpreted as deexciting known¹⁶⁶Er levels.     

A separation procedure for the analysis of90Sr,154Eu, and the actinides237Np,239Pu,241Am and244Cm

A procedure for the analysis of⁹⁰Sr,¹⁵⁴Eu,²³⁷Np,²³⁹Pu,²⁴¹Am and^242−244Cm was developed. Separation was done with the separating agent, di-2(ethyl hexyl)-phosphoric acid (HDEHP), and results in fractions containing the different elements to be analysed.⁹⁰Sr analysis was done by analysing its daughter nuclide⁹⁰Y, detected through the Cherenkov radiation emitted by this high energy β⁻-emitter.¹⁵⁴Eu was detected using γ-spectrometry with a lower Compton background as a result of the removal of other fission products.²⁴¹Am could also be detected with γ-spectrometry or together with^242−244Cm with α-spectrometry. The long-lived radionuclides²³⁷Np and²³⁹Pu were detected using inductively coupled plasma mass spectrometry (ICP-MS).     

Research for technique of preparing high-intensity241Am low-energy gamma-source

Systematically complicated technique used for preparing high-intensity (more than 8.0 GBq/cm²)²⁴¹Am -source by a new enamel technique is presented. High intensity²⁴¹Am -sources with activities ranging from 3.7 to 37 GBq have been made by this new technique. The activity and photon output have been measured. The results were compared with the data reported by the Radiochemical Centre Amersham in their specification. The photon output of²⁴¹Am -source produced by us meets the technical specification of²⁴¹Am -sources produced by Amersham. Moreover, the highest intensity can reach 1789 mCi/cm². The overall utilization ratio of²⁴¹Am activity (59.5 keV) is 31.2%.     

Comparison of alpha-spectrometry and alpha/gamma ratio method for the determination of americium in plutonium bearing fuel materials

Determination of americium is one of the requirements of chemical quality assurance of plutonium bearing fuel materials. Alpha-spectrometry is generally used for the determination of ²⁴¹Am in Pu bearing fuels since the efficiency of semiconductor detector used for alpha-spectrometry is independent of the alpha-particle energy in the 4 to 8 MeV range. However, this method has limitations for Pu samples containing extremely small or very large amounts of ²⁴¹Am. Thus an alternative methodology based on alpha/gamma (α/γ) activity ratio was developed and tested using different samples. The method is based on the determination of total γ-activity (of 60 keV peak) of an aliquot of the solution and the total α-activity present in the aliquot. The method is fast as it does not involve chemical separation of Pu and Am as required in the alpha-spectrometric method. Data obtained on synthetic and real life samples demonstrates the usefulness of the developed alpha/gamma ratio method for the determination of ²⁴¹Am in Pu bearing fuel samples.     

Adsorption and migration of <Superscript>241</Superscript>Am in aerated zone soil

As an important radioisotope in nuclear industry and other fields, ²⁴¹ Am is one of the most serious contamination concerns due to its high toxicity and long half-life. In order to supply useful reference for disposal of ²⁴¹Am waste with low-medium radioactivity, the adsorption and migration behavior of ²⁴¹Am on aerated zone soil were investigated by the static experimental method and column experiments. The results showed that more than 98% of the total ²⁴¹Am could be adsorbed from ²⁴¹Am solution of 0.32·10⁻⁷−1.1·10⁻⁷ mol/l by the soil at pH 4–9. The adsorption of ²⁴¹Am on the soil was a pH-dependent process at pH<4, but for pH>4, the adsorption rate of ²⁴¹Am on the soil changed minutely. The adsorption equilibrium was achieved within 24 hours and no significant effect on adsorption of ²⁴¹Am was observed at liquid-solid ratios of 50:1–500:1. The relationship between concentration of ²⁴¹Am and adsorption capacities of ²⁴¹Am can be described by the Freundlich adsorption equation. Adsorption of ²⁴¹Am on the soil can be inhibited by humic acid, ferric hydroxide colloid, or some anions, such as citric acid anion, saturated EDTA solution, C₂O₄ ²⁻ and CO₃ ²⁻. It was also noted that the adsorption rate of ²⁴¹Am drops in solutions containing Eu³⁺ or Nd³⁺, even 0.5 times above the ²⁴¹Am concentration. A migration distance of 8 mm for ²⁴¹Am(III) is observed only in the aerated zone soil containing ferric colloid, while a migration distance of less than 2 mm is noted in other soil samples after more than 250 days. All these results indicate that the aerated zone soil is an efficient sorbent for ²⁴¹Am and can inhibit the migration of ²⁴¹Am.     

Influence of241Am mobility by sodium humate

The influence of aqueous solution of sodium humate on the transport of²⁴¹Am from the soil into solution and acceleration of movement through a soil layer has been studied. It was found that under static condition the presence of 150 mg sodium humate in 100 ml water accelerates the liberation of²⁴¹Am from soil into the solution. The mobility of²⁴¹Am through a column of soil increased significantly since the concentration of sodium humate in the entering solution exceeded 100 mg.1^–1. Artificially contaminated podsol soil from Brno site and sodium humate isolated by alkaline extraction from sediments of North Bohemian (Duchcov) origin have been used for the investigation.     

Interference from uranium in neutron activation analysis or rare-earths in silicate rocks

A direct nondestructive method of analysis for²⁴¹Am utilizing photon counting and self-absorption correction factors is presented. The method gives favorable agreement for samples analyzed by radiochemical separation procedures and alpha particle spectrometry. The comparison was made over a range of approximately five orders of magnitude of²⁴¹Am concentrations. The method is reliable and relatively simple. Sensitivity for a ∼5-g sample and a counting intervals of 60 000 s is ∼0.2 pCi/g with an uncertainty of ±22%, which decreases to ±11% for increased counting intervals of 150 000 s and an increased sample size of ∼20 g.     

Indirect determination of241Pu activity in soils using low energy photon spectrometers

Actinides activity levels deposited after the Chernobyl accident on the coastal Mediterranean area at Monaco have been recently measured (1). The values obtained are low. However, our -measurements on humic soils from the southern Alps revealed high¹³⁷Cs level contamination areas and urged us to evaluate²⁴¹Pu activity levels. The indirect determination of²⁴¹Pu was based on the -activity measurement of the²⁴¹Am in situ ingrown.     

Determination of <Superscript>241</Superscript>Am/<Superscript>243</Superscript>Am ratios

Determination of ²⁴¹Am/²⁴³Am ratios is required for vanous purposes including assay of Am by isotope dilution techniques. Alpha-spectrometry on electrodeposited sources is a preferred technique for this determination. However, there is an inherent problem of tail contribution which necessitates the use of suitable algorithms to account for the same. Recently, in the frame of a Coordinated Research Program (CRP) of the International Atomic Energy Agency (IAEA), WinALPHA software has been developed which is a combination of an asymmetrical Gaussian for the main part of the peak and a low energy function. Therefore, it was of interest to compare the use of this algorithm with the routinely used method, in our laboratory, based on geometric progression (G. P.) decrease. Since, there are no reference materials available commercially for ²⁴¹Am/²⁴³Am ratios, synthetic mixtures covening a wide range (0.3 to 2.0) of ²⁴¹Am/²⁴³Am α-activity ratios were used and un-ignited electrodeposited sources were prepared for α-spectrometry. The α-spectra obtained using PIPS detector, were evaluated using the two algonthms The ²⁴¹Am/²⁴³Am α-activity ratios obtained were also compared with those determined by thermal ionization mass spectrometry (TIMS). An agreement of about 1% was obtained in the ²⁴¹Am/²⁴³Am ratios determined by the two methods and also by using the two algorithms for α-spectrum evaluation.     

Non-destructive determination of239Pu in wastes by application of γ-ray measurement

Amounts of²³⁹Pu in alpha-bearing wastes were determined by -ray measurement using a NaI/Tl/ scintillation detector. The deviations of measurement caused by the nonuniform distribution of²³⁹Pu in the wastes and by a volume factor were corrected by rotating and scanning the objects. Contribution from²⁴¹Am coexisting with²³⁹Pu was also corrected by taking into account the difference of the counts between A /356–470 keV/ and B /475–620 keV/ intervals. Attenuation of -ray of²³⁹Pu was estimated from the matrix density. Thus the content of²³⁹Pu could be determined within an accuracy of about 25% at the 1 mg level in a cardboard carton of 17 1.     

Sorption characteristics of237Np,238Pu and241Am in sedimentary materials

Adsorption experiments were performed to measure distribution coefficients of²³⁷Np(V),²³⁸Pu(IV) and²⁴¹Am(III) for sedimentary sequential chemical extraction of the adsorbed radionuclides was carried out with water, CaCl₂, KCl, NH₂OH−HCl, K-oxalate and H₂O₂ solutions, to elucidate their dominant sorption mechanisms. The distribution coefficient of²³⁷Np was two orders of magnitude smaller than that of²³⁸Pu and²⁴¹Am. Most of²³⁷Np adsorbed was extracted with CaCl₂ solution and its sorption was controlled by a reversible ion exchange reaction. The adsorbed²³⁸Pu was mainly extracted with NH₂OH−HCl+K-oxalate solution and its sorption was possibly controlled by irreversible reactions.     

Self-absorption effects on alpha-induced atmospheric nitrogen fluorescence yield

Nitrogen fluorescence induced by radiation can be used to detect the presence of radioactive contamination in the environment. Contamination quantification from the fluorescence signal requires: the source’s effective alpha spectrum; the specific radiation quantum fluorescence efficiency; optical attenuation length in air of the fluorescence signal; the absolute throughput and quantum efficiency of the optical instrumentation; calibration of the instrumentation; and radiation transport modeling of the “effective” array exposure rate given the alpha particle spectrum. Field testing conducted on optical instrumentation measured the nitrogen fluorescence yield generated by ²⁴¹Am alpha emissions. Laboratory studies of ²⁴¹Am via alpha spectrometry determined whether the presence of solids on source surfaces produced sufficient self-absorption to decrease fluorescence. Results from the laboratory studies provided correction to the effective alpha-source activity values in a model of the earlier optical-sensor field measurements, and determined the air fluorescence efficiency of alpha particles generated by the ²⁴¹Am sources used in the field experiments.     

Measurements of nuclear data of minor actinides for transmutation of high-level waste

For nuclear transmutation of minor actinides, delayed neutron emission measurement for²⁴¹Am was carried out in thermal neutron irradiation location. The neutron capture cross sections of²⁴¹Am were also measured radiochemically. The transmutation process of²⁴¹Am in reactor is discussed by calculating the yields of minor actinides with the nuclear data measured in this study and the evaluated values. The accelerator driven transmutation of minor actinides by high-flux neutrons from spallation reactions is also presented.     

Behaviour of239,240Pu and241Am in the Baltic Sea; Measurements and interpretation in 1980–1984

Concentrations of^239,240Pu and²⁴¹Am in filtered seawater, particulate fraction and sediment were measured. Methods for determination of these nuclides were critically chequed and a new rapid method for²⁴¹Am in sediment was developed. Due to seasonal variation a significant decrease of plutonium and americium concentrations in surface water takes place in summer. Americium is more efficiently associated with particulate matter than plutonium. From May 1980 to September 1984 soluble plutonium in the water was reduced to about half. The residence half-time of^239,240Pu in the water of Baltic Sea is of the order of 5 years. About similar concentrations of^239,240Pu and²⁴¹Am were found in particulates in water as in the surface layer of the sediment. The average K_d-values for plutonium and americium were 10⁵ and 10⁵–10⁶ ml/g, respectively.     

The determination of Br,Ag and I in pharmaceuticals using X-ray fluorescence excited by gamma sources

The possibility of using γ-radiation sources for the X-ray fluorescence analysis of Br, Ag, and I was studied on model samples. The results were applied for the determination of these elements in pharmaceutical products. The optimum channel range was selected and the accuracies obtainable with various types of radiation sources were compared. For routine analysis of pharmaceutical products and other substances of similar composition, the most suitable radiation sources are:¹²⁵I for the determination of low concentration of bromine;¹⁵³Gd for the determination of silver; and²⁴¹Am for that of iodine.     

Fallout241Am concentration in food and human tissue

Americium and plutonium concentrations in food samples and human tissue samples were determined using alpha-ray spectrometry.Food samples, representative of the average dietar intake over a period of 30d in Japan, were pruchased in Akita during 1985 and 1986. The food was divided into six groups: cereals, vegetable, fruits/beans, seaweeds, fish/shellfish, and meats/eggs/milk. Most of the. total ingestion of both Pu and Am was contributed by seaseed and fish/shellfish. The concentration of Am in the other food groups was low.A compoarison of the measured²⁴¹Am/^239+240Pu ratio in human liver with the predicted value of the ICRP-30 or ICRP-48 model showed that the half-life of Am in the liver is approximately 2–10y. The human tissue samples were obtained from subjects who died in Akita and Niigata Prefectures in northern Japan during 1981–1984. The median concentration of²⁴¹Am was 1.4 mBq/kg-wet in the stemum (n=11), 3.4 mBq/kg-wet in the liver (n=19), and 0.5 mBq/kg-wet in the lung (n=15). The ratio of²⁴¹Am/^239+240Pu was 0.34 in the sternum, 0.12 in the liver, and 0.14 in the lung.     

Reinvestigation of low-lying levels of231Th

Low-lying excited levels of²³¹Th fed through α-decay of²³⁵U were investigated by using α-γ and γ-γ coincidence technique. From the analyses for co-relating energy levels and transition intensities, we found that the most favorable transition from 205.3 keV ([631]7/2) level that is fed by the most dominant α transition from²³⁵U is 19.6 keV transition (205.3 keV [631]7/2⁻→185.7 keV [631]5/2⁻). We also found that the transition probability of 109.2 keV, 205.3 keV [631]7/2⁻→96.1 keV [633]9/2⁺, was corrected to be weak. These findings can explain why the 185.7 keV γ-ray is so strongly observed, 0.57 photons/ga, in the γ-spectrum associated with the α-decay of²³⁵U. The decay scheme of²³¹Th levels previously reported has been modified according to the present analysis.