Plutonium fractionation in southern Baltic Sea sediments

In this study, different chemical plutonium fractions (dissolved in water, connected to carbonates, connected to oxides, complexed with organic matter, mineral acids soluble and the rest) in sediments from the Vistula River estuary, the Gdańsk Basin and the Bornholm Deep were determined. The distribution of ^239+240Pu in analysed sediments samples was not uniform but dependent on its chemical form, depth and the sediment geomorphology. The highest amount of plutonium exists in middle parts of sediments and comes from the global atmospheric fallout from nuclear tests in 1958–1961. According to all analysed fractions, the biggest amount of ^239+240Pu was in the mobile form, connected to carbonate fractions from the Vistula River estuary, the Gulf of Gdańsk and the Bornholm Deep sediments.     

Plutonium isotopes concentration in the ground level air and rain samples from Kraków

The aim of the present work was to look at the background levels of plutonium in air and rain samples. Two sets of Petryanov type filters through which ca. 0.5 Mm³ each of air had passed and two large samples of collected rain (170 L and 182 L) were analysed for the content of plutonium alpha-emitters. In the article the radiochemical procedure applied to these samples is described. Obtained Pu activities in air were 0.5±0.1 nBqm^?3 and 0.7±0.1 nBqm^?3 for²³⁸Pu and 3.1±0.2 nBqm^?3 and 8.3±0.6 nBqm^?3 for^239+240Pu. Activities of rain samples were 7.5±0.7 mBqm^?3 and 14.3±0.8 mBqm^?3 for^239±240Pu and 0.4±0.1 mBqm^?3 and 2.1±0.2 mBqm^?3 for²³⁸Pu, respectively, for the two samples. The most interesting finding is the largely different²³⁸Pu to^239+240Pu activity ratios (from 0.03±0.01 to 0.18±0.01) measured in the samples. This result needs conformation, but as now it suggests different origins of plutonium isotopes in incoming to Kraków air.     

Pu and Am determination in the environment—method development

A high resolution inductively coupled plasma mass spectrometric (HR-ICP-MS) method for the determination of plutonium isotopes, Am and the ²⁴⁰Pu/²³⁹Pu isotope ratio utilising modification of Pu-02-RC Plutonium in Soil Samples, Pu-03-RC Plutonium in Soil Residue—Total Dissolution Method, Pu-11-RC Plutonium Purification—Ion Exchange Technique, Pu-12-RC Plutonium and/or Americium in Soil or Sediments, HASL-300 was developed. Total plutonium concentrations (^239+240Pu) measured in environmental samples by this HR-ICP-MS method were in good agreement with recommended data obtained from a-spectrometry. It was achieved the decreasing of the time to analyze the samples over than 33%.     

Determination of Separated Plutonium,Americium and Curium in Environmental Samples by Sequential Extraction Techniques

A simple, reliable and practical radiochemical method for sequential isolation and determination of plutonium, americium and curium in a wide variety of environmental samples including soils, river sediments and water was developed. The isotopes determined are: ²³⁸Pu, ^239,240Pu, ²⁴¹Am, ²⁴²Cm and ²⁴⁴Cm. The methods involve leaching of soil or sedimental samples with concentrated nitric acid using a pressure digestion technique. Subsequent concentration and separation of nuclides of interest from major matrix elements and other interfering alpha-emitters are carried out by coprecipitation with ferric hydroxide and solvent extractions. Sources suitable for alpha-spectrometry are prepared by electrodeposition from acidic ammonium chloride solution. ²⁴²Pu and ²⁴³Am are used as tracer isotopes of plutonium and americium-curium elements, respectively. Some results of analysis of soils, sediments and water are given. The alpha peaks from ²³⁸Pu, ^239,240Pu and ²⁴²Pu as well as ²⁴¹Am, ²⁴⁴Cm, ²⁴²Cm and ²⁴³Am are well resolved. The entire analytical procedures for plutonium, americium and curium are completed in less than sixteen hours.     

Fragment mass and kinetic energy distribution in isomeric fission of 240Pu

Fragment mass and kinetic energy distributions have been measured for isomeric fission of ²⁴⁰Pu. The mass distribution is asymmetric with the average heavy fragment mass nearly equal to that found for ground state spontaneous fission of ²⁴⁰Pu, but slightly lower than for n_th + ²³⁹Pu-fission. The average total fragment kinetic energy appears to be higher in isomeric fission (179.5_?0.7^+1.5 MeV) than in spontaneous fission from the ground state (176.8 ± 1.8 MeV).     

The Possibility of the Use of Coprecipitation with Lanthanum Fluoride for Preparation of Samples for Alpha-Spectrometric Determination of Plutonium

At present time the content of ²³⁹Pu, ²³⁸Pu especially in biological and environmental samples and nuclear fuels is frequently determinated. After radiochemical separation is plutonium usually electrodeposited on a metallic disk [1, 2]. Alpha-activity is then detected by silicon surface barrier detector.

The method of electrodeposition shows several disadvantages. The solution to be electrolyzed must have a definite composition, certain elements, e.g. iron, must not be present. The method is rather time-consuming and requires special equipment. Several other methods for preparation of samples using coprecipitations [3] or inorganic ionexchangers [4] have been studied. In this work was investigated the possibility of the use of coprecipitation of Pu³⁺ with LaF₃ for preparation of samples for alpha-speetroinetric determination of plutonium.     

Cesium,americium and plutonium isotopes in ground level air of Vilnius

Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of ¹³⁷Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995–2003 of ²⁴¹Am and ^239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m³, respectively. ²³⁸Pu/^239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in ²⁴⁰Pu/²³⁹Pu atomic ratio from 0.30 to 0.19 was observed in 1995–2003.     

Rapid methods for the determination of long-lived radionuclides in environmental samples by ICP-SFMS and radioanalytical techniques

Two improved sample preparation methods for the determination of americium and plutonium (Method 1) and plutonium (Method 2) from environmental samples by inductively coupled plasma sector field mass spectrometry (ICP-SFMS) and alpha spectrometry are presented. Both procedures involve a rapid CaF₂ co-precipitation step for pre-concentration and matrix removal followed by extraction chromatographic separations. The average recovery after sample preparation was better than 85 % for both americium and plutonium. The method developed also focused on the elimination of possible interferences in the mass spectrometric analysis caused by molecular ions (e.g. ²⁰⁸Pb¹⁶O ₂ ⁺ or ²³⁸U¹H⁺) by employing suitable matrix separation prior to ICP-SFMS analysis of the desolvated sample. Isotopes with alpha energies similar to the analytes that may cause interferences in alpha spectrometric analysis were also separated. For ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu and ²⁴¹Am detection limits of 15, 9.2, 14 and 23 fg g⁻¹, respectively were achieved by ICP-SFMS, and 0.1 mBq obtained by alpha spectrometry. The methods developed are especially applicable for monitoring purposes of anthropogenic transuranium elements, as the analysis (sample preparation and ICP-SFMS measurement) can be carried out within 6 hours for one batch of samples.     

Cesium, americium and plutonium isotopes in ground level air of vilnius

Systematic observations of radionuclide composition and concentration in the atmosphere have been carried out at the Institute of Physics in Vilnius since 1963. Increases in activity concentration of radionuclides in the atmosphere were observed after nuclear weapon tests and the Chernobyl NPP accident. At present the radiation situation in Lithuania is determined by two main sources of radionuclides, forest fire and resuspension products transferred from highly polluted region of the Ukraine and Belarus. The activity concentrations of ¹³⁷Cs were measured in two to three days samples while plutonium and americium in monthly samples. The extremely high activity concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am determined in the atmosphere during the Chernobyl accident can be explained by transport of “hot particles” of different composition. Activity concentration in 1995–2003 of ²⁴¹Am and ^239,240Pu isotopes ranged from 0.3 to 500 and from 1 to 500 nBq/m³, respectively. ²³⁸Pu/^239,240Pu activity ratio in measured samples differs from 0.03 to 0.45. A decrease in ²⁴⁰Pu/²³⁹Pu atomic ratio from 0.30 to 0.19 was observed in 1995–2003.     

Radiochemical determination of 237NP in soil samples contaminated with weapon grade plutonium

The Palomares terrestrial ecosystem (Spain) constitutes a natural laboratory to study transuranics. This scenario is partially contaminated with weapon-grade plutonium since the burnout and fragmentation of two thermonuclear bombs accidentally dropped in 1966. While performing radiometric measurements in the field, the possible presence of ²³⁷Np was observed through its 29 keV gamma emission. To accomplish a detailed characterization of the source term in the contaminated area using the isotopic ratios Pu-Am-Np, the radiochemical isolation and quantification by alpha spectrometry of ²³⁷Np was initiated. The selected radiochemical procedure involves separation of Np from Am, U and Pu with ionic resins, given that in soil samples from Palomares ^239+240Pu levels are several orders of magnitude higher than ²³⁷Np. Then neptunium is isolated using TEVA organic resins. After electrodeposition, quantification is performed by alpha spectrometry. Different tests were done with blank solutions spiked with ²³⁶Pu and ²³⁷Np, solutions resulting from the total dissolution of radioactive particles and soil samples. Results indicate that the optimal sequential radionuclide separation order is Pu-Np, with decontamination percentages obtained with the ionic resins ranging from 98% to 100%. Also, the addition of NaNO₂ has proved to be necessary, acting as a stabilizer of Pu-Np valences.     

Determination of plutonium isotopes in low activity waste of NPP origin

The inventory analysis of the alkaline low level liquid radioactive waste collected during more than 30 years of NPP “Kozloduy” operation requires determination of eighteen radioactive isotopes with different decay properties. Plutonium isotopes of interest are Pu-238, Pu-239/Pu-240, and Pu-242. The preliminary investigations of the supernatant phase of model and authentic waste samples showed essential challenges for determination of plutonium due to its various oxidation states and low concentration in the complex matrix. Plutonium concentration was determined in precipitate and supernatant after the calcium phosphate precipitation and in the different fractions of the anion exchange steps. The separation by anion exchange and final purification of plutonium fraction by extraction chromatography on TEVA resin (EiChroM Industries) was studied by variation of plutonium oxidation states. The sources were prepared by micro precipitation with NdF₃ and counted by alpha spectrometry. As a result from the performed experiments, plutonium determination procedure was optimized and applied to real waste samples.     

Characteristics of radionuclide contamination of different zones of Semipalatinsk Nuclear Test Site “Opytnoe pole”

Data on the spatial distribution of radionuclides (²⁴¹Am, ²³⁹Pu, ¹³⁷Cs and ¹⁵²Eu) formed during nuclear explosions of different types near P2 SNTS test site are presented. Radionuclide contamination induced by the explosions varies in the concentrations of individual radionuclides, their proportions and species. Examination of the variations is a crucial task to plan remediation activities as well as those aimed at decrease of radiation risk for population and prevention of repeated contamination. Concentrations of ²⁴¹Am and ^239+240Pu that are the most toxic radionuclides in the area lie in hundred thousands of Bqkg^?1. The most contaminated areas are classified by the radionuclide concentration, ratio and form present in soil.     

Alphaspektrometrische Isotopenverdünnungsanalyse von Plutoniumisotopen in Kernbrennstofflösungen

In einer bestrahlten Kernbrennstofflösung wurde die Plutoniumaktivität mit Hilfe der Isotopenverdünnungsanalyse bestimmt. Dabei wurde ²³⁸Pu als Tracerisotop verwendet. Die Abtrennung des Plutoniums wurde durch Extraktion und die Aktivitätsmessung mit Hilfe der Alphaspektrometrie unter Verwendung von Si-Halbleiterdetektoren vorgenommen. Die Störung durch ²⁴¹Am wurde durch gammaspektrometrische Messung berücksichtigt. Die Genauigkeit der ²³⁸Pu-Aktivitätsmessung und die der Messung der Gesamtaktivität beträgt ungefähr 1,5%. Die Bestimmung des ²³⁹Pu zu ²⁴⁰Pu Verhältnisses war nur mit einem groβen Fehler möglich, entsprechend der nahezu gleichen Alphaenergien dieser Isotope und der komplizierten Peakform. ²⁴¹Pu wurde durch alphaspektrometrische Differenzmessung der nachgebildeten ²⁴¹Am Aktivität bestimmt.

In irradiated nuclear fuel solution plutonium isotops were determined with the help of isotope dilution analysis. ²³⁸Pu was used as a tracer isotope. Plutonium was separated by extraction and the activity was measured by alphaspectroscopy using silicon detectors. Interfering ²⁴¹Am was recognized by gamma spectroscopic measurements. The accuracy of ²³⁸Pu determination and the determination of the total activity amounts to about 1-5%. For the ²³⁹Pu ratio we obtained a value with a large systematic error due to the similar alpha energies of these isotopes in the complicated shape of the peaks. The ²⁴¹Pu activity was determined by alphaspectroscopic difference measurement, and was calculated from the ingrown of ²⁴¹Am activity.     

Photofission of 238Pu, 240Pu, and 242Pu in the energy range 5–10 MeV

The cross sections for the photofission of plutonium isotopes ²³⁸Pu, ²⁴⁰Pu, and ²⁴²Pu in the energy range 5–10 MeV have been measured by using a beam of bremsstrahlung photons from the microtron installed at the Institute of Physics and Power Engineering (Obninsk). The energy regions below the fission barrier and above 6 MeV have been scanned with pitches of 0.05 and 0.1 MeV, respectively. In deriving the absolute cross section for ²³⁸Pu photofission, ²³⁸U photofission has been employed as a reference reaction. In measurements involving ²⁴⁰Pu and ²⁴²Pu nuclei, the neptunium isotope ²³⁷Np, which is characterized by a more regular dependence of the photofission cross section on excitation energy than ²³⁸U, has been chosen for the first time as a reference nucleus. The measured cross sections as functions of energy show resonance structures in the vicinity of the fission threshold that are consistent with those previously observed in the energy dependences of fissilities for corresponding direct reactions. The partial-wave cross sections for the J ^π K = 1^?0, 1^?1, and 2⁺0 photofission channels have been determined as functions of energy. At energies below some 5.5 MeV, the total cross section for photofission of each plutonium isotope being studied receives a significant contribution from quadrupole interaction. Within the one-dimensional model of a two-humped fission barrier, the parameters of the barriers for ²³⁸Pu, ²⁴⁰Pu, and ²⁴²Pu have been extracted from data and have then been compared with estimates based on previous measurements.     

Transmutation of 129I, 237Np, 238Pu, 239Pu, and 241Am using neutrons produced in target-blanket system ‘Energy plus Transmutation’ by relativistic protons

Target-blanket facility ‘Energy + Transmutation’ was irradiated by proton beam extracted from the Nuclotron Accelerator in Laboratory of High Energies of Joint Institute for Nuclear Research in Dubna, Russia. Neutrons generated by the spallation reactions of 0.7, 1.0, 1.5 and 2 GeV protons and lead target interact with subcritical uranium blanket. In the neutron field outside the blanket, radioactive iodine, neptunium, plutonium and americium samples were irradiated and transmutation reaction yields (residual nuclei production yields) have been determined using γ-spectroscopy. Neutron field's energy distribution has also been studied using a set of threshold detectors. Results of transmutation studies of ¹²⁹I, ²³⁷Np, ²³⁸Pu, ²³⁹Pu and ²⁴¹Am are presented.      

Hyperfine interactions and charge distributions of actinide ions recoiling into vacuum

The angular distribution of conversion electrons from the 4⁺→2⁺ transition in the ground-state rotational band of²⁴⁰Pu has been measuredvia the²³⁸U (α,2n)²⁴⁰Pu reaction. The electrons are emitted in flight from the Pu nuclei recoiling into vacuum atv/c?0.2%. The attenuation of the angular distribution by extranuclear fields is found to be less than 20% within 120 ps. The hyperfine interactions are discussed with particular attention to the high charge states of actinide recoil ions following internal conversion. Charge distributions ranging up to 45⁺ have been observed for²⁴⁰Cm nuclei in the²³⁹Pu(α,3n) reaction.     

237Np separation from environmental matrices by extraction chromatography method

Aliquat-336 anchored on hydrophobized silica gel was used for effective separation of ²³⁷Np from soil matrices and from model solutions. Alpha spectrometry for ²³⁷Np determination was used. The interfering radionuclides present in environmental samples such as ²³⁴U, ²³²Th, ²³¹Pa and ^239+240Pu were removed by separation with nitric acid solutions containing formic acid and ferrous sulfamate as reducing agents. Spiking samples with ^238,234U, ²³²Th and ²³⁸Pu were used to check separation effectiveness. A separation yield of ²³⁷Np from soil matrices was checked by measuring of added known amount activity and was found to be about 15%. The yield of separation for model solutions was about 56%. Different parameters of eluant on recovery of ²³⁷Np from column were studied.     

氢化钚与CO反应体系的耦合效应

氢化钚与CO反应体系有七个独立组分、四种元素和三个独立反应方程式,分别计算了CO(g)、CO2(g)和H2(g)在同时反应和单独反应中的平衡组成。计算表明：同时反应有耦合作用,低温有利于CO(g)的转化和Pu2O3(s)的生成。与单独反应相比,体系中有较多的Pu2O3(s)生成,其平衡组成也有较大差异。计算结果对钚的表面防腐有一定的参考价值。     

Determination of isotopic composition of plutonium in hot particles of the Chernobyl area

The knowledge of the isotopic composition of man-made transuranium elements (TUE) in the environmental samples is of great interest because, on the basis of these data, statements about the origin of the TUE can be made. One of the most radiotoxic elements released during reactor accidents and nuclear weapons tests was plutonium with the alpha emitters ²³⁸Pu, ²³⁹Pu, ²⁴⁰Pu, ²⁴²Pu and the beta-emitter ²⁴¹Pu which decays into ²⁴¹Am. The determination of plutonium in “hot” particles from the Chernobyl reactor was accomplished by means of solid state nuclear track detectors registering the alpha particles and by alpha spectroscopy after chemical treatment. Furthermore, in order to perform a complete analysis of the isotopic composition one of the “hot” particles has been investigated by resonance ionization mass spectrometry which possesses an excellent sensitivity and a good isotopic resolution.     

Sulphur and Oxygen Isotopes in Sulphates in Natural Waters: (2) Deep-Waters from Horizons Below Baltic Sea Floor

Abstract

In this paper we consider deep waters from horizons located under the Baltic-Sea bottom. The samples were taken twice from wells bored in Hel peninsula. The δ¹⁸O and δD values of these waters show their glacial origin since they have significantly low values (δ¹⁸O from ?14 to ?11 whereas the modern groundwaters in Gdańsk area have ?10%₀). In contrast to surface waters the sulphates dissolved in these deep waters have rather high and uniform δ¹⁸O values which are correlated with δ¹⁸O of H₂O but not correlated with δ³⁴S. The isotope patterns may be explained assuming that the waters are very old, in which the slow process of oxygen isotope exchange at low temperatures, but extended in time, could enrich the sulphate in heavier oxygen isotopes.