Fission product yields in the fast-neutron fission of238U

The fission yields of 38 fission products in the fast-neutron induced fission of²³⁸U have been determined using a rapid, multiscaling gamma-ray spectroscopic method. To obtain absolute yields for fission products having half-lives ranging from 32 s to 40 d, a total of 56 multi-scaling gamma-ray spectra were collected using various irradiation and cooling periods. Gamma-rays and photopeak areas of interest were assigned to the fission products by their energies and half-lives. Fission product activities were evaluated from spectral data using growth and decay calculations and fission yields were determined by normalizing the¹⁴⁰Ba yield to the average value from reported data. The depleted uranium target, covered with a boron-cadmium thermal neutron shield, was used to keep interference from the fission of²³⁵U minimal. Results for the cumulative fission yields, including 17 mostly short-lived fission products measured for the first time, are compared with previous measurements and with the recommended yields in recent evaluations. The agreement, and some discrepancies, in the comparisons are discussed. No explicit even-odd pairing effects are observed in the fission yield data for fast-neutron induced fission of²³⁸U.     

Nuclear decay studies of fission-product nuclides using an on-line mass separation technique

An isotope-separator-on-line (ISOL) system has been developed at the Idaho National Engineering Laboratory to enable a wide variety of nuclear decay studies to be made for fission-product radionuclides. The system is unique in that it utilizes the spontaneous fission source,²⁵²Cf, as the source of fission-product radioactivity. Fission products are transported to the ion source of the mass separator by the helium gas-jet technique. Mass-separated beams of previously unattainable rare-earth nuclides are produced with this system because of the higher yield of fission products with A>150, relative to that for thermal-neutron fission of²³⁵U, and the use of a relatively efficient ion source. Recent decay studies reported here include systematic measurements of rare-earth nuclide half-lives and comparison of them to theoretical prediction, a decay scheme investigation for¹⁵⁴Nd, and -strength function measurements for¹⁴⁰Cs.     

Determination of the 238U spontaneous fission decay constant without neutron irradiation

We have developed a methodology for measuring the decay constant of the spontaneous fission of ²³⁸U, l_f, using nuclear particle track detectors where thermal neutron irradiation is unnecessary. This methodology is based on the fact that the radiation damage caused by spontaneous fission of trans-uranium elements bearing a mass number close to 238 are similar to ²³⁸U spontaneous-fission ones. Loading a thick source of uranium (thickness greater than the fission fragment range) with a small amount of a suitable trans-uranium element (for instance, ²⁴²Pu, which presents a spontaneous fission half-life of 6.75^.10¹⁰ y), it is possible to determine the observation efficiency of a particle-track detector for fission fragments. Procedures concerning our thick source manufacture and uniformity tests of the trans-uranium distribution are also presented. These results make it possible for the exposure of thick uranium sources (without trans-uranium element) to lead to a l_f value.     

Elution of 235U fission products through a calcined hydrotalcite-packed column

Calcined hydrotalcite packed columns were utilized to sorb ²³⁵U fission products and their decay products. The elution behavior of some radionuclides was studied after washing the columns, either with distilled water or 0.5% NaCl solution. Afterwards, fission products and their decay products were eluted using 0.5% NaCl solution. It was found that no matter the washing process, ^99mTc, the b^--decay product of ⁹⁹Mo, was easily separated from ⁹⁹Mo which was strongly retained on the hydrotalcite. ¹³²I, the b^--decay product of ¹³²Te, was eluted slowly and was separated from ¹³²Te which was retained on the column. ¹³¹I and ¹⁴⁰Ba were eluted together with ^99mTc and ¹³²I, although in smaller proportions.     

On line ion exchange separation of short-lived Zr, Hf, Mo, Ta and W isotopes as homologs of transactinide elements

The short-lived isotopes of W and their descendants have been separated from nuclear reaction products arising in the bombardment of samarium target with²⁴Mg ions at the U-400 cyclotron of JINR-Dubna. Chemical separations were performed using previously elaborated fast and continuous ion exchange. In similar way products of²³⁵U fission, obtained at the microtron MT-25 during irradiation of²³⁵U target with photoneutrons were separated.     

Measurements of fission yield in 8 MeV bremsstrahlung induced fission of 232Th and 238U

The cumulative yields (i.e. the sum of isobaric independent yield up to the isobar of interest) for various fission products have been determined in the 8 MeV bremsstrahlung induced fission of ²³²Th and ²³⁸U by using off-line gamma ray spectrometric technique. From the cumulative yields of the fission products, their mass-chain yields (i.e. the sum of independent yields of all the isobars) were obtained by using charge distribution correction. The mass-chain yields in the ²³²Th(γ, f) and ²³⁸U(γ, f) reactions were compared with the data of similar excitation energy in the ²³²Th(n, f) and ²³⁸U(n, f) reactions to examine the effect of nuclear structure. From these data, it was found that the yields of fission products for the mass numbers 133–134, 138–140 and 143–144 as well as their corresponding complementary products are significantly higher than other fission products. Higher yields of the fission products around the mass numbers 133–134 and 143–144 were explained from the standard I and standard II asymmetric mode of fission, which indicates the role of shell closure proximity. However, the amplitude of yields for the mass numbers 133–134 and 143–144 are reverse in the ²³²Th(γ, f) and ²³²Th(n, f) reactions than in the ²³⁸U(γ, f) and ²³⁸U(n, f) reactions, which has been explained from the point of shell combinations of the complementary fragments.     

The determination of fission products in irradiated uranium by electrophoretic focussing of ions

Electrophoretic focussing of ions was applied to the separation of fission products present in solutions of nuclear uranium fuel irradiated in various European reactors. By combining two separation methods, all the long-lived fission products could be determined individually and quantitatively by counting with a NaI(T1) and a GM detector of known detection efficiency. Radiography and autoradiography were used for semi-quantitative purposes. The concentrations of²³⁵U and²³⁸U were determined from a short post-irradiation of the fuel solution and counting of¹⁴⁰Ba−¹⁴⁰La and²³⁹Np, respectively. An iterative calculus method is presented which allows calculation of the irradiation history of the fuel solution from the above analyses. without any a priori knowledge.     

Determination of uranium,plutonium and selected fission products in the coolant of the KS-150 reactor

The method of monitoring of U, Pu and some fission products (^103,106Ru,^134,137Cs and^141,144Ce) in gaseous CO₂ coolant is described. The method is based on the retention of the radionuclides studied by membrane filters built in by-pass of the burst-cartridge detection (BCD) system. The purpose of the present study was the determination of U, Pu in CO₂ and the verification of the possibility of the indirect monitoring of U and Pu contents in the coolant, using the gamma-spectrometric determination of selected fission products retained by the filter. For calibration of the proposed method after decomposition of the filters, uranium was determined spectrophotometrically using Arsenazo III, plutonium was determined radiometrically after its separation by extraction with 2-thenoyltrifluoracetone and the fission products were determined by gamma-spectrometry. From the results obtained it follows that a correlation exists between the U and Pu content in the coolant and the activity of certain fission products retained on the filter.     

Uranium enrichment measurements using the intensity ratios of self-fluorescence X-rays to 92 keV gamma ray in UXKα spectral region

In this paper, the known multigroup γ-ray analysis method for uranium (MGAU) as one of the non-destructive γ-ray spectrometry methods has been applied to certified reference nuclear materials (depleted, natural and enriched uranium) containing ²³⁵U isotope in the range of 0.32-4.51% atom ²³⁵U. Its analysis gives incorrect results for the low component ²³⁵U in depleted and natural uranium samples where the build-up of the decay products begins to interfere with the analysis. The results reveal that the build-up of decay products seems to be significant and thus the algorithms for the presence of decay products should be improved to resulting in the correct enrichment value. For instance, for the case of ²³⁵U analysis in depleted uranium or natural ore samples, self-induced X-rays such as 94.6 keV and 98.4 keV lying in UXK_α spectral region used by MGAU can be excluded from the calculation. Because the significant increases have been observed in the intensities of uranium self-induced X-rays due to γ-ray emissions with above 100 keV energy arising from decay products of ²³⁸U and ²³⁵U and these parents. Instead, the use of calibration curve to be made between the intensity ratios of self-fluorescence X-rays to 92^* keV γ-ray and the certified ²³⁵U abundances is suggested for the determination of ²³⁵U when higher amounts of decay products are detected in the γ-ray spectrum acquired for the MGAU analysis.     

The role of NAA in nuclear chemistry education

One of the missions of our Institute is the promotion of basic nuclear teaching for students as well as professional teaching for workers in nuclear industry and research. For nuclear chemistry education, we present here a one day teaching course on radioactive decay and nuclear reactions, and a two or three days course based on reactor irradiation of uranium oxide, instrumental and radiochemical analysis of fission products. In the first experiment, the neutron capture is presented as an example of nuclear reaction; the neutron activation of a silver coin with a Am-Be neutron source, followed by γ-ray spectrometry, is used to identify three radionuclides of silver and to calculate their half-lives. In the second experiment, our teaching reactor is used as a neutron source with a flux about 10¹⁰ n·cm⁻²·s⁻¹ at a low thermal power (10 kW). This low flux allows us to irradiate a small uranium sample which is usable for spectrometry after a short cooling time of about two hours. The first day is reserved for instrumental analysis of the fission products and a second day for the radiochemical separation of a fission radionuclides. With these experimental results, the students have to calculate the number of fissions in the irradiated sample. On optional third day for postgraduate students is devoted to the presentation of NAA and some applications as uranium determination by the fission product spectrometry.     

New approaches to reprocessing of oxide nuclear fuel

Dissolution of UO₂, U₃O₈, and solid solutions of actinides in UO₂ in subacid aqueous solutions (pH 0.9–1.4) of Fe(III) nitrate was studied. Complete dissolution of the oxides is attained at a molar ratio of ferric nitrate to uranium of 1.6. During this process actinides pass into the solution in the form of U(VI), Np(V), Pu(III), and Am(III). In the solutions obtained U(VI) is stable both at room temperature and at elevated temperatures (60 °C), and at high U concentrations (up to 300 mg mL^?1). Behavior of fission products corresponding to spent nuclear fuel of a WWER-1000 reactor in the process of dissolution the simulated spent nuclear fuel in ferric nitrate solutions was studied. Cs, Sr, Ba, Y, La, and Ce together with U pass quantitatively from the fuel into the solution, whereas Mo, Tc, and Ru remain in the resulting insoluble precipitate of basic Fe salt and do not pass into the solution. Nd, Zr, and Pd pass into the solution by approximately 50 %. The recovery of U or jointly U + Pu from the dissolution solution of the oxide nuclear fuel is performed by precipitation of their peroxides, which allows efficient separation of actinides from residues of fission products and iron.     

Specific activities of radioactive elements from fission product mixtures

Specific activities of radioactive elements at the time of chemical separation from fission product mixtures produced by thermal neutron fission of²³⁵U were computed byBateman's and other equations on an electronic computer. Computations were made for two fission times: fission was assumed to be complete in a few minutes in one case, and over a period of a year in the other case. It was also assumed that each element was separated instantly after allowing the fission products to decay for 1∼10 000 000 hrs (1 140 years). The computations were applied to 12 important elements: Ru, Zr, Nb, Cs, Sr, Pm, Tc, Ba, La, Ce, Kr and Y. Results are given as a diagram for each element. The diagrams are intended to be helpful in the chemical processing of a large quantity of fission products, and industrial or tracer application of these elements.     

Liquid chromatographic determination of the number of fissions in uranium/aluminium nuclear fuels

Modern liquid-chromatographic (LC) procedures have been developed for the determination of atom% fission in²³⁵U metallic nuclear fuels having atom% fission values 3% to 75%. The diluted dissolved fuel was injected directly into a high-performance LC column, and the eluted metal ions were detected with an on-line reaction system. The fission monitor,¹³⁹La, and the unfissioned U were determined with a precision of 1%, and a comparison with standard mass-spectrometric procedures gave good agreement (1%).     

Isomeric yields of130Sb,132Sb,134I,and136I in the thermal neutron fission of235U

Isomer yield ratios of¹³⁰Sb,¹³²Sb,¹³⁴I and¹³⁶I isomers formed in the thermal neutron fission of²³⁵U have been calculated from our previous experimental studies that led to the identification of these species. In those studies the iodine and antimony fractions formed in fission were rapidly separated and the decay of -rays belonging to each isomer pair were followed using Ge(Li) detectors and a multichannel analyzer. The isomer ratios were calculated from growth and decay considerations of these -rays. The results are compared with the recently published values obtained with an on-line isotope separator, those from LOHENGRIN, and those from model calculations. Angular momenta of fission fragments corresponding to the measured isomer yields have also been calculated.     

Sensitivity study on modeling radioxenon signals from radiopharmaceutical production facilities

As part of the Comprehensive Nuclear Test-Ban Treaty (CTBT), the International Monitoring System (IMS) was established to monitor the world for nuclear weapon explosions. As part of this network, systems are in place to monitor the atmosphere for radioxenon. The IMS routinely detects radioxenon from sources other than nuclear explosions. One of these radioxenon sources is radiopharmaceutical production facilities. This is a sensitivity study on the nuclear forensic signals possible from such facilities. A fission process model was produced to calculate the activity of ^131mXe, ^133mXe, ¹³³Xe and ¹³⁵Xe in the process utilized to produce ⁹⁹Mo and ¹³¹I for medical applications through high enriched uranium fission. The computer model accounts for fractionation of radionuclides within a decay chain that may result from filtering or chemical procedures. Ratios of the radioxenon isotopes are calculated as a function of decay time after the release. The ratios are then compared to those expected from nuclear explosions. The main conclusion from this work is that the two main factors that affect the nuclear forensic signal from radiopharmaceutical production facilities are the sample irradiation time and the use of emission gas storage tanks.     

The separation of99Tc from mixed fission products and its determination by neutron activation

Technetium is separated from the bulk of fission products and other elements in dissolved nuclear fuel by a ferric hydroxide precipitation followed by filtration and loading of the filtrate on an anion exchange resin. The technetium remains on the resin presumably as pertechnate ion. The resin is exposed to a neutron flux in a nuclear reactor activating⁹⁹Tc to¹⁰⁰Tc which decays with the emission of a 539keV gamma-ray with a 15.8 second half-life. This gamma-ray is conveniently counted with conventional solid state techniques.Work performed under contract to the U. S. Department of Energy under contract number DE-ACO7-76IDO1570.     

Nuclear decay studies of rare-earth fission-product nuclides using fast radiochemical separation techniques

A facility for the rapid radiochemical separation of individual rare-earth fission product nuclides from mixed fission products has been developed at the Idaho National Engineering Laboratory (INEL). This facility, called the INEL ESOL (elemental separation on-line) facility, includes an electroplated spontaneously fissioning²⁵²Cf source, a He jet transport system to deliver short half-life fission products from the²⁵²Cf hot cell to the radiochemistry laboratory, and a high pressure liquid chromatograph for the individual separation of rare-earth radioelemental fractions. The fission product collection and separation instrumentation is interfaced to a microprocessor that controls valves, motors and other devices and monitoring instrumentation. The data acquistion instrumentation can be controlled from a signal originating from the microprocessor or initiated manually. The results of some recent decay scheme studies on¹⁵³Pm and¹⁵⁴Pm are reported.     

Fission process and its application in fissile material identification

Summary In this work, prompt gamma-rays emitted by thermal neutron-induced fission decay using fast coincidence techniques are used to identify both light and heavy fragments and obtain gamma-ray signatures and radiation multiplicity. The measurements were carried out with ²³⁵U and ²³⁹Pu targets using the Intense Pulsed Neutron Source (IPNS) at Argonne National Laboratory. This study reports the recent results of a preliminary analysis of experimental data collected from the induced fission of ²³⁵U and ²³⁹Pu. In this paper, we discuss how these results could be used to characterize an unknown sample of fissile material.     

Limit of the INAA procedure for copper determination based on the64Cu 511 keV line

The²³⁵U/²³⁸U ratio is determined by neutron activation analysis counting the ϕ-rays of short half-lives fission products and²³⁹U. The effect of the neutron spectrum hardening using a⁶LiD converter is also demonstrated. The²³⁵U/²³⁸U ratio is determined using short irradiation, waiting and counting times.     

Elemental analysis of biological tissues of Dmdmdx/J and C57BL/6J mice strains investigated by neutron activation analysis

Radioactivity measurement of short-lived nuclides is the basis of decay data measurement, which requires rapid separation and purification of the interested nuclides from complicated fission products. A rapid separation system based on SISAK and extraction chromatography technique was established to isolate ⁹⁵Y, which half-life is 10.3 min. With the best conditions studied in this paper, ⁹⁵Y was separated successfully from complicated fission products under the mini-reactor in the China Institute of Atomic Energy. Decontamination factors to other nuclides except ⁹⁴Y are higher than 2 × 10³.