Multielement analysis of uraniferous rocks by INAA: Special reference to interferences due to uranium and fission of uranium

The presence of uranium in a sample enhances the true values of La, Ce, Nd, Sm determined by INAA if appropriate corrections are not made for the interference. The enhancement of the true values comes about because the (n, γ) activation products of these elements, viz.¹⁴⁰La,¹⁴¹Ce,¹⁴⁷Nd,¹⁵³Sm, are also produced from the fission of²³⁵U (～0.72% natural isotopic abundance) even when La, Ce, Nd, Sm are totally absent in the given sample. In a 5 hour irradiation 1 μg of U is found to be equal to 0.28 μg of Ce and 0.23 μg of Nd while the equivalent La is found to be dependent upon the delay from end of irradiation to sample counting time. A numerical procedure is given to correct for these interferences. Spectral interferences from fission and (n, γ) β products of uranium in the determination of other trace elements by INAA is also investigated. Uranium is found to be determined best using the 278 keV gamma-ray of²³⁹Np.     

Determination of uranium fission interference factors for INAA

Instrumental neutron activation analysis (INAA) is a very suitable technique for the determination of several elements in different kinds of matrices. However, when the sample contains high uranium concentration this method presents interference problems of uranium fission products. The same radioisotopes used in INAA are formed in uranium fission. Among these radioisotopes are ¹⁴¹Ce, ¹⁴³Ce, ¹⁴⁰La, ⁹⁹Mo, ¹⁴⁷Nd, ¹⁵³Sm and ⁹⁵Zr. The purpose of this study was to evaluate uranium fission interference factors to be used in the INAA of environmental and geological samples containing high levels of U. The obtained interference factors agreed with literature reported values. The results point to the viability of using these experimentally determined interference factors for the correction of uranium fission products.     

Determination of rare earth elements in the biological reference materials Pine Needles and Spruce Needles by neutron activation analysis

Instrumental neutron activation analysis was applied to determine La, Ce, Nd, Sm, Eu, Tb, Yb, Lu and Sc in two biological reference materials: NIST 1575 Pine Needles and BCR-CRM 101 Spruce Needles. The purpose was to contribute to the reference data for these two reference materials. The results were obtained with a good precision (relative standard deviations less than 15%). For the Pine Needles reference material there are already some proposed values and our results showed, in general, a good agreement with the data published. The contribution of uranium fission products to La, Ce, Nd and Sm was evaluated and considered in the determination of these elements. Interferences in the determination of rare earth elements in biological materials are also discussed.     

Correcting for uranium fission in instrumental neutron activation analysis of high-uranium rocks

Failure to correct for fission products of²³⁵U is shown to result in significant errors in the measured concentrations of La, Sm, Nd, Ba, Zr, and Mo by Instrumental Neutron Activation Analysis of high uranium rocks. Measured and calculated correction factors are presented as the ratio of the fission product to parts per million by weight of uranium in the rock. Potential errors in petrogenetic interpretations of uncorrected data are outlined.     

A compilation of infinite dilution resonance integrals,II

In this second part the list of resonance integrals is completed with 63 values for (n, γ) reactions mainly from the second part of the periodic system. The resonance integral for (n, fission) of²³⁵U is included as well as thermal and epithermal self-shielding curves for the elements Sm, Eu, Gd, Dy and Cd.     

Determination of rare earth elements in recent and fossil shells by radiochemical neutron activation analysis

Seven rare earth elements (La, Ce, Sm, Eu, Tb, Yb and Lu) in marine shell samples were determined by neutron activation analysis. In order to measure γ-ray using a Ge(Li) detector without serious interference from the intense Compton background from²⁴Na, a simple radiochemical separation was performed by a co-precipitation method with hydrated iron(III) oxide. The chemical yields for shell samples (91–99%) were determined by a re-activation technique for Gd and Yb. The interference from the²³⁵U(n, fission) reaction was corrected for determination of La and Ce. The data obtained in this study showed the behavior of rare earth elements in shells during the process of fossilization.     

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%).     

Application of 14 MeV neutron activation analysis to the determination of Ce and Sm markers in biological materials

The rare-earth elements are very suitable multiple particulate markers for the investigation of matter flow in the gastro-intestinal tract of animals by means of the indicator activation method. A rapid determination of cerium and samarium in biological samples is possible with the aid of a 14 MeV neutron generator. The activity of^139mCe has to be corrected for the interferences of²⁸Al and^143mSm. For the determination of samarium the radionuclides¹⁵⁵Sm and¹⁵³Sm are used. In order to increase the specific activity of these nuclides, which are produced mainly by means of nuclear reactions with thermal neutrons, the samples are irradiated inside a polyethylene moderator block. The deviation from the linearity of the calibration curve for samarium is discussed.     

Yields of rare earth fission products in the spontaneous fission of californium-252

Cumulative fission yields of rare earth isotopes have been determined in the spontaneous fission of²⁵²Cf by fast radiochemical separation and gamma-ray spectrometry. The determined yield values are compared with the available literature data. The yield values for¹⁴⁷Nd,¹⁵¹Nd and¹⁵¹Pm differ from the reported values. The yield for¹⁴⁵Ce is determined for the first time.     

Sequential separation of transuranic elements and fission products from uranium metal ingots in electrolytic reduction process of spent PWR fuels

A sequential separation procedure has been developed for the determination of transuranic elements and fission products in uranium metal ingot samples from an electrolytic reduction process for a metallization of uranium dioxide to uranium metal in a medium of LiCl-Li₂O molten salt at 650 °C. Pu, Np and U were separated using anion-exchange and tri-n-butylphosphate (TBP) extraction chromatography. Cs, Sr, Ba, Ce, Pr, Nd, Sm, Eu, Gd, Zr and Mo were separated in several groups from Am and Cm using TBP and di(2-ethylhexyl)phosphoric acid (HDEHP) extraction chromatography. Effect of Fe, Ni, Cr and Mg, which were corrosion products formed through the process, on the separation of the analytes was investigated in detail. The validity of the separation procedure was evaluated by measuring the recovery of the stable metals and ²³⁹Pu, ²³⁷Np, ²⁴¹Am and ²⁴⁴Cm added to a synthetic uranium metal ingot dissolved solution.     

High-Precision Measurements of the 143Nd/144Nd Isotope Ratio in Certified Reference Materials without Nd and Sm Separation by Multiple Collector Inductively Coupled Plasma Mass Spectrometry

We present a precise and accurate method for the determination of ¹⁴³Nd/¹⁴⁴Nd isotope ratio without Nd and Sm separation by multiple collector inductively coupled plasma mass spectrometry. We corrected instrumental mass discrimination by applying the natural constant ¹⁴⁶Nd/¹⁴⁴Nd ratio as an internal standard after isobaric interference correction of ¹⁴⁴Sm on ¹⁴⁴Nd using interference-free ¹⁴⁷Sm/¹⁴⁹Sm ratio for Sm mass fractionation. The present method was validated by duplicate analyses of several certified reference materials after dissolution and cation-exchange resin purification. The precision (2σ) of the ¹⁴³Nd/¹⁴⁴Nd ratio is less than 10 ppm (internal) and 20 ppm (external), respectively.     

Spontaneous fission yields for 238U in molybdenum measured in Archaean zircons

The relative cumulative fission yields of ^95,97,98,100Mo produced by spontaneous fission of ²³⁸U contained in Archaean zircons, were measured by sensitive thermal ionization mass spectrometry (TIMS). The relative yields for ^95,97,98,100Mo are 0.58 : 1.08 : 1.04 : 1.0, respectively. Combined with mass spectrometrically-determined ^{99,101,102,104}Ru fission yields,¹ the mass distribution from 95￡A￡104 can be delineated. Assuming an “absolute” fission yield of 6.1±0.4% for the cumulative fission yield at mass 97, it is possible to express the Mo and Ru relative spontaneous fission yields for ²³⁸U as “absolute” values. There is no evidence for a significant isotope anomaly at mass 98. This revised version was published online in July 2006 with corrections to the Cover Date.     

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.     

Separation of rare earth,nuclear-fuel burn-up monitors in the 10−9 mole range by high-pressure liquid chromatography with UV-detection

Anion-exchange chromatography of the rare earth (Sm, Nd, Pr, Ce) ions in methanol-nitric acid-water media is performed using high-pressure liquid chromatography. The separation method is especially designed for determination of¹⁴⁸Nd in the nuclear fuel cycle in order to find precise burn-up values. The high-pressure liquid chromatography method presented here is very fast, gives high resolutions, and enables collection of selected fractions containing nmoles of rare earth by UV monitoring at 280 nm of the eluate.     

Some investigations of sea sands from the Black Sea coastline

Alpha to spontaneous fission branching ratios of heavy actinides such as²³⁸Pu and²⁴⁰Pu in solution have been determined by solid state nuclear track detectors (SSNTDs). The detectors used in the present studies are LR-115, CR-39 (DOP), Lexan polycarbonate and Tuffak polycarbonate. Before using Tuffak polycarbonate, a detailed and systematic study on the registration and chemical etching characteristics of fission fragment tracks in this detector was also carried out. The experimentally measured values of alpha to spontaneous fission ratios by this method are found to agree well with the expected values.     

Massen- und Ladungsverteilung bei der Spaltung von 249Cf mit thermischen Neutronen. Vorläufige Mitteilung

The distribution of mass and charge in the thermal-neutron-induced fission of ²⁴⁹Cf has been investigated by radiochemical determination of the fission yields of 25 mass chains and one shielded nuclide (independent yield). The mass distribution is asymmetric, as in all known cases of low-energy fission. The fission yield data indicate a value of 6 ± 1.5 for v , the average number of neutrons emitted per fission. The division of nuclear charge, as indicated by the independent yield of ¹³⁶Cs, is consistent with the equal charge displacement hypothesis characteristic of low-energy fission.     

Determination of <Superscript>151</Superscript>Sm and <Superscript>147</Superscript>Pm using liquid scintillation tracer methods

The long-lived rare earth isotopes ¹⁵¹Sm (90 years, β _max = 76.3 keV) and ¹⁴⁷Pm (2.62 years, β _max = 224.6 keV) are low-yield fission products that generally require lengthy separation procedures to isolate and count by their beta emissions. We will describe novel liquid scintillation counting techniques using radioactive tracers to determine radiochemical yields from an environmental matrix. The recovery of ¹⁵¹Sm is determined from the alpha decay (2.25 MeV) of ¹⁴⁷Sm in the natural Sm carrier and is in excellent agreement with the gravimetric recovery. The ¹⁴⁷Pm recovery is determined by the use of ¹⁴⁵Pm (17.7 years, EC) tracer, custom-produced at LANL using an isotopically enriched target of ¹⁴⁴Sm. We have determined the ¹⁴⁵Pm recovery both from the 37.4 keV k_α1 X-ray, and the electron-capture emissions by LSC. A comparison of these recovery methods is presented.     

Absolute fission yields in the fast neutron induced fission of 233U by track etch combined with gamma-ray spectrometry

The absolute fission yields of twenty seven fission products were determined in the fast neutron induced fission of ²³³U, employing track etch in combination with gamma-ray spectrometry. The total number of fissions was measured by registering the fission tracks on a small strip of lexan, a solid state track detector. The fission products were analysed by gamma-ray spectrometry. The measured yield values were compared to the ENDF/B-VI compilation and show a good agreement.     

Isotope shifts and electronic configurations of the odd parity energy levels of singly ionised samarium

Isotope shift ΔT (148–154) has been evaluated for twelve low-lying even and 89 odd parity levels of singly ionised samarium (Sm II) from the isotope shift (IS) studies in 182 spectral lines of Sm II in the 3890–4525 Å region. These studies were carried out on a recording Fabry-Perot spectrometer using eriched isotopes¹⁴⁸Sm (96%) and¹⁵⁴Sm (98%) excited in liquid nitrogen-cooled hollow-cathodes. Earlier data on isotope shifts are available for only eight lines in this region. It has been found that for a few spectral lines there are errors both in magnitudes and signs of isotope shifts, reported earlier. Most of the 89 odd parity levels of Sm II, for which ΔT values have been evaluated presently, have in literature either no electronic configuration assignments or only tentative assignments. We have suggested the leading configuration for most of these odd levels of Sm II on the basis of ΔT values evaluated in the present studies.     

Analyse par spectrometrie gamma directe des produits de fission de235U

The γ-spectra of fission products of²³⁵U are analysed by a Ge(Li) detector after colling times of 3, 7 and 110 hrs. The possibility of the use of these results is demonstrated for measuring the mass distribution. Some preliminary values for the fission of²³²Th by 14 MeV neutrons are given.