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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS2020

Cerium Stable Isotope Analysis of Synthetic and Terrestrial Rock Reference Materials by MC-ICPMS

Cerium is the most abundant rare earth element (REE) in the solar photosphere, CI chondrites, and the Earth. It has four main stable isotopes (masses: 136,138,140, and 142), with 138Ce being the most studied species, used in geochronology and petrogenesis. In addition, more abundant 140Ce and 142Ce are suggested to be potentially applicable in geochemical investigations. In this work, we developed a modified four-step ion chromatography procedure for Ce chemical separation. Using a MC-ICPMS, we designed a cup configuration to measure 142Ce/140Ce ratio of the samples with an optimized Nd correction equation. A 0.03‰ (2SD) reproducibility was obtained for Ce Ames metal standard. We analyzed ten different igneous and one sedimentary geochemical reference materials. Mean δ142Ce range from −0.07 to 0.32‰. Most of the samples show a heavier Ce isotopic composition than the Ce Ames standard. The majority of rocks have a homogenous δ142Ce. The δ142Ce does not show any correlation with rock chemical composition including their Ce content or rock types. A carbonatite (SARM 40) has a mean δ142Ce of −0.07 ± 0.13‰ (2SD), lower than the other rocks, suggesting the possibility of a pronounced isotopic fractionation. Our work demonstrates the applicability of the developed methodology and the potential of Ce stable isotopes for future geochemical studies. Production of a larger database of δ142Ce values is required to obtain a clearer view on the similarities and differences between different geological material and explaining Ce stable isotope dynamics.

Cerium↗
DOE OSTI2025

Particle signal considerations for isotope ratio analysis with single particle multi-collector inductively coupled plasma mass spectrometry

Particle analysis has benefitted from the advent of single particle inductively coupled plasma-mass spectrometry (spICP-MS) due to its robustness, sensitivity, and high-throughput nature. Previous methods of spICP-MS have typically utilized quadrupole or time-of-flight mass analyzers and therefore employ electron multiplier-based detectors (such as secondary electron multipliers or microchannel plates). However, to obtain precise measurements on elemental or isotopic ratios within individual particles, multi-collector ICP-MS (MC-ICP-MS) can be used. Here, we investigate Ce isotope ratios, specifically 142 Ce/ 140 Ce, by spMC-ICP-MS using an all-Faraday cup collector array. Using 1 μm (diameter) cerium dioxide particles, integration times of the Faraday cup detectors were varied from 50–500 ms. The signal from the cerium isotopes in the particles was used to determine isotope ratios, which closely matched the expected natural isotopic abundances. Due to the signal decay response from the Faraday cups, the signal from particles lasts much longer than the expected 1–2 ms (up to 100 s of ms). To explore this effect on isotope ratio analysis, multiple ratio analysis methods were used to determine how to obtain optimal precision and accuracy. Relative differences were around 2% for methods that calculated isotope ratios from summing the total signal of an individual particle before calculating the ratio (rather than using every data point individually). It was found that summing all data points per particle, or integrating under the signal peak, yielded both accurate and precise isotope ratios within the particle population. Particles were also sampled off a solid substrate via microextraction, and isotope ratios were determined with relative differences of 0.13% to 9%. This demonstrates the ability to use spMC-ICP-MS to obtain isotope ratios on particles, with little to no relative difference in comparison to the expected ratio, even when operating Faraday detectors at fast 50 ms integration times.

Szakas, Sarah E. [Oak Ridge National Laboratory (O↗
DOE OSTI2014

Sub-nanosecond Half-life Measurement of the Yrast I{sup π}=5{sup −} State in the N=78 Nucleus {sup 136}{sub 58}Ce using Fast-timing Coincident Gamma-ray Spectroscopy

We report on the measurement of the half-life of the yrast I{sup π}=5{sup −} state in the transitional nucleus {sup 136}Ce using a combined HPGe-LaBr3(Ce) scintillator gamma-ray detection array. The measured value for the E1 decay is approximately half a nanosecond, which corresponds to an E1 decay strength of approximately 2×10{sup −6} Wu. This value is in line with single-particle type E1 decays in this mass region and suggests no sign of additional K-hindrance associated with axially symmetric quadrupole deformations observed for lighter cerium isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2011

Nuclear Data Sheets for A = 127

The 1996 evaluation for the A=127 mass chain (1996Ki01) has been revised. The experimental results from various decays and reactions for the A=127 mass chain have been compiled and evaluated. The nuclides covered in this evaluation are from {sup 127}Ag to {sup 127}Nd. The data are summarized and presented, together with adopted level schemes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

R-matrix Resolved Resonance Region Evaluation of 140,142 Ce

Oak Ridge National Laboratory completed the resolved resonance region (RRR) evaluation of the two most abundant cerium isotopes, 140 Ce (88.45%) and 142 Ce (11.11%), as requested by the US Nuclear Criticality Safety Program. These evaluations are based on recent high-resolution transmission and capture measurements performed on nat Ce and highly enriched 142 Ce samples at the JRC-Geel Linear Accelerator facility, as well as measured thermal constants available from the EXFOR database. Starting from the resonance parameters of the ENDF/B-VIII.0 library followed by a preliminary R-matrix analysis, an updated set of resonance parameters and corresponding covariance information were derived by fitting these measured data using the Reich–Moore approximation of the R -matrix theory, as implemented in the SAMMY code system. The 140 Ce RRR upper energy limit was kept at 200 keV, whereas the 142 Ce resonance region was extended from 13 to 26 keV. Updated statistical properties were obtained for the new evaluations and compared to those derived from the ENDF/B-VIII.0 nuclear data library. The new evaluation work improved some of the discrepancies found in previous work, such as the capture resonance integral and stellar Maxwellian-averaged cross sections. These integral quantities were mainly derived from the fit of the latest measured data, especially the neutron capture yield data for 142 Ce isotope.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Status of a New Resonance Evaluation for Cerium to Support Nuclear Criticality Safety Applications

A new resonance evaluation is currently being carried out at Oak Ridge National Laboratory (ORNL) for isotopes of cerium. This new evaluation will provide a much-needed update of the resolved and unresolved resonance parameters for {sup 140}Ce and {sup 142}Ce based on new and existing experimental cross section data. The physics of the resolved resonance region will be greatly improved, and new resonance parameter covariance data will be generated. Cerium exists predominately as {sup 140}Ce and {sup 142}Ce and can be found in chemical processing streams because it is used commercially as a catalyst or additive in chemical applications (e.g., glass polishing powder). Cerium has neutron-absorbing properties that can influence the reactivity of systems with fissionable material. The need for improved cerium cross section data has been identified specifically for the Hanford Plutonium Finishing Plant as part of the Nuclear Criticality Safety Program (NCSP) nuclear data request. Furthermore, cerium is a high-yield fission product, making it relevant for reactor calculations. Currently, ENDF/B-VII.1 evaluations for cerium isotopes (described in Section II) do not include the covariance data needed to support sensitivity/uncertainty analyses of systems involving cerium. In addition, the available cerium resonance parameters in ENDF/B-VII.1 are based on parameters provided in the Atlas of Neutron Resonances: Resonance Parameters and Thermal Cross- Sections. Z = 1-100 by S. Mughabghab; hence, the 'evaluated' resonance parameters are not based on a detailed R-matrix analysis. Furthermore, differential measurements are needed in the resonance region to accurately predict the neutron resonances. ORNL has completed new differential measurements on natural samples of cerium, and measurements of an enriched {sup 142}Ce sample are planned. A corresponding resonance evaluation for {sup 140}Ce and {sup 142}Ce being conducted by ORNL will provide detailed cross section resonance parameters and corresponding evaluated covariance data in the resonance region in support of the NCSP. The target uncertainty requested by the NCSP is on the order of 1-2% for the total cross section and less than 6% for the capture cross section in the resolved resonance region. New cerium resonance evaluations will significantly improve radiation transport calculations for systems involving cerium in processes in the DOE Complex. Also, the new evaluations will provide much-needed evaluated covariance data to support sensitivity/ uncertainty analyses.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2011

Splitting of the Pygmy Dipole Resonance

In recent years investigations have been made to study the electric Pygmy Dipole Resonance (PDR) systematically, mainly in semi-magic nuclei. For this purpose the well understood high resolution ({gamma},{gamma}') photon scattering method is used. In complementary ({alpha},{alpha}'{gamma}) coincidence experiments at E{sub {alpha}} = 136 MeV a similar {gamma}-energy resolution and a high selectivity to E1 transitions can be obtained at the Big-Bite Spectrometer (BBS) at KVI, Groningen. In comparison to the ({gamma},{gamma}') method a structural splitting of the PDR is observed in the N = 82 nuclei {sup 138}Ba and {sup 140}Ce and in the Z = 50 nucleus {sup 124}Sn. The low energy part is excited in ({gamma},{gamma}') as well as in ({alpha},{alpha}'{gamma}) while the high energy part is observed in ({gamma},{gamma}') only. The experimental results together with theoretical QPM and RQTBA calculations on {sup 124}Sn which are able to reproduce the splitting of the PDR qualitatively are presented. The low-lying group of J{sup {pi}} = 1{sup -} states seem to represent the more isoscalar neutron-skin oscillation of the PDR while the energetically higher-lying states seemingly belong to the transitional region between the PDR and the isovector Giant Dipole Resonance (IVGDR).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

The Study of (n, 2n) Reaction Cross Sections for Ce and Nd Isotopes up to 20 MeV

Neutron cross section calculations for {sup 136}Ce(n, 2n){sup 135}Ce, {sup 138}Ce(n, 2n){sup 137}Ce, {sup 140}Ce(n, 2n){sup 139}Ce, {sup 142}Ce(n, 2n){sup 141}Ce, {sup 142}Nd(n, 2n){sup 141}Nd, {sup 144}Nd(n, 2n){sup 143}Nd, {sup 146}Nd(n, 2n){sup 145}Nd, {sup 148}Nd(n, 2n){sup 147}Nd, and {sup 150}Nd(n, 2n){sup 149}Nd were done in the incident energy range from 10 to 20 MeV. The calculations were performed using three codes TALYS-1.6 for two-component Exciton model, EMPIRE-3.2 Malta for Exciton model, and ALICE/ASH for the Geometry-Dependent Hybrid (GDH) model. The results of model calculations were compared with the available experimental data and also with the evaluated data in the TENDL-2015 (based on the modified TALYS code), ENDF/B-VII.1 libraries. The calculated cross section data were compared with the available experimental data obtained from EXFOR and also compared with semiempirical formulas around 14–15 MeV. The results of model calculation were found to be in good agreement with the experimental data given in literature and semiempirical data around 14–15MeV.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1994

REE chemistry and Sm-Nd systematics of late Archean weathering profiles in the Fortescue Group, Western Australia

Two weathering profiles, each consisting of an upper, sericite-rich zone and a lower, chlorite-rich zone, are preserved between flows of the Mt. Roe Basalt in the Fortescue Group, Hamersley Basin, Western Australia. REE concentrations in samples from these two profiles, which originally developed ca 2,760 Ma, show large variations depending on stratigraphic position. LREE abundances and (La/Yb)N are greatest at depths of 3-6 m below the paleosurface of the Mt. Roe #1 profile and are somewhat lower in samples above this level. The LREEs reach concentrations 6-9 times greater than in the underlying basalt, and thus appear to have been mobilized downward in the paleosol and concentrated in its middle part. LREE concentrations in the #2 profile show a similar distribution but with a sharp increase in all REE concentrations within 50 cm of the paleosurface. The distinction between the REE profiles in the two paleosols may be related to the difference in the overlying material. The #1 paleosol is overlain by a few meters of sediments and then by basalt, whereas the #2 paleosol is directly overlain by basalt. The LREEs appear to have been mobilized both during chemical weathering of the parental basalt and during later lower-greenschist-facies metamorphism and metasomatism of the paleosols. Remobilization of the REEs during the regional metamorphism of the Fortescue Group is confirmed by a whole-rock Sm-Nd reference isochron of Mt. Roe #1 samples with an age of 2,151 +/- 360 Ma. Variable initial 143Nd/144Nd values of unweathered basalt samples which may represent the paleosol protolith prevents a confident determination of the magnitude of LREE mobility. Both the initial mobilization of the REEs during weathering and the metasomatic remobilization appear to have taken place under redox conditions where Ce was present dominantly as Ce3+, because Ce anomalies are not developed within the sericite zone samples regardless of concentration. Europium anomalies in the paleoweathering profile are somewhat variable and were probably modified by mobilization of Eu2+ at metamorphic conditions. In all samples, the HREEs appear to have been relatively immobile and correlate with Al, Ti, Cr, V, Zr, and Nb. Sm-Nd systematics and REE patterns of four unweathered basalt samples indicate derivation of the Mt. Roe Basalts from a heterogeneous and enriched source having epsilon Nd between -4.0 and -7.4. Initial 143Nd/144Nd values of these basalts are even lower than those reported by NELSON et al. (1992) for Fortescue Group basalts and indicate a substantial crustal component in the generation of Mt. Roe Basalts.

NASA Discipline Exobiology↗
DOE OSTI2022

Column separation of tetravalent cerium fission products from trivalent rare earth radio-isotopes

Rapid and efficient isolation of individual rare earth element (REE) radioisotopes from complex mixtures is necessary to support the fields of nuclear forensics, medical isotope production and nuclear physics measurements. The separations must be robust and generate sufficiently high purity samples for subsequent radiological analysis. Current methodologies utilize a laborious two step Ce(IV)-iodate precipitation followed by Ce(IV)-nitrate di-(2-ethylhexyl)phosphoric acid/n-heptane extraction. This work reports an alternative method to isolate Ce fission product isotopes equilibrated with milligrams of cold carrier, from the remaining REE’s using a Ce(IV)/LN-resin (Eichrom Technologies) based separation. Optimization of Ce(IV) loading, REE(III) elution volume and subsequent Ce(III) stripping step utilized 166m Ho tracer. Mixed fission product experiments provided a further test of this LN-resin method, with analysis of purified 141/144 Ce, 147 Nd and 91 Y. Overall, while decontamination factors were lower for the LN-resin method, (vs. the combined precipitation/extraction) the simplicity of the technique and the satisfactory fission product analysis results point to the efficacy of this method.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2016

Manipulating the Rate-Limiting Step in Water Oxidation Catalysis by Ruthenium Bipyridine–Dicarboxylate Complexes

In order to gain a deeper mechanistic understanding of water oxidation by [(bda)Ru(L) 2 ] catalysts (bdaH 2 = [2,2'-bipyridine]-6,6'-dicarboxylic acid; L = pyridine-type ligand), a series of modified catalysts with one and two trifluoromethyl groups in the 4 position of the bda 2– ligand was synthesized and studied using stopped-flow kinetics. The additional $-$CF 3 groups increased the oxidation potentials for the catalysts and enhanced the rate of electrocatalytic water oxidation at low pH. Stopped-flow measurements of cerium(IV)-driven water oxidation at pH 1 revealed two distinct kinetic regimes depending on catalyst concentration. At relatively high catalyst concentration (ca. ≥10 –4 M), the rate-determining step (RDS) was a proton-coupled oxidation of the catalyst by cerium(IV) with direct kinetic isotope effects (KIE > 1). At low catalyst concentration (ca. ≤10 –6 M), the RDS was a bimolecular step with k H /k D ≈ 0.8. The results support a catalytic mechanism involving coupling of two catalyst molecules. The rate constants for both RDSs were determined for all six catalysts studied. The presence of $-$CF 3 groups had inverse effects on the two steps, with the oxidation step being fastest for the unsubstituted complexes and the bimolecular step being faster for the most electron-deficient complexes. Finally, though the axial ligands studied here did not significantly affect the oxidation potentials of the catalysts, the nature of the ligand was found to be important not only in the bimolecular step but also in facilitating electron transfer from the metal center to the sacrificial oxidant.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Rapid fusion method for the determination of refractory thorium and uranium isotopes in soil samples

Recently, approximately 80% of participating laboratories failed to accurately determine uranium isotopes in soil samples in the U.S Department of Energy Mixed Analyte Performance Evaluation Program (MAPEP) Session 30, due to incomplete dissolution of refractory particles in the samples. Failing laboratories employed acid dissolution methods, including hydrofluoric acid, to recover uranium from the soil matrix. The failures illustrate the importance of rugged soil dissolution methods for the accurate measurement of analytes in the sample matrix. A new rapid fusion method has been developed by the Savannah River National Laboratory (SRNL) to prepare 1-2 g soil sample aliquots very quickly, with total dissolution of refractory particles. Soil samples are fused with sodium hydroxide at 600 ºC in zirconium crucibles to enable complete dissolution of the sample. Uranium and thorium are separated on stacked TEVA and TRU extraction chromatographic resin cartridges, prior to isotopic measurements by alpha spectrometry on cerium fluoride microprecipitation sources. Plutonium can also be separated and measured using this method. Batches of 12 samples can be prepared for measurement in <5 hours.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

140,142 Cerium Resolved Resonance Region Evaluation [Slides]

The presentation covers an overview of 140,142 Ce Isotopes, including new evaluations of 140,142 Ce that were requested by the Hanford Plutonium Finishing plant to the Nuclear Criticality Safety Program. It also discusses current ENDF/B-VIII.0 evaluation, which has an error in the 1-2 keV range. It was evaluated using multi-level Breit-Wigner and 142Ce has room for extending resolved resonance region current upper limit from 13 keV. The presentation also discusses new transmission and capture measurements of nat Ce and 142 Ce from Klaus Guber. It also states that no known integral experiments prominently feature Cerium.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2019

Rapid concentration and isotopic measurements of ultra-trace 235 U fission products with comparison to an ORIGEN isotope depletion model

We introduce the application of an automated online separation–direct analysis method, RAPID (Rapid Analysis of Post-Irradiation Debris), for the simultaneous measurement of both radioactive and stable fission isotopes from an irradiated highly-enriched uranium target. Developed for the measurement of the concentration and isotopic composition of over 40 elements down to the femtogram level, the RAPID method possesses the sensitivity, stability, and precision needed to achieve accurate, low-level analyses of elements of non-natural origin. The isotopic compositions and concentrations of key fission elements cesium, strontium, yttrium, lanthanum, cerium, praseodymium, neodymium, promethium, and samarium have been measured repeatedly over a six-week period. The validity of these measurements was confirmed using ORIGEN (Oak Ridge Isotope GENeration), an isotope depletion and decay modeling software, to within 1–3%.

07 ISOTOPE AND RADIATION SOURCES↗