SEARCH · Search NASA
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
Currently, 31 rubidium, 35 strontium, 35 molybdenum, and 38 rhodium isotopes have been observed and the discovery of these isotopes is described here. For each isotope a brief synopsis of the first refereed publication, including the production and identification method, is presented.
Experimentally measured isotopic concentrations of well characterized spent nuclear fuel (SNF) samples have been collected and analyzed by previous researchers. These sets of experimental data have been used extensively to validate the accuracy of depletion code predictions for given sets of burnups, initial enrichments, and varying power histories for different reactor types. The purpose of this report is to present the diversity of data in a concise manner and summarize the current accuracy of depletion modeling. All calculations performed for this report were done using the Oak Ridge Isotope GENeration (ORIGEN) code, an internationally used irradiation and decay code solver within the SCALE comprehensive modeling and simulation code. The diversity of data given in this report includes key actinides, stable fission products, and radioactive fission products. In general, when using the current ENDF/B-VII.0 nuclear data libraries in SCALE, the major actinides are predicted to within 5% of the measured values. Large improvements were seen for several of the curium isotopes when using improved cross section data found in evaluated nuclear data file ENDF/B-VII.0 as compared to ENDF/B-V-based results. The impact of the flux spectrum on the plutonium isotope concentrations as a function of burnup was also shown. The general accuracy noted for the actinide samples for reactor types with burnups greater than 5,000 MWd/MTU was not observed for the low-burnup Hanford B samples. More work is needed in understanding these large discrepancies. The stable neodymium and samarium isotopes were predicted to within a few percent of the measured values. Large improvements were seen in prediction for a few of the samarium isotopes when using the ENDF/B-VII.0 libraries compared to results obtained with ENDF/B-V libraries. Very accurate predictions were obtained for 133 Cs and 153 Eu. However, the predicted values for the stable ruthenium and rhodium isotopes varied as much as 10% of the measured values, and 109 Ag was consistently over-predicted by as much as 170%. In general, there is a larger uncertainty for modeling radioactive fission products when compared to either the actinides or the stable fission products in SNF. The relative C/E ratios ranged from a few percent for 137 Cs up to 60% and 100% for 106 Ru and 125 Sb, respectively. Limited or no radioactive fission products data exist in the current data sets for reactor types other than PWRs and BWRs. More work is needed in obtaining a greater diversity of radioactive fission product data. While performing this survey, issues leading to inconsistencies in nuclear fission yield data were discovered that specifically impacted the fission product noble gases. Emphasis was given to this legacy data, and corrective actions were taken as described in this report. After the fission yield data were corrected, the stable xenon and krypton fission products were predicted to within 5% of their measurements. However, preliminary results not explicitly given in this report indicate that the relative C/E ratio for the radioactive isotope 85 Kr varied as much as 10%. Due to the complex migration and the difficulty in measuring noble gases in the fuel, a more thorough investigation is needed to understand how accurately depletion codes can calculate these gas concentrations.
Nuclear structure data pertaining to all nuclei with mass number A=93 (Se, Br, Kr, Rb, Sr, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag) have been compiled and evaluated and incorporated into the ENSDF data file. This publication for A=93 supersedes the previous publication by C.M. Baglin, Nuclear Data Sheets80, 1 (1997) (literature cutoff date November 1996) and subsequent revisions by C.M. Baglin of the ENSDF files for 93Br and {sup 93}Kr (literature cutoff 26 February 2001) and for {sup 93}Rh (literature cutoff 27 February 2001); it includes all data available prior to 15 December 2010. Significant changes since prior evaluations include the following: 2010Hw03 identified several high-spin states in {sup 93}Kr in {sup 252}Cf SF decay; in addition to the many low-spin levels already known in {sup 93}Rb from {beta}{sup -} decay, several higher-spin states have now been identified in a {sup 252}Cf SF decay study (2009Hw03); this SF decay has also been used to identify additional states in {sup 93}Sr (2003Hw01) and the {sup 238}U({sup 82}Se,X{gamma}) reaction (2007Bu35) has provided new information on {sup 93}Y. (HI,xn{gamma}) reaction studies have expanded our knowledge of the structure of {sup 93}Zr (2002Fo03, 2005Pa48), {sup 93}Nb (2007Wa45), {sup 93}Mo (2005Fu01), {sup 93}Tc (2003Ha22) and {sup 93}Pd (2004So04,2004Ru02). Considerable information on {sup 93}Nb was provided by a (p,2n{gamma}) study (2010Or01, 2006Or09, 2007Or01). The level schemes of {sup 93}Ru, {sup 93}Rh and {sup 93}Pd have undergone the most extensive revision thanks to studies of {sup 93}Rh {epsilon} decay (2004De40), {sup 94}Ag {epsilon}p decay (2004Mu30) and {sup 94}Ag p decay (2005Mu15, 2005Mu30), respectively. The half-life of the Zr member of this chain is of particular interest because of {sup 93}Zr's large contribution to long-term activity of nuclear reactor waste and also due to its potential as a supernova chronometer. During 2010, two new well-documented measurements of T{sub 1/2}({sup 93}Zr) were published (2010Ya01 and 2010Ca01); one agrees well with an earlier, undocumented measurement but, unfortunately, the other is many standard deviations lower for reasons which are not immediately apparent.
This study demonstrates a new method of radioisotope labeling of ultra-high molecular weight polyethylene inserts in prosthetic joints for wear studies. The radioisotopes {sup 97}Ru, {sup 100}Pd, {sup 100}Rh, and {sup 101m}Rh are produced in fusion evaporation reactions induced by {sup 12}C ions in a {sup 92}Zr target foil. The fusion products recoil-implant into ultra-high molecular weight polyethylene plugs, machined to fit into the surface of the inserts. During laboratory simulations of the joint motion, a wear rate of the labeled polyethylene may be measured and the pathways of wear debris particles can be traced by detecting characteristic gamma-rays. The concentration profiles of the radioisotopes extend effectively uniformly from the polyethylene surface to a depth of about 4 {mu}m. The multiplicity of labeling and the use of several gamma-ray lines aids with avoiding systematic measurement uncertainties. Two polyethylene plugs were labeled and one was fitted into the surface of the tibial insert of a knee prosthesis, which had been worn in. Actuation over close to 100,000 cycles with a 900 N axial load and a 24 deg. flexion angle removed (14{+-}1)% of the gamma-ray activity from the plug. Most of this activity dispersed into the serum lubricant identifying this as the important debris pathway. Less than 1% activity was transferred to the femoral component of the prosthesis and the measured activity on the tibial tray was insignificant. Assuming uniform wear across the superior surface of the insert, a wear rate of (12{+-}3) mm{sup 3}/Megacycle was determined. This is consistent with wear rate measurements under similar conditions using other techniques.
Following the reports of two pairs of chiral doublet bands observed in {sup 105}Rh, the adiabatic and configuration-fixed constrained triaxial relativistic mean-field calculations are performed to investigate their triaxial deformations with the corresponding configuration and the possible multiple chiral doublet (M{chi}D) phenomenon. The existence of the M{chi}D phenomenon in {sup 105}Rh is highly expected.
High-spin excited states in the neutron-rich nucleus {sup 115}Rh have been identified for the first time by studying prompt {gamma} rays from the spontaneous fission of {sup 252}Cf with the Gammasphere detector array. A new yrast band and a sideband are built in {sup 115}Rh. This level scheme is proposed to be built on the 7/2{sup +} ground state. The existence of a large signature splitting and an yrare band in {sup 115}Rh shows typical features of a triaxially deformed nucleus. The rigid triaxial rotor plus particle model is used to interpret the level structure of {sup 115}Rh. The level energies, the {gamma} branching ratios, the large signature splitting in the yrast band, and the inverted signature splitting in the yrare band in {sup 115}Rh are reproduced very well. Strong K mixing occurs in {sup 115}Rh at high spin.
High-spin excited states in the very neutron-rich nucleus {sup 114}Rh have been studied by examining the prompt {gamma} rays emitted in the spontaneous fission of {sup 252}Cf with the Gammasphere detector array. A high-spin level scheme of {sup 114}Rh has been established for the first time with 13 new levels. The level scheme is proposed to be built on a 7{sup -} state. The existence of a relatively large signature splitting and an yrare band show features which may indicate triaxial deformation. The phenomenon of signature inversion has been observed in {sup 114}Rh at I=12 ({h_bar}/2{pi}). The observed signature inversion of {sup 114}Rh is interpreted successfully in terms of the triaxial projected shell model. Theoretical calculations suggest that the negative-parity, yrast band of {sup 114}Rh has the two-quasi-particle configuration of {pi}g{sub 9/2} x {nu}h{sub 11/2}, consistent with the systematics of odd-odd Rh isotopes. The signature inversion at spin 12 ({h_bar}/2{pi}) may be attributed to the change of rotational mode, from quasi-particle aligned rotation at low spins to collective rotation at high spins.
By adopting the fully quantal triaxial particle-rotor model, the candidate chiral doublet bands in odd-A nuclei {sup 103}Rh and {sup 105}Rh with {pi}g{sub 9/2}{sup -1} x {nu}h{sub 11/2}{sup 2} configuration are studied. For the doublet bands in both nuclei, agreement is excellent for the observed energies over the entire spin range and B(M1)/B(E2) at higher spin range. The evolution of the chiral geometry with angular momentum is discussed in detail by using the angular momentum components and their probability distributions. Chirality is found to change from chiral vibration to nearly static chirality at spin I=37/2 and back to another type of chiral vibration at higher spin. The influence of the triaxial deformation {gamma} is also studied.
Analysis of high statistics triple coincidence fission γ data from {sup 252}Cf at Gammasphere including angular correlations yielded well-expanded high-spin level schemes with more complete and reliable spin/parity assignments for {sup 82}Ge, {sup 118,120,122}Cd and {sup 114,115}Rh. Both the quasi-particle/hole couplings and quasi-rotational degrees of freedom are implied to play roles in these Cd isotopes. Evidence for triaxial shapes and octupole components in the Cd isotopes is presented. These Cd isotopes may have triaxial deformations. High-spin level schemes of {sup 114,115}Rh have been established for the first time. The existence of a relatively large signature splitting and an yrare band shows typical features of a triaxially deformed nucleus. Possible excited deformed rotational bands are observed, for the first time, in {sup 82}Ge. From the multipole mixing ratio measurement, the ground state configurations of {sup 109,111}Ru, as well as excited states in {sup 103,107}Mo and {sup 111}Ru were determined.
Heavy even-even nuclei exhibit low-energy collective excitations that are separated in scale from the microscopic (fermion) degrees of freedom. This separation of scale allows us to approach nuclear vibrations within an effective field theory (EFT). In odd-mass nuclei collective and single-particle properties compete at low energies, and this makes their description more challenging. In this article we describe spherical odd-mass nuclei with ground-state spin I = 1/2 by means of an EFT that couples a fermion to the collective degrees of freedom of an even-even core. The EFT relates observables such as energy levels, electric quadrupole transition strengths, and magnetic dipole moments of the odd-mass nucleus to those of its even-even neighbor and allows us to quantify theoretical uncertainties. For isotopes of rhodium and silver the theoretical description is consistent with data within experimental and theoretical uncertainties. Here, several testable predictions are made.
The origin of ubiquitous nucleosynthetic isotope anomalies in meteorites may represent spatial and/or temporal heterogeneity in the sources that supplied material to the nascent solar nebula, or enhancement by chemical processing. For elements beyond the Fe peak, deficits in s-process isotopes have been reported in some (e.g., Mo, Ru, W) but not all refractory elements studied (e.g., Os) that, among the iron meteorites, are most pronounced in IVB iron meteorites. Palladium is a non-refractory element in the same mass region as Mo and Ru. In this study, we report the first precise Pd isotopic abundances from IVB irons to test the mechanisms proposed for the origin of isotope anomalies. First, this study determined the existence of a cosmogenic neutron dosimeter from the reaction {sup 103}Rh(n, β{sup −}){sup 104}Pd in the form of excess {sup 104}Pd, correlated with excess {sup 192}Pt, in IVB irons. Second, all IVB irons show a deficit of the s-process only isotope {sup 104}Pd (ε {sup 104}Pd = −0.48 ± 0.24), an excess of the r-only isotope {sup 110}Pd (ε{sup 110}Pd = +0.46 ± 0.12), and no resolvable anomaly in the p-process {sup 102}Pd (ε {sup 102}Pd = +1 ± 1). The magnitude of the Pd isotope anomaly is about half that predicted from a uniform depletion of the s-process yields from the correlated isotope anomalies of refractory Mo and Ru. The discrepancy is best understood as the result of nebular processing of the less refractory Pd, implying that all the observed nucleosynthetic anomalies in meteorites are likely to be isotopic relicts. The Mo–Ru–Pd isotope systematics do not support enhanced rates of the {sup 22}Ne(α,n){sup 25}Mg neutron source for the solar system s-process.
At the 8{sup th} Temperature Symposium the results have been presented for the Interpolating Constant Volume Gas thermometer at INRIM (then IMGC), featuring a cryogenic pressure transducer, with an expanded uncertainty of less then 1.5 mK. However, for its fixed points this scale still relied on a NPL calibration as carried by rhodium-iron thermometer 232324. After the clarification, in 2005, by the Consultative Committee on Thermometry (CCT) of the definition of the equilibrium hydrogen (e-H2) triple point this scale was due to be adjusted for the isotopic content in the e-H2 fixed point cell. Only when this thermometer was re-calibrated in 2010 at INRIM at the three fixed points of the ICVGT was this adjustment performed, being the isotopic composition of the hydrogen cell known. With the start of the Neon Project in 2005, it became clear that a second adjustment would soon be needed, once the CCT will have decided on the way to deal with the isotopic composition of neon. The paper presents the experimental data of 2010, discusses the stability of the thermometer, and the size of the correction at the hydrogen point and of the likely correction (and its uncertainty) to be applied to the neon point, the isotopic composition of this cell being known as well.
The interactions of ground water with minerals and contaminants are of broad interest for geochemists but are not well understood. Experiments on the molecular scale can determine reaction parameters (i.e. rates of ligand exchange, activation entropy, activation entropy, and activation volume) that can be used in computations to gain insight into reactions that occur in natural groundwaters. Experiments to determine the rate of isotopic ligand exchange for three environmentally relevant metals, rhodium (Rh), iron (Fe), and neptunium (Np), are described. Many environmental transformations of metals (e.g. reduction) in soil occur at trivalent centers, Fe(III) in particular. Contaminant ions absorb to mineral surfaces via ligand exchange, and the reversal of this reaction can be dangerous, releasing contaminants into the environment. Ferric iron is difficult to study spectroscopically because most of its complexes are paramagnetic and are generally reactive toward ligand exchange; therefore, Rh(III), which is diamagnetic and less reactive, was used to study substitution reactions that are analogous to those that occur on mineral oxide surfaces. Studies on both Np(V) and Np(VI) are important in their own right, as 237 Np is a radioactive transuranic element with a half-life of 2 million years.
General Atomics and the University of Missouri Research Reactor (MURR) completed research and development of selective gaseous extraction of fission products from irradiated fuel, which included training and education of MURR students. The process used porous fuel and after irradiation flowed product gases through the fuel to selectively removed desired fission products with the primary goal of demonstrating the removal of rhodium 105. High removal rates for the ruthenium/rhodium (Ru/Rh), tellurium/iodine (Te/I) and molybdenum/technetium (Mo/Tc) series were demonstrated. The success of this research provides for the reuse of the target for further production, significantly reducing the production of actinide wastes relative to processes that dissolve the target. This effort was conducted under DOE funding (DE-SC0007772). General Atomics objective of the project was to conduct R&D on alternative methods to produce a number of radioactive isotopes currently needed for medical and industry applications to include rhodium-105 and other useful isotopes. Selective gaseous extraction was shown to be effective at removing radioisotopes of the ruthenium/rhodium, tellurium/iodine and molybdenum/technetium decay chains while having trace to no quantities of other fission products or actinides. This adds a new, credible method to the area of certain commercial isotope production beyond current techniques, while providing significant potential reduction of process wastes. Waste reduction, along with reduced processing time/cost provides for superior economic feasibility which may allow domestic production under full cost recovery practices. This provides the potential for improved access to domestically produced isotopes for medical diagnostics and treatment at reduced cost, providing for the public good.
The kinetics of the reaction of benzyl radicals with [L{sup 1}(H{sub 2}O)RhH{l_brace}D{r_brace}]{sup 2+} (L{sup 1}=1,4,8,11-tetraazacyclotetradecane) were studied directly by laser-flash photolysis. The rate constants for the two isotopologues, k=(9.3 {+-} 0.6) x 10{sup 7} M{sup -1} s{sup -1} (H) and (6.2 {+-} 0.3) x 10{sup 7} M{sup -1} s{sup -1} (D), lead to a kinetic isotope effect k{sub H}/k{sub D}=1.5 {+-} 0.1. The same value was obtained from the relative yields of PhCH{sub 3} and PhCH{sub 2}D in a reaction of benzyl radicals with a mixture of rhodium hydride and deuteride. Similarly, the reaction of methyl radicals with {l_brace}[L{sup 1}(H{sub 2}O)RhH]{sup 2+} + [L{sup 1}(H{sub 2}O)RhD]{sup 2+}{r_brace} produced a mixture of CH{sub 4} and CH{sub 3}D that yielded k{sub H}/k{sub D}=1.42 {+-} 0.07. The observed small normal isotope effects in both reactions are consistent with reduced sensitivity to isotopic substitution in very fast hydrogen-atom abstraction reactions. These data disprove a literature report claiming much slower kinetics and an inverse kinetic isotope effect for the reaction of methyl radicals with hydrides of L{sup 1}Rh.
We show for the first time that atomically dispersed Rh cations on ceria, prepared via high-temperature atom trapping synthesis, are the active species for (CO+NO) reaction. This provides a direct link with the organometallic homogeneous Rh(I) complexes capable of catalyzing dry (CO+NO) reaction but without the stability concern. In particular, thermally stable Rh cations in 0.1wt% Rh1/CeO2 achieve full NO conversion with a TOF of ~ 330 hr-1 per Rh atom at 120 °C. Under dry conditions, the main product above 100 °C is N2 with N2O being the minor product. The presence of water promotes low-temperature activity of 0.1wt% Rh1/CeO2 starting at 50 °C with full NO conversion at ~120 °C. In the case with the wet stream, however, ammonia and nitrogen are the main products with only minor N2O amounts. NH3 formation at such low temperatures is attractive because of the potential to use this as a passive SCR system. Because of the uniformity of Rh ions on the support, we are able to observe the intermediates of (CO+NO) reaction via infrared measurements on Rh cations on zeolite and ceria. Furthermore, we show that ammonia formation correlates with the WGS activity of the material and thus, rhodium hydride Rh-H species are involved in this reaction: we detect Rh(CO)Hx species on ceria using isotopic IR measurements. These findings provide new mechanistic understanding for the catalytically active species in TWC catalysis and open up a new avenue for the synthesis of novel emissions control catalysts with 100% atom economy of ultra-expensive precious metals such as Rh.
Reprocessing is essential to closing nuclear fuel cycle. Natural uranium contains only 0.7 percent 235U, the fissile (see glossary for technical terms) isotope that produces most of the fission energy in a nuclear power plant. Prior to being used in commercial nuclear fuel, uranium is typically enriched to 3–5% in 235U. If the enrichment process discards depleted uranium at 0.2 percent 235U, it takes more than seven tonnes of uranium feed to produce one tonne of 4%-enriched uranium. Nuclear fuel discharged at the end of its economic lifetime contains less one percent 235U, but still more than the natural ore. Less than one percent of the uranium that enters the fuel cycle is actually used in a single pass through the reactor. The other naturally occurring isotope, 238U, directly contributes in a minor way to power generation. However, its main role is to transmute into plutoniumby neutron capture and subsequent radioactive decay of unstable uraniumand neptuniumisotopes. 239Pu and 241Pu are fissile isotopes that produce more than 40% of the fission energy in commercially deployed reactors. It is recovery of the plutonium (and to a lesser extent the uranium) for use in recycled nuclear fuel that has been the primary focus of commercial reprocessing. Uraniumtargets irradiated in special purpose reactors are also reprocessed to obtain the fission product 99Mo, the parent isotope of technetium, which is widely used inmedical procedures. Among the fission products, recovery of such expensive metals as platinum and rhodium is technically achievable, but not economically viable in current market and regulatory conditions. During the past 60 years, many different techniques for reprocessing used nuclear fuel have been proposed and tested in the laboratory. However, commercial reprocessing has been implemented along a single line of aqueous solvent extraction technology called plutonium uranium reduction extraction process (PUREX). Similarly, hundreds of types of reactor fuels have been irradiated for different purposes, but the vast majority of commercial fuel is uranium oxide clad in zirconium alloy tubing. As a result, commercial reprocessing plants have relatively narrow technical requirements for used nuclear that is accepted for processing.
During the purification of radioisotopes, decay periods or time dependent purification steps may be required to achieve a certain level of radiopurity in the final product. Actinum-225 (Ac-225), Silver-111 (Ag-111), Astatine-211 (At-211), Ruthenium-105 (Ru-105), and Rhodium-105 (Rh-105) are produced in a high energy proton irradiated thorium target. Experimentally measured cross sections, along with MCNP6-generated cross sections, were used to determine the quantities of Ac-225, Ag-111, At-211, Ru-105, Rh-105, and other co-produced radioactive impurities produced in a proton irradiated thorium target at Brookhaven Linac Isotope Producer (BLIP). Ac-225 and Ag-111 can be produced with high radiopurity by the proton irradiation of a thorium target at BLIP.