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At least 469 records · Page 26

Solid earth as a recycling systems and the lateral growth of Precambrian North America

If plotted on mass vs time diagrams, geologic entities (for example, continental and oceanic crust, sediments, and mineral resources) display an exponential (power law) relationship, with entity per unit time increasing toward the present. This relationship is consistent with the concept of recycling and can be simulated mathematically. The approach is based on the plate tectonic theory and considers area-age or mass-age distributions of crystalline basement and sediments for major global tectonic realms. Each tectonic realm is characterized by a specific lifespan, which is an inverse function of its recycling rate. The estimated average half-area of half-mass ages are given. The corresponding parameters for continental crust are 690 Ma for K/Ar, and approximately 1200 Ma for Rb/St and U-Th/Pb dating pairs. Tectonic diversity preserved in the geologic record is therefore a function of time, with oceanic tectonic realms, because of their rapid recycling, underrepresented in the rocks older than approximately 300 Ma. The Sm/Nd isotopic systematic of sediments suggest that, for a near steady-state post-Archean sedimentary mass, recycling is approximately 90 + or - 5 percent cannibalistic. This yields an estimated upper limit on crust-mantle exchange via sediment subduction of approximately 1.1 + or - 0.5 x 10 g a(sup -1) considerably less than demanded by isotopic constraints. The discrepancy may indicate the existence of additional loci, such as orogenic belts, for significant crust-mantle interaction.

Veizer, Jan↗

G EANT 4 atomic relaxation data for transfermium nuclei (Z = 101–104)

Advanced theoretical methods can accurately calculate various atomic observables and predict electronic structure. Still, systematic computations of the radiative and non-radiative transition probabilities and energies are missing for the actinides and all the transfermium elements. However, these compilations are needed for comprehensive Monte-Carlo simulations (such as GEANT4) of the radioactive decay of transfermium nuclei. These simulations can forma basis for data analysis of experiments, especially with complex detection setups. Investigation of the transfermium nuclei is crucial for understanding the nature of the nuclear force. In this study, simulations based on data from the Jena Atomic Calculator (JAC) and the data from the Evaluated Atomic Data Library (EADL) present in GEANT4 were found compatible for the three elements Ba(Z = 56), U(Z = 92), and Fm(Z = 100), thus, validating the JAC calculations. For Z> 100, we also found sound agreement between simulations that used data generated with JAC and experimental results involving No(Z = 102) and Rf(Z = 104) isotopes. In conclusion, these results demonstrate that JAC can produce reliable atomic data sets for transfermium elements, which will assist in analyzing nuclear-decay-spectroscopy experiments.

GEANT4↗

Assignments of autoionization states of O2-asterisk

Attention is given to the uncertainties that remain concerning the autoionization states of O2 leading to the a 4Pi(u) and A 2Pi(u) states of O2(+), as well as some of the assignments of the autoionization states and the determinations of effective quantum numbers and quantum defects. The former problems of vibrational assignments are unambiguously established in view of a study of isotopic oxygen molecules. A systematic examination of the known Rydberg series is conducted, and new assignments and interpretations for several autoionization states leading to the various states of O2(+) are suggested.

Wu, C. Y. Robert↗

The Abundance and Isotopic Composition of Hg in Extraterrestrial Materials

During the three year grant period we made excellent progress in our study of the abundances and isotopic compositions of Hg and other volatile trace elements in extraterrestrial materials. At the time the grant started, our collaborating PI, Dante Lauretts, was a postdoctoral research associate working with Peter Buseck at Arizona State University. The work on chondritic Hg was done in collaboration with Dante Lauretta and Peter Buseck and this study was published in Lauretta et a1 (2001a). In July, 2001 Dante Lauretta accepted a position as an Assistant Professor in the Lunar and Planetary Laboratory at the University of Arizona. His funding was transferred and this grant has supported much of his research activities during his first two years at the U of A. Several other papers are in preparation and will be published soon. We presented papers on this topic at Goldschmidt Conferences, the Lunar and Planetary Science Conferences, and the Annual Meetings of the Meteoritical Society. The work done under this grant has spurred several new directions of inquiry, which we are still pursuing. Included in this paper are the studies of bulk abundances and isotopic compositions of metreoritic Mercury, and the development of a thermal analysis ICP-MS technique applied to thermally liable elements.

Blum, J. D.↗

Consistent Nuclear Data Evaluations for Criticality Safety [Slides]

This presentation covers consistent nuclear data evaluations for criticality safety. Topics include the evaluation procedure, n+ 139 La evaluation, the work in progress for the n+ 233 U evaluation (emphasis on capture), and a concluding Summary.

07 ISOTOPE AND RADIATION SOURCES↗

3.4-Billion-year-old biogenic pyrites from Barberton, South Africa: sulfur isotope evidence

Laser ablation mass spectroscopy analyses of sulfur isotopic compositions of microscopic-sized grains of pyrite that formed about 3.4 billion years ago in the Barberton Greenstone Belt, South Africa, show that the pyrite formed by bacterial reduction of seawater sulfate. These data imply that by about 3.4 billion years ago sulfate-reducing bacteria had become active, the oceans were rich in sulfate, and the atmosphere contained appreciable amounts (>>10(-13) of the present atmospheric level) of free oxygen.

NASA Discipline Exobiology↗

Performance and optimization of a combustion interface for isotope ratio monitoring gas chromatography/mass spectrometry

Conditions and systems for on-line combustion of effluents from capillary gas chromatographic columns and for removal of water vapor from product streams were tested. Organic carbon in gas chromatographic peaks 15 s wide and containing up to 30 nanomoles of carbon was quantitatively converted to CO2 by tubular combustion reactors, 200 x 0.5 mm, packed with CuO or NiO. No auxiliary source of O2 was required because oxygen was supplied by metal oxides. Spontaneous degradation of CuO limited the life of CuO reactors at T > 850 degrees C. Since NiO does not spontaneously degrade, its use might be favored, but Ni-bound carbon phases form and lead to inaccurate isotopic results at T < 1050 degrees C if gas-phase O2 is not added. For all compounds tested except CH4, equivalent isotopic results are provided by CuO at 850 degrees C, NiO + O2 (gas-phase mole fraction, 10(-3)) at 1050 degrees C and NiO at 1150 degrees C. The combustion interface did not contribute additional analytical uncertainty, thus observed standard deviations of 13C/12C ratios were within a factor of 2 of shot-noise limits. For combustion and isotopic analyses of CH4, in which quantitative combustion required T approximately 950 degrees C, NiO-based systems are preferred, and precision is approximately 2 times lower than that observed for other analytes. Water must be removed from the gas stream transmitted to the mass spectrometer or else protonation of CO2 will lead to inaccuracy in isotopic analyses. Although thresholds for this effect vary between mass spectrometers, differential permeation of H2O through Nafion tubing was effective in both cases tested, but the required length of the Nafion membrane was 4 times greater for the more sensitive mass spectrometer.

NASA Discipline Exobiology↗

Recovery and Recycle of Irradiated Low-Enriched Uranium from the Production of 99 Mo

Technetium-99m ( 99m Tc), the daughter (decay product) of molybdenum-99 ( 99 Mo), is the most commonly used medical radioisotope in the world. 99 Mo is produced primarily from the fissioning of 235 U. A potential future producer, Eden Radioisotopes, is planning to irradiate low-enriched-uranium metal-foil targets for production of 99 Mo. Their plan is to recover, purify, and recycle the irradiated LEU in a new set of targets inside their facility. This study assesses processes to (1) purify and recycle uranium following 99 Mo recovery and (2) convert the uranium to metal for subsequent foil production and target fabrication. A UREX (uranium recovery by extraction) liquid–liquid extraction flowsheet that utilizes centrifugal contactors was developed using the Argonne model for universal solvent extraction (AMUSE) to recover and purify the uranium. The calculated flowsheet predicted high decontamination from Pu and most fission products and >99.99% recovery of uranium. Suggestions for conversion of the UREX U-product (uranyl nitrate in dilute nitric acid) to U metal were provided based on literature studies and earlier laboratory studies performed at Argonne National Laboratory.

07 ISOTOPE AND RADIATION SOURCES↗

Organic chemistry of Murchison meteorite: Carbon isotopic fractionation

The carbon isotopic composition of individual organic compounds of meteoritic origin remains unknown, as most reported carbon isotopic ratios are for bulk carbon or solvent extractable fractions. The researchers managed to determine the carbon isotopic ratios for individual hydrocarbons and monocarboxylic acids isolated from a Murchison sample by a freeze-thaw-ultrasonication technique. The abundances of monocarboxylic acids and saturated hydrocarbons decreased with increasing carbon number and the acids are more abundant than the hydrocarbon with the same carbon number. For both classes of compounds, the C-13 to C-12 ratios decreased with increasing carbon number in a roughly parallel manner, and each carboxylic acid exhibits a higher isotopic number than the hydrocarbon containing the same number of carbon atoms. These trends are consistent with a kinetically controlled synthesis of higher homologues for lower ones.

Yuen, G. U.↗

Lunar and Planetary Science XXXV: Weird Martian Minerals: Complex Mars Surface Processes

The session "Complex Mars Surface" included the following reports:A Reappraisal of Adsorbed Superoxide Ion as the Cause Behind the Reactivity of the Martian Soils; Sub-Surface Deposits of Hydrous Silicates or Hydrated Magnesium Sulfates as Hydrogen Reservoirs near the Martian Equator: Plausible or Not?; Thermal and Evolved Gas Analysis of Smectites: The Search for Water on Mars; Aqueous Alteration Pathways for K, Th, and U on Mars; Temperature Dependence of the Moessbauer Fraction in Mars-Analog Minerals; Acid-Sulfate Vapor Reactions with Basaltic Tephra: An Analog for Martian Surface Processes; Iron Oxide Weathering in Sulfuric Acid: Implications for Mars; P/Fe as an Aquamarker for Mars; Stable Isotope Composition of Carbonates Formed in Low-Temperature Terrestrial Environments as Martian Analogs; Can the Phosphate Sorption and Occlusion Properties Help to Elucidate the Genesis of Specular Hematite on the Mars Surface?; Sulfate Salts, Regolith Interactions, and Water Storage in Equatorial Martian Regolith; Potential Pathways to Maghemite in Mars Soils: The Key Role of Phosphate; and Mineralogy, Abundance, and Hydration State of Sulfates and Chlorides at the Mars Pathfinder Landing Site.

Source record↗

Nonbiological fractionation of iron isotopes

Laboratory experiments demonstrate that iron isotopes can be chemically fractionated in the absence of biology. Isotopic variations comparable to those seen during microbially mediated reduction of ferrihydrite are observed. Fractionation may occur in aqueous solution during equilibration between inorganic iron complexes. These findings provide insight into the mechanisms of iron isotope fractionation and suggest that nonbiological processes may contribute to iron isotope variations observed in sediments.

NASA Discipline Exobiology↗

Pre-Transient Characterization of MLOF-1 Test Pin

This study focuses on the pre-transient characterization of U-10Zr test and sibling fuel pins for the THOR-M-LOF test series. Using neutron radiography, element contact profilometry (ECP), precise gamma scan (PGS), and gas assay, sampling, and recharge (GASR) analysis, it was confirmed that the fuel pins were intact and suitable for testing. Key fuel behaviors quantified include axial elongation, diametral strain, fluff structure geometry, axial isotope distribution, and fission gas release. Any deviations from historically expected behaviors were investigated and attributed to factors other than the irradiation behavior of the fuel pin. These pre-transient measurements establish a baseline for future post-transient analysis, which will be used to inform fuel performance models and safety criteria for sodium-cooled fast reactors (SFRs). The results will enhance understanding of transient fuel behavior and expand limited data on LOF scenarios.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Rapid analysis of 237 Np and Pu isotopes in unseparated sample matrices using ICP-MS/MS

Inductively coupled plasma tandem mass spectrometry (ICP-MS/MS) is an emerging technique for measuring actinide isotopes when assessing pre- and post- detonation nuclear material. In this study, ICP-MS/MS was investigated for direct Np and Pu quantitation in unseparated, dissolved bulk soil matrices. To achieve this, purified nitric oxide (NO) was investigated for the reactivity of Th, Np, U, Pu, Am, and Cm. Purifying NO prior to the collision reaction cell (CRC) results in increased sensitivity and allows for higher gas flows to be utilized for the removal of interferences. Here, the interference from uranium hydrides was mitigated to less than 3.85 x 10 -11 . This method was demonstrated on standard reference materials which were measured for 237 Np and 238,239,240 Pu in dilute sample digestions. The 238 Pu measurement was validated by spiking into a standard reference material and was accurately measured with an excess of 85000 of 238 U.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Removal of High Specific Activity Fission Products from Uranyl Sulfate Waste Solutions

The Savannah River National Laboratory (SRNL) is currently providing support to SHINE Medical Technologies (SHINE) which plans to deploy a low energy, accelerator-based neutron source to fission low enriched U in a uranyl sulfate target solution for 99 Mo production. The 99 Mo is initially separated from the fission products and target solution by an extraction column. Subsequent washing of the column will generate waste solutions containing residual U and fission product activity. A small number of high specific activity fission products (e.g., 90 Sr, 137 Cs, and 144 Ce) in these streams will likely control the classification of the low level waste (LLW). If a sufficient amount of the high specific activity isotopes are separated from the SHINE waste streams and concentrated into a waste form, it would be possible to treat a majority of the wash solutions from the column operations as a lower class of LLW (Class A versus Class B or C or Class B versus Class C). The high specific activity fission product elements could then be dispositioned as a much smaller volume of waste rather than requiring the disposal of the entire waste stream at the higher waste classification. The Savannah River Site (SRS) has experience with using monosodium titanate (MST) and crystalline silicotitanate (CST) to remove Cs and Sr from high salt content waste solutions generated during the reprocessing of nuclear fuels and targets. Both of these materials have worked very well for their intended purposes at the SRS where the fission product elements are removed from highly alkaline waste. On the other hand, SHINE waste streams from the extraction column contain H 2 SO 4 which makes the solution acidic. Additionally, the SRS waste streams do not contain other fission product elements such as transition metals or lanthanides because they precipitate upon neutralization of the SRS waste and are not present in the supernate which is dispositioned as LLW following treatment. As such, there are inherent differences between SHINE and SRS waste treatment strategies. Savannah River National Laboratory was tasked with performing scoping studies to see if MST and CST would remove Sr, Cs, and Ce from an acidic mixed metal simulant solution. Batch contact experiments were performed using MST and two CST type materials. The MST material is a 15 wt % powder in 0.15 M NaOH slurry. The MST showed low adsorption for elements of interest from acidic solution. Furthermore, the powder size makes MST non-ideal for column operations. A CST IE-911 ion exchange material had high Cs adsorption, moderate Sr, and marginal Ce adsorption. Based on adsorption of all species, the ion exchange capacity was found to be 0.032 meq/mL. A bench-top column experiment to measure elemental breakthrough curves was performed using CST IE-911 where chromatographic separations of the mixed simulant were expected to occur. While most elements behaved as expected, the lanthanide series, containing Ce, broke though the column earlier than expected. The second CST material, CST R9120, displayed high adsorption for all elements in the acidic mixed simulant solutions in a batch contact study, and had a calculated loading capacity of 0.091 meq/mL. Future studies to develop a waste treatment flowsheet should focus on CST R9120 to treat SHINE waste solutions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Recent Metallic Fuel Data Recovery in FIPD

The Metallic Fuels Irradiation and Physics Database (FIPD) [1] is an organized collection of metallic fuel test pin data (U-xPu-yZr, = 0 ~ 28; y = 2 ~ 10) and documentation available to industry. FIPD mainly contains three types of data: (1) Fuel pin fabrication data, including fuel slug diameter, fuel slug length, cladding diameter, smear density, etc. (2) Fuel pin operation conditions, including axial distributions for power, temperatures, fluences, burnup, and isotopic densities, etc. and (3) Fuel pin post-irradiation examination (PIE) data, including fission gas release and gas chemistry, profilometry, and neutron radiography, etc. The operating conditions for pins with PIE data available in FIPD span significant ranges across key parameters. The fuel peak burnup extends from less than 5% up to 20 at%. The cladding peak temperature varies from about 490°C to 660°C. Finally, the cladding peak DPA shows a wide range from less than 5 to 120. These broad ranges reflect the diverse testing conditions and operational parameters captured in the available PIE data. More detail about FIPD can be found in ref. [2]. The database development is an ongoing effort covering metallic fuel experiments from the Experimental Breeder Reactor II (EBR-II) and the Fast Flux Test Facility (FFTF). As reported in the ref. [3, 4], most of the PIE data generated during the IFR program [5] has been collected, reviewed, processed, and integrated into FIPD. The most recently added PIE data can be found in ref. [4], which shows the collection of over 95% of the PIE data by the time of this paper. The recent improvements to the database are summarized in this paper.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Continuous-Energy ENDF/B-VIII.0 Cross Section and SCALE 6.2.4 Performance for Nuclear Criticality Safety Applications: 1 H, C, 58,60 Ni, 182,183,184,186 W, 235,238 U, 239 Pu

As part of the nuclear data evaluation and validation cycle, the ENDF/B-VIII.0 cross-section library released in 2018 requires testing to determine areas of improvement and deterioration. Previous work by the authors investigated the performance of 16 O, 56 Fe, and 63,65 Cu cross sections, with this study acting as an extension of the prior work. In addition to the isotopes and nuclear criticality safety benchmarks of interest to the prior work, benchmarks from the International Criticality Safety Benchmark Evaluation Project Handbook were selected for their k eff sensitivity to 1 H, C, 58,60 Ni, 182,183,184,186 W, 235,238U, or 239 Pu cross sections and were modeled in the SCALE code system maintained by Oak Ridge National Laboratory. In total, 253 benchmark configurations were selected for their sensitivities and modeled using SCALE 6.2.4 Criticality Safety Analysis Sequences (CSAS) continuous-energy Monte Carlo k eff calculations. This collection includes and expands upon the 99 benchmarks in the prior work. The AMPX-processed ENDF/B-VIII.0 library was decomposed into individual ENDF/B-VIII.0 datum libraries for each isotope of interest. Doing so allowed for the individual substitution of an ENDF/B-VIII.0 cross section in the place of ENDF/B-VII.1, determining isotope-specific effects of ENDF/B-VIII.0 relative to ENDF/B-VII.1. Full library calculations with entirely ENDF/B-VII.1 data or entirely ENDF/B-VIII.0 data were also executed. As a measure of performance, the average relative deviation was determined as the ratio of the deviation between calculated and experimental keff to the propagated calculational and experimental uncertainty. With calculated full library and isotope-specific ENDF/B-VIII.0 k eff ’s, an optimized combination of data libraries was estimated and confirmed with SCALE calculations. This showed that reverting 239 Pu, 58 Ni, 16 O, and 65 Cu cross sections to ENDF/B-VII.1 resulted in improved performance relative to the full ENDF/B-VIII.0 library. Across all 253 benchmarks, the average relative deviation was 1.29σ for the full ENDF/B-VII.1 library, 1.17σ for the full ENDF/B-VIII.0 library, and 0.97σ for the optimized combination. The reversion of 239 Pu, 58 Ni, 16 O, and 65 Cu cross sections to ENDF/B-VII.1 in the 99 benchmarks of the prior work resulted in further improved experimental agreement compared to the previously reported improvement from 16 O and 65 Cu alone. Therefore, it is suggested that applications with significant sensitivities to 239 Pu, 58 Ni, 16 O, and 65 Cu consider their choice of nuclear data library.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Fission of Relativistic Nuclei with Fragment Excitation and Reorientation

Experimental studies of fission induced in relativistic nuclear collisions show a systematic enhancement of the excitation energy of the primary fragments by a factor of ~2, before their decay by fission and other secondary fragments. Although it is widely accepted that by doubling the energies of the single-particle states may yield a better agreement with fission data, it does not prove fully successful, since it is not able to explain yields for light and intermediate mass fragments. State-of-the-art calculations are successful to describe the overall shape of the mass distribution of fragments, but fail within a factor of 2–10 for a large number of individual yields. In this work, we present a novel approach that provides an account of the additional excitation of primary fragments due to final state interaction with the target. Our method is applied to the 238 U + 208 Pb reaction at 1GeV/nucleon (and is applicable to other energies), an archetype case of fission studies with relativistic heavy ions, where we find that the large probability of energy absorption through final state excitation of giant resonances in the fragments can substantially modify the isotopic distribution of final fragments in a better agreement with data. Finally, we demonstrate that large angular momentum transfers to the projectile and to the primary fragments via the same mechanism imply the need of more elaborate theoretical methods than the presently existing ones.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗