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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.

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At least 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Complexity of Uranyl Peroxide Cluster Speciation from Alkali-Directed Oxidative Dissolution of Uranium Dioxide

Solid UO 2 dissolution and uranium speciation in aqueous solutions that promote formation of uranyl peroxide macroanions was examined, focusing on the role of alkali metals. UO 2 powders were dissolved in solutions containing XOH (X = Li, Na, or K) and 30% H 2 O2. Inductively coupled plasma optical emission spectroscopy (ICP-OES) measurements of solutions revealed linear trends of uranium versus alkali concentration in solutions resulting from oxidative dissolution of UO 2 , with X:U molar ratios of 1.0, showing that alkali availability determines the U concentrations in solution. The maximum U concentration in solution was 4.36 x 10 5 parts per million (ppm), which is comparable to concentrations attained by dissolving UO 2 in boiling nitric acid, and was achieved by lithium hydroxide-promoted dissolution. Lastly, Raman spectroscopy and electrospray ionization mass spectrometry (ESI-MS) of solutions indicate that dissolution is accompanied by formation of various uranyl peroxide cluster species, the identity of which is alkali concentration-dependent, revealing remarkably complex speciation at high concentrations of base.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Complex Topologies from Simple Building Blocks: Uranium(IV) Thiophosphates

Six new uranium thiophosphates Cs 5 Na 6 [U(PS 4 ) 4 ](PS 4 ) (1), Rb 5 Na 3 [U(PS 4 ) 4 ] (2), CsNa[U(PS 4 ) 2 ] (3), Cs 1.67 Na 0.52 I 0.19 [U(PS 4 ) 2 ] (4), Cs 1.033 Na 1.343 I 0.376 [U(PS 4 ) 2 ] (5), and Rb 1.35 Na 0.93 I 0.28 [U(PS 4 ) 2 ] (6) were obtained from halide flux reactions and characterized using single crystal X-ray diffraction. The structures of these compounds consist of a pseudo-tetrahedral uranium unit that in combination with a set of PS 4 group coordination modes can result in an isolated [U(PS 4 ) 4 ] 8– unit, a [U(PS 4 ) 2 ] 2– chain, or a [U(PS 4 ) 2 ] 2– slab. Optical and magnetic properties of 3 and 4 were collected. Both compounds exhibit paramagnetic behavior, and CsNa[U(PS 4 ) 2 ] (3) exhibits a magnetic transition at 200–225 K between two paramagnetic states that both have similar effective magnetic moments of 4.13 and 4.19 µ B /F.U., and strong antiferromagnetic interactions with θ = -183 and -172 K, for the high- and low-temperature states, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Targeted Synthesis of Uranium(IV) Thiosilicates

Two new uranium(IV) thiosilicates, Cs 2 Na 4 [U 2 (SiS 4 ) 2 (Si 2 S 8 )] and Cs 2.12 Na 3.88 [U 2 (SiS 4 ) 2 (Si 2 S 7 )], were obtained by flux crystal growth using SiS 2 as a silicon source. The former compound contains a novel Si 2 S 8 6– unit that features a terminal persulfide group. The magnetic susceptibility measurements performed on this compound revealed paramagnetic behavior with a moment of 3.49 μ B per uranium atom as obtained from a Curie–Weiss law fit and showed no magnetic transition down to 2 K. Finally, the structures are based on closely related isomeric planar and 3D topologies that can be transformed into one another by a rotation of the structural units.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Uranium Hexafluoride Hydrolysis Reaction Dynamics from Cryogenic Layering, FTIR Spectroscopy, and Isotopic Substitution

The first direct evidence that the hydrolysis reaction of uranium hexafluoride (UF 6 ) follows multiple competing pathways which are driven by the ratio of water to UF 6 , temperature, and isotopic composition is presented. Using temperature dependent infrared spectroscopy, it is shown the hydrolysis can be prevented at temperatures below 150 K, and that water-rich environments promote the formation of uranium oxyfluoride intermediates. Spectral shifts reveal isomeric transitions and the growth of polymeric species, with reaction reversibility observed at high water concentrations. Additionally, controlled heating rates affect the emergence of intermediates. The final particulate product consistently forms as uranyl fluoride hydrate, though its morphology and spectral signature vary with reaction conditions and annealing. These findings help clarify long-standing uncertainties surrounding UF 6 hydrolysis.

Chemical reactions↗
DOE OSTI2014

Photochemical route to actinide-transition metal bonds: synthesis, characterization and reactivity of a series of thorium and uranium heterobimetallic complexes

A series of actinide-transition metal heterobimetallics has been prepared, featuring thorium, uranium and cobalt. Complexes incorporating the binucleating ligand N[-(NHCH2PiPr2)C6H4]3 and Th(IV) (4) or U(IV) (5) with a carbonyl bridged [Co(CO)4]- unit were synthesized from the corresponding actinide chlorides (Th: 2; U: 3) and Na[Co(CO)4]. Irradiation of the isocarbonyls with ultraviolet light resulted in the formation of new species containing actinide-metal bonds in good yields (Th: 6; U: 7); this photolysis method provides a new approach to a relatively rare class of complexes. Characterization by single-crystal X-ray diffraction revealed that elimination of the bridging carbonyl is accompanied by coordination of a phosphine arm from the N4P3 ligand to the cobalt center. Additionally, actinide-cobalt bonds of 3.0771(5) and 3.0319(7) for the thorium and uranium complexes, respectively, were observed. The solution state behavior of the thorium complexes was evaluated using 1H, 1H-1H COSY, 31P and variable-temperature NMR spectroscopy. IR, UV-Vis/NIR, and variable-temperature magnetic susceptibility measurements are also reported.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Enrichment of specific protozoan populations during in situ bioremediation of uranium-contaminated groundwater

The importance of bacteria in the anaerobic bioremediation of groundwater polluted with organic and/or metal contaminants is well-recognized and in some instances so well understood that modeling of the in situ metabolic activity of the relevant subsurface microorganisms in response to changes in subsurface geochemistry is feasible. However, a potentially significant factor influencing bacterial growth and activity in the subsurface that has not been adequately addressed is protozoan predation of the microorganisms responsible for bioremediation. In field experiments at a uranium-contaminated aquifer located in Rifle, CO, acetate amendments initially promoted the growth of metal-reducing Geobacter species followed by the growth of sulfate-reducers, as previously observed. Analysis of 18S rRNA gene sequences revealed a broad diversity of sequences closely related to known bacteriovorous protozoa in the groundwater prior to the addition of acetate. The bloom of Geobacter species was accompanied by a specific enrichment of sequences most closely related to the amoeboid flagellate, Breviata anathema, which at their peak accounted for over 80% of the sequences recovered. The abundance of Geobacter species declined following the rapid emergence of B. anathema. The subsequent growth of sulfate-reducing Peptococcaceae was accompanied by another specific enrichment of protozoa, but with sequences most similar to diplomonadid flagellates from the family Hexamitidae, which accounted for up to 100% of the sequences recovered during this phase of the bioremediation. These results suggest a prey-predator response with specific protozoa responding to increased availability of preferred prey bacteria. Thus, quantifying the influence of protozoan predation on the growth, activity, and composition of the subsurface bacterial community is essential for predictive modeling of in situ uranium bioremediation strategies.

breviata↗
DOE OSTI2017

Uranium extraction: Fuel from seawater

Over four billion tonnes of uranium are currently in the oceans that could be harvested for nuclear fuel, but current capture methods have limited performance and reusability. Now, an electrochemical method using modified carbon electrodes is shown to be promising for the extraction of uranium from seawater.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2014

Carbonate-H2O2 Leaching for Sequestering Uranium from Seawater

Uranium adsorbed on amidoxime-based polyethylene fiber in simulated seawater can be quantitatively eluted at room temperature using 1M Na2CO3 containing 0.1 M H2O2. This efficient elution process is probably due to formation of an extremely stable uranyl-peroxo-carbonato complex in the carbonate solution. After washing with water, the sorbent can be reused with little loss of uranium loading capacity. Possible existence of this stable uranyl species in ocean water is also discussed.

carbonate-peroxide leaching sequestering uranium s↗
DOE OSTI2016

Critical Need for Plutonium and Uranium Isotopic Standards with Lower Uncertainties

Certified reference materials (CRMs) traceable to national and international safeguards database are a critical prerequisite for ensuring that nuclear measurement systems are free of systematic biases. CRMs are used to validate measurement processes associated with nuclear analytical laboratories. Diverse areas related to nuclear safeguards are impacted by the quality of the CRM standards available to analytical laboratories. These include: nuclear forensics, radio-chronometry, national and international safeguards, stockpile stewardship, nuclear weapons infrastructure and nonproliferation, fuel fabrication, waste processing, radiation protection, and environmental monitoring. For the past three decades the nuclear community is confronted with the strange situation that improvements in measurement data quality resulting from the improved accuracy and precision achievable with modern multi-collector mass spectrometers could not be fully exploited due to large uncertainties associated with CRMs available from New Brunswick Laboratory (NBL) that are used for instrument calibration and measurement control. Similar conditions prevail for both plutonium and uranium isotopic standards and for impurity element standards in uranium matrices. Herein, the current status of U and Pu isotopic standards available from NBL is reviewed. Critical areas requiring improvement in the quality of the nuclear standards to enable the U. S. and international safeguards community to utilize the full potential of modern multi-collector mass spectrometer instruments are highlighted.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2016

Isotope ratio characteristics and sensitivity for uranium determinations using a liquid sampling-atmospheric pressure glow discharge ion source coupled to an Orbitrap mass analyzer

Abstract The continued development of the liquid sampling-atmospheric pressure glow discharge (LS-APGD) microplasma as an ion source for diverse, elemental/isotopic analysis applications continues. To this end, characterization of the capabilities in performing precise and accurate isotope ratio (IR) determinations is essential. Based on past experience with the Thermo Exactive Orbitrap mass analyzer, the LS-APGD was interfaced with this instrument for these tests. While the Orbitrap platform has demonstrated excellent mass resolution and accuracy in “organic” mass spectrometry (MS) applications, work using an Orbitrap for IR analysis is very sparse. These efforts build off previous work in this coupling, where the importance of a few of the LS-APGD discharge parameters and Orbitrap data acquisition methods on IR precision and accuracy were probed. Presented here are the results of a study that evaluated the analytical precision for natural uranium sample (assumed 235U/238U = 0.0072) determinations. The instrumental parameters evaluated include the number of microscans and scans making up a data acquisition set, uranium concentration/signal level, sample make-up, and Fourier transform digitization window. Ultimately, a precision of 0.41% relative standard deviation (RSD) can be achieved for a single determination, with a reproducibility of 1.63 %RSD over 10 separate analytical measurements. A preliminary study of matrix effects on IR measurements of U is presented, highlighting the importance of pre-mass selection before injection into the Orbitrap. The analytical system sensitivity is suggested with the ability to produce a calibration function having an R2 value of >0.99 over a range of 4 orders of magnitude of concentration (~1 – 1000 ng mL-1). These efforts demonstrate the very promising pairing of the LS-APGD ionization source and the Orbitrap, pointing as well to definitive paths forward to better utilize both components in high quality isotope ratio mass spectrometry (IRMS).

Environmental Molecular Sciences Laboratory↗
DOE OSTI2015

A two-dimensional, finite-difference model of the oxidation of a uranium carbide fuel pellet

The oxidation of spent uranium carbide fuel, a candidate fuel for Generation IV nuclear reactors, is an important process in its potential reprocessing cycle. However, the oxidation of uranium carbide in air is highly exothermic. A model has therefore been developed to predict the temperature rise, as well as other useful information such as reaction completion times, under different reaction conditions in order to help in deriving safe oxidation conditions. Finite difference-methods are used to model the heat and mass transfer processes occurring during the reaction in two dimensions and are coupled to kinetics found in the literature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Characterization of PAH matrix with monazite stream containing uranium, gadolinium and iron

Uranium (U) gadolinium (Gd) and iron (Fe) containing alkaline waste simulated effluent (relevant to alkaline effluent of monazite ore) has been treated with a novel amphoteric resin viz, Polyamidehydroxamate (PAH) containing amide and hydroxamic acid groups. The resin has been synthesized in an eco-friendly manner by polymerization nad conversion to functional groups characterized by FT-IR spectra and architectural overview by SEM. Coloration of the loaded matrix and de-coloration after extraction of uranium is the special characteristic of the matrix. Effluent streams have been analyzed by ICP-AES, U loaded PAH has been characterized by FT-IR, EXAFS, Gd and Fe by X-ray energy values of EDXRF at 6.053 KeVand 6.405 KeV respectively. The remarkable change has been observed in Mössbauer spectrum of Fe-loaded PAH samples.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Systematic Measurements and Analyses for Lead Void Reactivity Worth in a Plutonium Core and Two Uranium Cores with Different Enrichments

To validate lead (Pb) nuclear cross sections, a series of integral experiments to measure lead void reactivity worth was conducted systematically in three fast neutron spectra with different fuel compositions on the Comet critical assembly of the National Criticality Experiments Research Center. Previous experiments in high-enriched uranium (HEU)/Pb and low-enriched uranium (LEU)/Pb systems had been performed in 2016 and 2017, respectively. A follow-on experiment in a plutonium (Pu)/Pb system has been completed. The Pu/Pb system was constructed using lead plates and weapons-grade Pu plates that had been used in the Zero Power Physics Reactor (ZPPR) of Argonne National Laboratory until the 1990s. Furthermore, the HEU/Pb system was reexamined on the Comet critical assembly with a newly installed device that can measure the compression of the stack, improving reproducibility. Using the lead void reactivity worth measured in these three cores with different fuel compositions, the latest nuclear data libraries, JENDL-4.0 and ENDF/B-VIII.0, were tested with the Monte Carlo calculation code MCNP® version 6.1. As a result, the calculations by ENDF/B-VIII.0 were confirmed to agree with lead void reactivity worth measured in all the cores. It was furthermore found that the calculations by JENDL-4.0 overestimate by more than 20% for the Pu/Pb core while being in good agreement for the HEU/Pb and LEU/Pb cores.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Generation of the Thermal Scattering Law of Uranium Dioxide with Ab Initio Lattice Dynamics to Capture Crystal Binding Effects on Neutron Interactions

Scattering of thermal neutrons and Doppler broadening of epithermal neutron resonances in uranium and its compounds may be sensitive to crystal binding. The thermal scattering law (TSL) for uranium dioxide, which captures crystal binding effects, has been reevaluated for ENDF/B-VIII.0. Phonon spectra were generated using ab initio lattice dynamics for the paramagnetic phase and validated against experiment. Improved agreement with the Debye-Waller coefficient as a function of temperature is found relative to the spectrum used for the ENDF/B-VII.1 evaluation. The TSL was generated using the phonon expansion method within the NJOY nuclear data processing package and was found to be in reasonable agreement with inelastic neutron scattering measurements. The present evaluation predicts a reduction in the inelastic scattering cross section relative to ENDF/B-VII.1 and a total scattering cross section consistent with neutron transmission experiments

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Measurement of Photoneutrons from Depleted Uranium and Comparison Study Using MCNPX-PoliMi

High-energy photon interrogation is a nondestructive technique that is used to detect special nuclear materials and characterize nuclear waste. The development of such systems is complex and requires Monte Carlo simulations to optimize system performance. Monte Carlo simulations rely on various scattering, absorption, and photonuclear cross-section data. While the scattering and absorption cross-section data have been extensively studied and validated with experiments, the results obtained from photonuclear simulations are often found to underpredict measured results, indicating uncertainties in the photonuclear cross sections themselves. Thus, there is a need for new measured results that can be used to quantify underpredictions in simulations using photonuclear cross-section data. In the present work, we interrogated depleted uranium with a 9-MV electron linac and detected photoneutrons with trans-stilbene organic scintillators. The measurement of photoneutrons with organic scintillators is challenging due to the presence of the intense photon flux, which causes issues such as pulse pile-up, detector saturation, and poor signal-to-background ratio. To mitigate these challenges, we used iron and polyethylene shielding of varying thicknesses around the depleted uranium target and a neural network–based digital pulse processing algorithm to recover neutron and photon information from piled-up events. Our goal was to compare the measured photoneutron count rate with the simulated rate obtained using the MCNPX-PoliMi transport code. For a light output window of 0.28 to 2.67 MeVee (1.66- to 6.85-MeV proton recoil energy), we found that the simulated count rate obtained using the ENDF/B-VII photonuclear cross-section library underpredicts the measured rate by 32.8% 3.2%. Additionally, we compared the simulated and measured photoneutron light output distributions. For the least thicknesses of shielding, the simulation was found to underpredict measurements in the 0.70- to 2.67-MeVee light output window. For the greatest thicknesses of shielding, the simulation was found to underpredict the measurement across the entire light output window of 0.28 to 2.67 MeVee.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2017

Process Developments in the Fabrication of Depleted Uranium Hohlraums

Research at General Atomics and Lawrence Livermore National Laboratory has been focused on evaluating depleted uranium (DU) hohlraum fabrication over the past 10 years to improve the yield, thereby increasing the availability of DU hohlruams required to support the increased shot rate at the National Ignition Facility. The more straightforward gold (Au) hohlraum fabrication involves four basic steps: mandrel fabrication, electroplating, back machining and milling, and leaching. For Au, the overall fabrication yield of this process approaches 98%. Depleted uranium lined hohlraum fabrication, however, requires deposition of a multilayer of thin films after the mandrel fabrication step. These thin film deposition processes have historically proven difficult to execute on a complex cylindrical geometry of a hohlraum, resulting in unacceptable stress-driven delamination, with net yields ranging 20% to 35%. Recent hohlraum design and fabrication process changes, as well as material selections implemented between 2014 and 2016, have improved the fabrication yield to over 60%. Additionally, these changes are discussed here as well as plans for future improvements.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Anthropogenic uranium signatures in turtles, tortoises, and sea turtles from nuclear sites

Chelonians (turtles, tortoises, and sea turtles) grow scute keratin in sequential layers over time. Once formed, scute keratin acts as an inert reservoir of environmental information. For chelonians inhabiting areas with legacy or modern nuclear activities, their scute has the potential to act as a time-stamped record of radionuclide contamination in the environment. Here, we measure bulk (i.e., homogenized scute) and sequential samples of chelonian scute from the Republic of the Marshall Islands and throughout the United States of America, including at the Barry M. Goldwater Air Force Range, southwestern Utah, the Savannah River Site, and the Oak Ridge Reservation. We identify legacy uranium ( 235 U and 236 U) contamination in bulk and sequential chelonian scute that matches known nuclear histories at these locations during the 20th century. Our results confirm that chelonians bioaccumulate uranium radionuclides and do so sequentially over time. This technique provides both a time series approach for reconstructing nuclear histories from significant past and present contexts throughout the world and the ability to use chelonians for long-term environmental monitoring programs (e.g., sea turtles at Enewetok and Bikini Atolls in the Republic of the Marshall Islands and in Japan near the Fukushima Daiichi reactors).

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
DOE OSTI2020

Occupational Contamination with a Highly Enriched Uranium Solution

This medical case report describes the first reported instance of occupational skin contamination with a uranyl nitrate solution containing highly enriched uranium. The report provides an overview of the unique medical treatment and management considerations in such a case. Herein, internal dose assessment is covered in detail. The discussion covers key points regarding uranium characteristics, chemical and radiological damage to body tissues from HEU exposure, and resources available for assistance with a case of radiological contamination. This information adds to the limited medical literature on this topic and provides a valuable reference for medical personnel when dealing with this uncommon problem.

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗