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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Discriminating Uranium Isotopes Based on Fission Signatures Induced by Delayed Neutrons

The use of active interrogation to induce delayed neutron emission is a well-established technique for the characterization of special nuclear materials. Delayed neutrons have isotope-characteristic spectral and temporal signatures, which provide the basis for isotope identification. However, in bulk materials that contain an appreciable fissile (e.g., 235 U or 233 U) fraction, such as highly enriched uranium (HEU), delayed neutrons have a high probability of inducing additional fissions. As a result, the overall delayed neutron signature consists of two distinct components: the “primary” delayed neutrons (emitted directly by fission fragments) and the “secondary prompt” fission neutrons produced in fission induced by primary delayed neutrons. These prompt products differ from “primary” delayed neutrons both in their energy spectra and in the presence of coincident radiation released by the parent fission event. The presence and relative quantity of prompt products from delayed fission depend on the cross section of the material in the energy range of delayed neutrons, which may differ significantly between isotopes, thus providing an exploitable means for isotope differentiation. Here, we demonstrate two experimental approaches for discriminating between 235 U and 238 U isotopes based on the measurement of delayed neutron-induced fission products. First, HEU and depleted uranium objects are differentiated through the detection of high-energy prompt neutrons from delayed fission using both recoil-based organic liquid scintillators and thermalization spectra from a custom-built capture-gated composite detector. Secondly, coincident radiation measurements are used as the basis for discrimination by comparing the overall rates and time evolution of fission events when delayed neutrons are present.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2020

Giant magnetic anisotropy energy and long coherence time of uranium substitution on defected Al 2 O 3 (0001)

Nanomagnets with giant magnetic anisotropy energy and long coherence time are desired for various technological innovations such as quantum information procession and storage. Based on the first-principles calculations and model analyses, we demonstrate that a single uranium atom substituting Al on the Al 2 O 3 (0001) surface may have high structural stability and large magnetic anisotropy energy up to 48 meV per uranium atom. As the magnetization resides in the localized $\textit{f}$ shell and is not much involved in chemical bonding with neighbors, long coherence time up to ~1.6mS can be achieved for the quantum spin states. These results in this work suggest a different strategy for the search of ultrasmall magnetic units for diverse applications in the quantum information era.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Magnetic anisotropy in uranium monosulfide probed by magnetic torque measurements

We have studied the magnetic torque in uranium monosulfide (US) single crystals to explore the magnetic anisotropy in this material. Uranium monosulfide crystallizes in a cubic, NaCl-type of crystal structure and exhibits the largest magnetocrystalline anisotropy observed in cubic systems. By performing detailed torque measurements we observe a strongly anisotropic behavior in the paramagnetic phase due to crystal defects and quadrupolar pair interactions. Our studies also confirm the presence of a large anisotropy in the ferromagnetic state of the US system with the <100>, <111>, and <110> directions being the hard, easy, and intermediate axes, respectively. Furthermore, the anisotropy in the paramagnetic phase shows similar characteristics to the anisotropy observed in the ferromagnetic phase, as characterized by second and fourth rank susceptibility terms. The similarity of the anisotropic behaviors in paramagnetic and ferromagnetic phases is the consequence of strong magnetoelastic properties in this system, which possibly lead to the rhombohedral structural distortion, not only in the ferromagnetic phase but also in the paramagnetic phase (induced by applied magnetic field).

36 MATERIALS SCIENCE↗
DOE OSTI2014

Using Monte Carlo ray tracing simulations to model the quantum harmonic oscillator modes observed in uranium nitride

Recently an extended series of equally spaced vibrational modes was observed in uranium nitride (UN) by performing neutron spectroscopy measurements using the ARCS and SEQUOIA time-of- flight chopper spectrometers [A.A. Aczel et al, Nature Communications 3, 1124 (2012)]. These modes are well described by 3D isotropic quantum harmonic oscillator (QHO) behavior of the nitrogen atoms, but there are additional contributions to the scattering that complicate the measured response. In an effort to better characterize the observed neutron scattering spectrum of UN, we have performed Monte Carlo ray tracing simulations of the ARCS and SEQUOIA experiments with various sample kernels, accounting for the nitrogen QHO scattering, contributions that arise from the acoustic portion of the partial phonon density of states (PDOS), and multiple scattering. These simulations demonstrate that the U and N motions can be treated independently, and show that multiple scattering contributes an approximate Q-independent background to the spectrum at the oscillator mode positions. Temperature dependent studies of the lowest few oscillator modes have also been made with SEQUOIA, and our simulations indicate that the T-dependence of the scattering from these modes is strongly influenced by the uranium lattice.

Lin, J. Y. Y.↗
DOE OSTI2022

Crystal structure of a trigonal polymorph of aquadioxidobis(pentane-2,4-dionato-κ 2 O , O ′)uranium(VI)

The title compound, [UO 2 (acac) 2 (H 2 O)] consists of a uranyl(VI) unit ([O=U=O] 2+ ) coordinated to two monoanionic acetylacetonate (acac, C 5 H 7 O 2 ) ligands and one water molecule. The asymmetric unit includes a one-half of a uranium atom, one oxido ion, one-half of a water molecule and one acac ligand. The coordination about the uranium atom is distorted pentagonal–bipyramidal. The acac ligands and O w atom comprise the equatorial plane, while the uranyl O atoms occupy the axial positions. Intermolecular hydrogen bonding between complexes results in the formation of two-dimensional hexagonal void channels along the c- axis direction with a diameter of 6.7 Å. The monoclinic ( P 2 1 / c space group) polymorph was reported by Alcock & Flanders [(1987). Acta Cryst. C 43 , 1480–1483].

Hernandez, Alejandro↗
DOE OSTI2015

Influence of Carbon and Microbial Community Priming on the Attenuation of Uranium in a Contaminated Floodplain Aquifer

The capacity for subsurface sediments to sequester metal contaminants, such as uranium (U), and retain them after bioremediation efforts are completed is critical to site stewardship. Sediments enriched in natural organic matter are capable of sequestering significant quantities of U, but may also serve as sources to the aquifer, contributing to plume persistence. Two types of sediments were compared to better understand the mechanisms contributing to the sequestration and release of U in the presence of organic matter. Artificially bioreduced sediments were retrieved from a field experimental plot previously stimulated with acetate while naturally bioreduced sediments were collected from a location enriched in organic matter but never subject to acetate amendment. Batch incubations demonstrated that the artificially bioreduced sediments were primed to rapidly remove uranium from the groundwater whereas naturally bioreduced sediments initially released a sizeable portion of sediment U before U(VI)-removal commenced. Column experiments confirmed that U release persisted for 65 pore volumes in naturally bioreduced sediments, demonstrating the sink-source behavior of this sediment. Acetate addition to artificially bioreduced sediments shifted the microbial community from one dominated by sulfate-reducing bacteria within Desulfobacteraceae to the iron-reducing family Geobacteraceae and Firmicutes during U(VI) reduction. In contrast, initial Geobacteraceae communities innaturally reduced sediments were replaced by clone sequences with similarity to opportunistic Pseudomonas spp. during U release, while U(VI) removal occurred concurrent with enrichment of Firmicutes. These investigations stress the importance of characterizing zones with heterogeneous carbon pools at U contaminated sites prior to the determination of a remedial strategy.

Artificially reduced Rifle sediments↗
DOE OSTI2018

Production of near-full density uranium nitride microspheres with a hot isostatic press

Depleted uranium nitride (UN) kernels with diameters ranging from 420 to 858 microns and theoretical densities (TD) between 87 and 91 percent were postprocessed using a hot isostatic press (HIP) in an argon gas media. This treatment was shown to increase the TD up to above 97%. Uranium nitride is highly reactive with oxygen. Therefore, a novel crucible design was implemented to remove impurities in the argon gas via in situ gettering to avoid oxidation of the UN kernels. The density before and after each HIP procedure was calculated from average weight, volume, and ellipticity determined with established characterization techniques for particle. Furthermore, micrographs confirmed the nearly full densification of the particles using the gettering approach and HIP processing parameters investigated in this work.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2018

Characterization of Uranium Ore Concentrate Chemical Composition via Raman Spectroscopy

Uranium Ore Concentrate (UOC, often called yellowcake) is a generic term that describes the initial product resulting from the mining and subsequent milling of uranium ores en route to production of the U-compounds used in the fuel cycle. Depending on the mine, the ore, the chemical process, and the treatment parameters, UOC composition can vary greatly. With the recent advent of handheld spectrometers, we have chosen to investigate whether either commercial off-the-shelf (COTS) handheld devices or laboratory-grade Raman instruments might be able to i) identify UOC materials, and ii) differentiate UOC samples based on chemical composition and thus suggest the mining or milling process. Twenty-eight UOC samples were analyzed via FT-Raman spectroscopy using both 1064 nm and 785 nm excitation wavelengths. These data were also compared with results from a newly developed handheld COTS Raman spectrometer using a technique that lowers background fluorescence signal. Initial chemometric analysis was able to differentiate UOC samples based on mine location. Additional compositional information was obtained from the samples by performing XRD analysis on a subset of samples. The compositional information was integrated with chemometric analysis of the spectroscopic dataset allowing confirmation that class identification is possible based on compositional differences between the UOC samples, typically involving species such as U3O8, α-UO2(OH)2, UO4•2H2O (metastudtite), K(UO2)2O3, etc. While there are clearly excitation λ sensitivities, especially for dark samples, Raman analysis coupled with chemometric data treatment can nicely differentiate UOC samples based on composition and even mine origin.

Su, Yin-Fong↗
DOE OSTI2018

Uranium polyhydrides at moderate pressures: Prediction, synthesis, and expected superconductivity

Hydrogen-rich hydrides attract great attention due to recent theoretical (1) and then experimental discovery of record high-temperature superconductivity in H 3 S [T c = 203 K at 155 GPa (2)]. Here we search for stable uranium hydrides at pressures up to 500 GPa using ab initio evolutionary crystal structure prediction. Chemistry of the U-H system turned out to be extremely rich, with 14 new compounds, including hydrogen-rich UH 5 , UH 6 , U 2 H 13 , UH 7 , UH 8 , U 2 H 17 , and UH 9 . Their crystal structures are based on either common face-centered cubic or hexagonal close-packed uranium sublattice and unusual H 8 cubic clusters. Our high-pressure experiments at 1 to 103 GPa confirm the predicted UH 7 , UH 8 , and three different phases of UH 5 , raising confidence about predictions of the other phases. Many of the newly predicted phases are expected to be high-temperature superconductors. The highest-T c superconductor is UH 7 , predicted to be thermodynamically stable at pressures above 22 GPa (with T c = 44 to 54 K), and this phase remains dynamically stable upon decompression to zero pressure (where it has T c = 57 to 66 K).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Effect of Plutonium on Uranium Oxide Microstructural Fingerprint

The analysis of particulates from environmental sampling is routinely performed for nuclear forensics applications. In order to increase the tools available for nuclear forensics applications, capability development materials (CDMs), or reference particulates, are necessary for developing and benchmarking new analytical methods. Historically, these CDM particulates have been produced with highly controlled and characterized isotopic and size parameters for applications in developing and benchmarking particle sizers and mass spectrometry analytical methods [1- 4]. However, the development of CDMs with highly characterized particle morphology and phase of the particles is vital for aiding in the development and benchmarking of particle analytical methods for those parameters. In many cases, key properties such as crystallographic phase, morphology, and microstructure, may be correlated to processing history of environmental sampling particulates [5]. To that end, this work investigates determining the structural fingerprint of produced Pu-doped uranium oxide CDMs using transmission electron microscopy (TEM). The particulates, one of which shown in Figure 1, were synthesized to Fig. 1. Single particulate of uranium oxide fabricated using the THESEUS technique. develop capabilities for environmental sampling investigations. These particles are monodisperse at diameter of 1 μm and a range of plutonium concentrations from 0- 1,000 ppm. Given their small diameter, TEM analysis was ideal for studying the particulate structural fingerprint in detail. Previous investigations confirmed the external homogeneity of the particulates at different plutonium concentrations, however this analysis focuses on determining the grain structure, phase distribution, and porosity of the particulates.

Mayer, Jack [Univ. of Florida, Gainesville, FL (Un↗
DOE OSTI2022

Optical spectroscopic tools for standoff uranium detection

Rapid and standoff analysis of uranium is important for many applications. We present the recent advances in standoff detection of uranium using emission and laser-induced fluorescence spectroscopy in conjunction with ultrafast laser filament ablation-based solid sampling.

(020.3260) Isotope shifts, (140.3440) Laser-induce↗
DOE OSTI2017

The ultimate mineral processing challenge: Recovery of rare earths, phosphorus and uranium from Florida phosphatic clay

We report phosphate beneficiation in Florida generates more than one tonne of phosphatic clay, or slime, per tonne of phosphate rock produced. Since the start of the practice of large-scale washing and desliming for phosphate beneficiation, more than 2 Gt of slime has accumulated, containing approximately 600 Mt of phosphate rock, 600 kt of rare earth elements (REEs) and 80 million kilograms of uranium. The recovery of these valuable elements from the phosphatic clay is one of the most challenging endeavors in mineral processing, because the clay is extremely dilute, with an average solids concentration of 3 percent, and fine in size, with more than 50 percent having particle size smaller than 2 μm, and it contains nearly 50 percent clay minerals as well as large amounts of magnesium, iron and aluminum. With industry support and under funding from the Critical Materials Institute, the Florida Industrial and Phosphate Research Institute in conjunction with the Oak Ridge National Laboratory undertook the task to recover phosphorus, rare earths and uranium from Florida phosphatic clay. This paper presents the results from the preliminary testing of two approaches. The first approach involves three-stage cycloning using cyclones with diameters of 12.4 cm (5 in.), 5.08 cm (2 in.) and 2.54 cm (1 in.), respectively, to remove clay minerals followed by flotation and leaching. The second approach is a two-step leaching process. In the first step, selective leaching was conducted to remove magnesium, thus allowing the production of phosphoric acid suitable for the manufacture of diammonium phosphate (DAP) in the second leaching step. The results showed that multistage cycloning with small cyclones is necessary to remove clay minerals. Finally, selective leaching at about pH 3.2 using sulfuric acid was found to be effective for removing more than 80 percent of magnesium from the feed with minimal loss of phosphorus.

36 MATERIALS SCIENCE↗
DOE OSTI2013

Low Enriched Uranium Core Design for the Massachusetts Institute of Technology Reactor (MITR) with Un-finned 12 mil-thick Clad UMo Monolithic Fuel

This report contains the results of reactor fuel element design for conversion of the Massachusetts Institute of Technology Reactor (MITR) from the use of highly enriched uranium (HEU) fuel to the use of low enriched uranium (LEU) fuel. The analyses were performed by staff members of the Global Threat Reduction Initiative (GTRI) Reactor Conversion Program at the Argonne National Laboratory (ANL) and the Massachusetts Institute of Technology Nuclear Reactor Laboratory. The core conversion to LEU is being performed with financial support of the U.S. government.

Bergeron, A.↗
DOE OSTI2013

Preliminary Accident Analyses for Conversion of the Massachusetts Institute of Technology Reactor (MITR) from Highly Enriched to Low Enriched Uranium

The Massachusetts Institute of Technology Reactor (MITR-II) is a research reactor in Cambridge, Massachusetts designed primarily for experiments using neutron beam and in-core irradiation facilities. It delivers a neutron flux comparable to current LWR power reactors in a compact 6 MW core using Highly Enriched Uranium (HEU) fuel. In the framework of its non-proliferation policies, the international community presently aims to minimize the amount of nuclear material available that could be used for nuclear weapons. In this geopolitical context most research and test reactors, both domestic and international, have started a program of conversion to the use of LEU fuel. A new type of LEU fuel based on an alloy of uranium and molybdenum (U-Mo) is expected to allow the conversion of U.S. domestic high performance reactors like MITR. This report presents the preliminary accident analyses for MITR cores fueled with LEU monolithic U-Mo alloy fuel with 10 wt% Mo. Preliminary results demonstrate adequate performance, including thermal margin to expected safety limits, for the LEU accident scenarios analyzed.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2014

Preliminary Evaluation of Alternate Designs for HFIR Low-Enriched Uranium Fuel

Engineering design studies of the feasibility of conversion of the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) to low-enriched uranium (LEU) fuel are ongoing at Oak Ridge National Laboratory (ORNL) as part of an effort sponsored by the U.S. Department of Energy s Global Threat Reduction Initiative (GTRI)/Reduced Enrichment for Research and Test Reactors (RERTR) program. The fuel type selected by the program for the conversion of the five high-power research reactors in the U.S. that still use HEU fuel is a new U-Mo monolithic fuel. Studies by ORNL have previously indicated that HFIR can be successfully converted using the new fuel provided (1) the reactor power can be increased from 85 MW to 100 MW and (2) the fuel can be fabricated to a specific reference design. Fabrication techniques for the new fuel are under development by the program but are still immature, especially for the complex aspects of the HFIR fuel design. In FY 2012, the program underwent a major shift in focus to emphasize developing and qualifying processes for the fabrication of reliable and affordable LEU fuel. In support of this new focus and in an effort to ensure that the HFIR fuel design is as suitable for reliable fabrication as possible, ORNL undertook the present study to propose and evaluate several alternative design features. These features include (1) eliminating the fuel zone axial contouring in the previous reference design by substituting a permanent neutron absorber in the lower unfueled region of all of the fuel plates, (2) relocating the burnable neutron absorber from the fuel plates of the inner fuel element to the side plates of the inner fuel element (the fuel plates of the outer fuel element do not contain a burnable absorber), (3) relocating the fuel zone inside the fuel plate to be centered on the centerline of the depth of the plate, and (4) reshaping the radial contour of the relocated fuel zone to be symmetric about this centerline. The present studies used current analytical tools to evaluate the various alternate designs for cycle length, scientific performance (e.g., neutron scattering), and steady-state and transient thermal performance using both safety limit and nominal parameter assumptions. The studies concluded that a new reference design combining a permanent absorber in the lower unfueled region of all of the fuel plates, a burnable absorber in the inner element side plates, and a relocated and reshaped (but still radially contoured) fuel zone will allow successful conversion of HFIR. Future collaboration with the program will reveal whether the new reference design can be fabricated reliably and affordably. Following this feedback, additional studies using state-of-the-art developmental analytical tools are proposed to optimize the design of the fuel zone radial contour and the amount and location of both types of neutron absorbers to further flatten thermal peaks while maximizing the performance of the reactor.

Renfro, David G.↗
DOE OSTI2014

Preliminary Evaluation of Alternate Designs for HFIR Low-Enriched Uranium Fuel

Engineering design studies of the feasibility of conversion of the High Flux Isotope Reactor (HFIR) from high-enriched uranium (HEU) to low-enriched uranium (LEU) fuel are ongoing at Oak Ridge National Laboratory (ORNL) as part of an effort sponsored by the U.S. Department of Energy’s Global Threat Reduction Initiative (GTRI)/Reduced Enrichment for Research and Test Reactors (RERTR) program. The fuel type selected by the program for the conversion of the five high-power research reactors in the U.S. that still use HEU fuel is a new U-Mo monolithic fuel. Studies by ORNL have previously indicated that HFIR can be successfully converted using the new fuel provided (1) the reactor power can be increased from 85 MW to 100 MW and (2) the fuel can be fabricated to a specific reference design. Fabrication techniques for the new fuel are under development by the program but are still immature, especially for the “complex” aspects of the HFIR fuel design. In FY 2012, the program underwent a major shift in focus to emphasize developing and qualifying processes for the fabrication of reliable and affordable LEU fuel. In support of this new focus and in an effort to ensure that the HFIR fuel design is as suitable for reliable fabrication as possible, ORNL undertook the present study to propose and evaluate several alternative design features. These features include (1) eliminating the fuel zone axial contouring in the previous reference design by substituting a permanent neutron absorber in the lower unfueled region of all of the fuel plates, (2) relocating the burnable neutron absorber from the fuel plates of the inner fuel element to the side plates of the inner fuel element (the fuel plates of the outer fuel element do not contain a burnable absorber), (3) relocating the fuel zone inside the fuel plate to be centered on the centerline of the depth of the plate, and (4) reshaping the radial contour of the relocated fuel zone to be symmetric about this centerline. The present studies used current analytical tools to evaluate the various alternate designs for cycle length, scientific performance (e.g., neutron scattering), and steady-state and transient thermal performance using both safety limit and nominal parameter assumptions. The studies concluded that a new reference design combining a permanent absorber in the lower unfueled region of all of the fuel plates, a burnable absorber in the inner element side plates, and a relocated and reshaped (but still radially contoured) fuel zone will allow successful conversion of HFIR. Future collaboration with the program will reveal whether the new reference design can be fabricated reliably and affordably. Following this feedback, additional studies using state-of-the-art developmental analytical tools are proposed to optimize the design of the fuel zone radial contour and the amount and location of both types of neutron absorbers to further flatten thermal peaks while maximizing the performance of the reactor.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2015

Elevated and Low Temperature Deformation of Cast Depleted Uranium

Goals: Understand crystal structure and micro-structure changes during high and low temperature deformation of uranium, in particular texture, and develop constitutive micro-structure based model for uranium deformation. Deliverables achieved: Completed texture measures for 11 pre- and post-dU compression samples, quantified texture pre- and post-deformation, and provided data to constrain deformation models.

Materials Science(36)↗
DOE OSTI2015

Demonstration of femtosecond laser ablation inductively coupled plasma mass spectrometry for uranium isotopic measurements in U-10Mo nuclear fuel foils

The use of femtosecond laser ablation inductively coupled plasma mass spectrometry was used to demonstrate the feasibility of measuring the isotopic ratio of uranium directly in U-10Mo fuel foils. The measurements were done on both the flat surface and cross sections of bare and Zr clad U-10Mo fuel foil samples. The results for the depleted uranium content measurements were less than 10% of the accepted U235/238 ratio of 0.0020. Sampling was demonstrated for line scans and elemental mapping over large areas. In addition to the U isotopic ratio measurement, the Zr thickness could be measured as well as trace elemental composition if required. A number of interesting features were observed during the feasibility measurements which could provide the basis for further investigation using this methodology. The results demonstrate the feasibility of using fs-LA-ICP-MS for measuring the U isotopic ratio in U-10Mo fuel foils.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗