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At least 109 records · Page 6

230Th/234U radiochronometry for uranium materials by alpha spectrometry for nuclear forensics analysis

We have developed an alpha spectrometry method for 230Th/234U radiochronometry to determine the model separation age for uranium materials. This method offers an alternative to the more commonly used, but significantly more resource intensive multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) while providing similar accuracy and precision. The development included radiochemical separation of uranium and thorium, calibration of the 232U tracer and the alpha spectrometry measurement. The method was validated by analyzing a certified reference material, CRM 125-A, which is a uranium oxide pellet assay, isotopic, and radiochronometric standard. The results were compared to those obtained by our routine MC-ICP-MS 230Th/234U radiochronometry analysis method to assess the performance parameters for alpha spectrometry compared to the state-of-the-art technique.

Macsik, Zsuzsanna [Los Alamos National Laboratory

ROADRUNNER uranium nitride MiniFuel: Experimental design, fabrication and pre-irradiation baseline characterization for accelerated burnup testing

Uranium nitride (UN) is a promising fuel candidate for advanced reactor systems owing to its high uranium density and thermal conductivity; however, its qualification remains constrained by the scarcity of well-controlled irradiation performance data. Here, to address this limitation, the ROADRUNNER (Research On ADvancing the peRformance of UraNium Nitrides in Extreme enviRonments) campaign employs the MiniFuel platform in the High Flux Isotope Reactor (HFIR) to enable accelerated burnup irradiation testing under tightly controlled and largely isothermal conditions. This paper presents the experimental design, fuel fabrication, and pre-irradiation baseline characterization of the ROADRUNNER UN MiniFuel campaign. Thirty-six UN minidisc specimens were fabricated with systematically varied as-fabricated density (86–96% of theoretical density), carbon impurity content (961–5240 ppm), oxygen content (≤ ∼2000 ppm), and grain size (2.5–24 μm). The irradiation matrix spans nominal fuel temperatures of 873 K, 1173 K, and 1473 K and target burnups of 3.75%, 6.0%, and 7.5% fissions per initial metal atom (FIMA). Neutronic and thermal analyses were performed to define specimen-specific burnup accumulation and temperature histories, establishing the boundary conditions for subsequent in-pile behavior. Comprehensive pre-irradiation characterization—including dimensional metrology, density verification, impurity analysis, X-ray diffraction, Raman spectroscopy, scanning electron microscopy, X-ray computed tomography, and confocal profilometry—provides a detailed baseline for post-irradiation examination. Pre-irradiation data were further used to generate predictive estimates of fission gas release and swelling using existing empirical correlations. This quantitative comparison reveals substantial inter-model divergence at intermediate and elevated temperatures that exceeds propagated input uncertainties, highlighting structural gaps in the historical irradiation database. The ROADRUNNER irradiation campaign is currently underway in HFIR, with initial firs cycle completed in late 2025 and remaining targets scheduled through 2027. The experimental design and baseline dataset presented here establish the framework needed to interpret forthcoming post-irradiation measurements and to provide discriminating data for the validation and refinement of physics-based UN fuel performance models.

Lopes, Denise Adorno [Oak Ridge National Laborator

Depletion benchmark for a high-assay low-enriched uranium fuel experiment in the advanced test reactor

Reactor physics depletion benchmarks for high-assay low-enriched uranium (HALEU) fuel are limited in number. In particular, there is limited data for HALEU benchmarks for U-10Mo (uranium-10% molybdenum) plate fuel that is being developed for use in the United States’ high performance research reactors including the Advanced Test Reactor (ATR), Advanced Test Reactor Critical Facility (ATR-C), High Flux Isotope Reactor (HFIR), Massachusetts Institute of Technology Reactor (MITR), University of Missouri Research Reactor (MURR), National Bureau of Standards Reactor (NBSR). These six reactors currently operate with highly enriched uranium dispersed fuel in an aluminum matrix. In support of conversion to a HALEU fuel, qualification of U-10Mo formed into a monolithic foil is being performed. Fuel qualification involves irradiating fuel specimens in the ATR. The irradiation tests provide an opportunity to benchmark depletion capabilities of reactor physics codes in support of the ATR operation, as well as develop benchmarks that can be used by other institutions to benchmark other reactor physics codes. This paper documents the development of a benchmark model of the irradiation of the ATR Full-size plate In center flux trap Position 7 (AFIP-7) experiment using the depletion codes MC21 and Advanced Dimensional Depletion for Engineering of Reactors (ADDER).

Nielsen, Joseph W. [Idaho National Laboratory (INL

Direct Extraction of Uranium Oxides with N,N -Di(2-ethylhexyl)isobutyramide

The direct extraction of uranium from voloxidized nuclear fuel into an organic solvent offers several potential advantages over conventional hydrometallurgical reprocessing, including reducing the reprocessing plant footprint, providing an initial degree of decontamination from fission products, and minimizing the amount of secondary waste from nitric acid. In this work, the direct extraction of uranium oxides into 1.5 M N,N-di(2-ethylhexyl)isobutyramide (DEHiBA) in n-dodecane is examined. UV–vis spectra and distribution ratios of HNO 2 in 1.5 M DEHiBA as well as the equilibrium organic phase H 2 O concentrations in HNO 3 -loaded 1.5 M DEHiBA are also reported. Hypothesized reaction stoichiometries for the direct extraction of uranium from UO 2 , α-U 3 O 8 , and ε-UO 3 are verified through analysis of organic-phase U, HNO 2 , and HNO 3 concentrations after dissolution. Water generated by the dissolution results in the formation of a separate aqueous phase, which will need to be accounted for in future flowsheet design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Quantifying Outer- and Inner-Coordination Sphere Effects Using Uranium Redox Chemistry in Molten Salt Solutions

Defining the relative influence of intramolecular and intermolecular forces is a fundamental problem in chemistry that is difficult to quantify. To address this challenge, we developed a method to evaluate the relative impact of direct chemical bonding in the inner-coordination sphere vs effects from cations in the outer-coordination sphere by comparative analysis of uranium redox reactivity in various molten salts. We observed that outer-coordination sphere cations (M 1+ ) and inner-coordination sphere anions (X 1– ) both affected uranium redox reactivity, with more polarizing M 1+ and larger X 1– favoring uranium in low oxidation states. Changing M 1+ (Li, Na, K) shifted the U IV + e 1– ⇌ U III (U IV/III ) and U III + 3e 1– → U 0 metal potentials by +330 and +240 mV, respectively. Changing X 1– (Cl, Br, I) caused larger shifts of +440 mV for the U IV/III redox potential and +1060 mV for the U 0 metal deposition potential. Using Coulomb’s Law, we correlated these potentials with electrostatic interactions between UIII and the molten salt. This model provided a facile way of predicting redox chemistry within molten salts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

ATONA TE-TIMS of minor uranium isotopes (FY25 Mid-Year Report)

Isotopic measurements of the minor isotopes of uranium ( 233 U, 234 U, 236 U) are indispensable measures for material accountability and processing history but can be particularly challenging to accurately measure due to the very low abundance of the minor isotopes relative to 238 U, or 235 U in the case of highly enriched uranium (HEU). The goal of this project is to quantify detection limits for minor uranium isotope species at environmental levels (e.g 236 U/ 238 U < 10 -7 ) utilizing an ATONA-outfitted instrument and the Total Evaporation Thermal Ionization Mass Spectrometry (TE-TIMS) method. In the first half of Fiscal Year 2025, we set out to identify a suitable experimental material (Task 1) and to optimize our TE-TIMS measurement routine (Task 2). We have successfully identified a material and are in the process of getting an aliquot shipped to LANL. Simultaneously, we began working on our measurement routine utilizing CRM 112A. The results of each task are discussed in detail below.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS

High Flux Isotope Reactor Low-Enriched Uranium High Density Silicide Fuel Preliminary Design Update: System Transient Analysis

As a part of conversion efforts from highly enriched uranium (HEU) to low-enriched uranium (LEU) fuel under direction of the National Nuclear Security Administration of the U.S. Department of Energy, multiple proposed designs of the High Flux Isotope Reactor (HFIR) have been created and assessed regarding reactor physics performance metrics, including designs utilizing uranium silicide dispersion fuel (U3Si2-Al). This report updates the previous analyses that evaluated the nuclear safety performance of LEU fuel designs with respect to selected accident events from the HFIR Safety Analysis Report (SAR). Both the Low Density (LD) and High Density (HD) Optimized designs’ reactivity initiated accident fuel performance improved relative to the HEU fuel, attributed to greater 238 U negative Doppler feedback. However, the thermal margins for primary coolant system accidents were reduced with some acceptance criteria unable to be met. The need to resolve reduced thermal margin, open modeling items, and unresolved assumptions was identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Assessment of Uranium Isotope Impacts

This report examines the benefits and challenges associated with recycling recovered uranium (RU) from the used nuclear fuel (UNF) discharged from a once-through sodium-cooled fast reactor (SFR) with high-assay low-enriched uranium (HALEU) which has a higher residual U-235 content in the RU. However, there are three minor uranium isotopes that influence the value of the RU. There will be trace quantities of U-232 in RU, which can increase dose rates and, in turn, increase the cost of fuel fabrication. Additionally, the U-234 and U-236 isotopes are found in higher concentration in RU than in NU, and act as neutron poisons, requiring higher U-235 concentrations to compensate for the neutron poisoning effects of these isotopes.

07 ISOTOPE AND RADIATION SOURCES

Uranium Sorbent Development

This report describes the synthesis of amidoxime-based sorbents for uranium extraction from natural waters. Two sorbents were tested, a commercial polyacrylonitrile-based commercial yarn and a nonwoven polypropylene fabric that was grafted with polyacrylonitrile and itaconic acid. The commercial yarn was chosen due to the ease of access and anticipated reproducibility. The polypropylene fabric was produced exclusively during the previous DOE funded Uranium from Seawater campaign and is no longer available. The polypropylene fabric represented a comparison against material developed to extract uranium from seawater, not freshwater.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Experimental investigations of a uranium plasma pertinent to a self-sustaining plasma source

The research is pertinent to the realization of a self-sustained fissioning plasma for applications such as nuclear propulsion, closed cycle MHD power generation using a plasma core reactor, and heat engines such as the nuclear piston engine, as well as the direct conversion of fission energy into optical radiation (nuclear pumped lasers). Diagnostic measurement methods and experimental devices simulating plasma core reactor conditions are discussed. Studies on the following topics are considered: (1) ballistic piston compressor (U-235); (2) high pressure uranium plasma (natural uranium); (3) sliding spark discharge (natural uranium); (4) fission fragment interaction (He-3 and U-235); and (5) nuclear pumped lasers (He-3 and U-235).

Schneider, R. T.

Measured emissivities of uranium and tungsten plasmas.

Uranium and tungsten absorption coefficients between 2,500-8500 A were measured as functions of thermodynamic variables. A gas-driven shock tube was used to obtain plasma temperatures, heavy metal partial pressures, and total pressures in the ranges 7,000-12,000 K, 0.02-1.0 atm, and 3.0-48 atm, respectively. Emission and absorption data were recorded both photographically and photoelectrically. The spectral distributions, thermal dependence and line-to-continuum ratios of the uranium and tungsten radiation differ distinctly. The uranium data are compared with theoretical predictions and with results from other experiments.

Miller, M. H.

Testing of uranium nitride fuel in T-111 cladding at 1200 K cladding temperature

Two groups of six fuel pins each were assembled, encapsulated, and irradiated in the Plum Brook Reactor. The fuel pins employed uranium mononitride (UN) in a tantalum alloy clad. The first group of fuel pins was irradiated for 1500 hours to a maximum burnup of 0.7-atom-percent uranium. The second group of fuel pins was irradiated for about 3000 hours to a maximum burnup of 1.0-atom-percent uranium. The average clad surface temperature during irradiation of both groups of fuel pins was approximately 1200 K. The postirradiation examination revealed the following: no clad failures or fuel swelling occurred; less than 1 percent of the fission gases escaped from the fuel; and the clad of the first group of fuel pins experienced clad embrittlement whereas the second group, which had modified assembly and fabrication procedures to minimize contamination, had a ductile clad after irradiation.

Rohal, R. G.

Uranium nitride behavior at thermionic temperatures

The feasibility of using uranium nitride for in-core thermionic applications was evaluated in electrically heated thermal gradient tests and in flat plate thermionic converters. These tests indicated that grain boundary penetration of uranium nitride into both tungsten and rhenium will occur under thermal gradient conditions. In the case of the tungsten thermionic converter, this led to grain boundary rupture of the emitter and almost total loss of electrical output from the converter. It appears that uranium nitride is unsuitable for thermionic applications at the 2000 K temperatures used in these tests.

Phillips, W. M.

Unrestrained swelling of uranium-nitride fuel irradiated at temperatures ranging from 1100 to 1400 K (1980 to 2520 R)

Six fuel pins were assembled, encapsulated, and irradiated in the Plum Brook Reactor. The fuel pins employed uranium mononitride (UN) in a stainless steel (type 304L) clad. The pins were irradiated for approximately 4000 hours to burnups of about 2.0 atom percent uranium. The average clad surface temperature during irradiation was about 1100 K (1980 deg R). Since stainless steel has a very low creep strength relative to that of UN at this temperature, these tests simulated unrestrained swelling of UN. The tests indicated that at 1 percent uranium atom burnup the unrestrained diametrical swelling of UN is about 0.5, 0.8, and 1.0 percent at 1223, 1264, and 1306 K (2200, deg 2273 deg, and 2350 deg R), respectively. The tests also indicated that the irradiation induced swelling of unrestrained UN fuel pellets appears to be isotropic.

Rohal, R. G.

Calculations of the Electron Energy Distribution Function in a Uranium Plasma by Analytic and Monte Carlo Techniques

Electron energy distribution functions were calculated in a U235 plasma at 1 atmosphere for various plasma temperatures and neutron fluxes. The distributions are assumed to be a summation of a high energy tail and a Maxwellian distribution. The sources of energetic electrons considered are the fission-fragment induced ionization of uranium and the electron induced ionization of uranium. The calculation of the high energy tail is reduced to an electron slowing down calculation, from the most energetic source to the energy where the electron is assumed to be incorporated into the Maxwellian distribution. The pertinent collisional processes are electron-electron scattering and electron induced ionization and excitation of uranium. Two distinct methods were employed in the calculation of the distributions. One method is based upon the assumption of continuous slowing and yields a distribution inversely proportional to the stopping power. An iteration scheme is utilized to include the secondary electron avalanche. In the other method, a governing equation is derived without assuming continuous electron slowing. This equation is solved by a Monte Carlo technique.

Bathke, C. G.

Vacuum ultraviolet spectra of uranium hexafluoride/argon mixtures

The transmission properties of room temperature helium at pressures up to 20 atmospheres were determined in the wavelength range from 80 to 300 nm. Similarly, the transmission properties of uranium hexafluoride at 393 K (pressures less than 1.0 mm) were determined in the wavelength range from 80 to about 120 nm. The results show that high pressure helium is sufficiently transparent in the vacuum ultraviolet region (provided trace contaminants are removed) to be utilized as a transparent purge gas in future fissioning gaseous uranium plasma reactor experiments. Absorption cross sections for uranium hexafluoride were calculated from the data between 80 and 120 nm and were of the order of 10 to the -17 power sq cm.

Krascella, N. L.

Properties of radio-frequency heated argon confined uranium plasmas

Pure uranium hexafluoride (UF6) was injected into an argon confined, steady state, rf-heated plasma within a fused silica peripheral wall test chamber. Exploratory tests conducted using an 80 kW rf facility and different test chamber flow configurations permitted selection of the configuration demonstrating the best confinement characteristics and minimum uranium compound wall coating. The overall test results demonstrated applicable flow schemes and associated diagnostic techniques were developed for the fluid mechanical confinement and characterization of uranium within an rf plasma discharge when pure UF6 is injected for long test times into an argon-confined, high-temperature, high-pressure, rf-heated plasma.

Source record

Uranium plasma emission at gas-core reaction conditions

The results of uranium plasma emission produced by two methods are reported. For the first method a ruby laser was focused on the surface of a pure U-238 sample to create a plasma plume with a peak plasma density of about 10 to the 20th power/cu cm and a temperature of about 38,600 K. The absolute intensity of the emitted radiation, covering the range from 300 to 7000 A was measured. For the second method, the uranium plasma was produced in a 20 kilovolt, 25 kilojoule plasma-focus device. The 2.5 MeV neutrons from the D-D reaction in the plasma focus are moderated by polyethylene and induce fissions in the U-235. Spectra of both uranium plasmas were obtained over the range from 30 to 9000 A. Because of the low fission yield the energy input due to fissions is very small compared to the total energy in the plasma.

Williams, M. D.