The Challenges of α-Uranium: Fundamental Understanding of a Past and Future Nuclear Fuel Material [Poster]
The challenges of α-uranium: fundamental understanding of a past and future nuclear fuel material.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
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Demonstrating compliance with moderator content limits in uranium dioxide powder upon leaving a furnace environment
A challenge was posed to the criticality safety consultant to consider whether instrumentation identified by Plant Management in an existing facility could be claimed as appropriate safety measures to ensure compliance with moderator content limits in uranium dioxide (UO{sub 2}) powder. During processing of low enriched UO{sub 2}, trays of powder are heated in a steam and hydrogen environment in order to reduce fluoride levels. Whilst in the furnace environment criticality safety is ensured by the geometry of the furnace trays used to convey the powder; however, upon leaving the furnace the UO{sub 2} is bulked to a 210 litre drum subject to limited moderation control. Under fault conditions there is a potential that the powder may become wetted due to an imbalance in furnace gas flows resulting in steam condensing in the cooling section of the furnace. Therefore, the safety case methodology followed suggests that two independent and diverse safety measures are provided to terminate the progression of the fault(s) to criticality. The existing criticality safety case credits an infra-red moisture meter as one of two safety measures; however, the calibration procedure required to ensure this device remains suitable is a considerable challenge from a plant operability perspective. As an initial review failed to identify any suitable like-for-like replacement, the National Nuclear Laboratory (NNL) Nuclear Safety Section were requested by the customer to consider the existing criticality safety case and investigate whether any existing instrumentation could be used as an alternative method of detecting conditions in which excess moisture could be present within the furnace trays. A number of solutions were proposed and the benefits and challenges around each are discussed in this paper, concluding with the approach adopted by the project. (authors)
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
The Stability of SiO{sub 2} Fe{sub 3}O{sub 4} Nanoparticles for Uranium Extraction in Acidic Media - 20189
This comprehensive study has shown that the proposed strategy of SiO{sub 2} coating of Fe{sub 3}O{sub 4} nanoparticles (NPs) for the use of uranium (U) extraction in acidic media was successful. The breakdown of Fe{sub 3}O{sub 4} in acidic media has proven to be a challenge when applying to a nuclear waste removal scenario, leading to the dissolution of Fe{sub 3}O{sub 4} and preventing uptake of U ions in the waste. To overcome this a SiO{sub 2} passivating layer was grafted to the Fe{sub 3}O{sub 4} NPs, to which an acid stability test was conducted between pH 3 and pH 4. It has been shown via Transmission Electron Microscopy (TEM) and zeta potential measurements that the uncoated Fe{sub 3}O{sub 4} NPs exhibit rapid coagulation when exposed to acidic conditions, moving from a stable zeta potential of -44 mV to an unstable zeta potential of +6 mV. SiO{sub 2} coated Fe{sub 3}O{sub 4} on the other hand can remain stable for several hours and continue to be stable beyond that. Throughout acid exposure the zeta potential of these NPs remained at ∼ -38 mV, showing great stability. As a functionality is needed on the surface of the NPs for separation and extraction, the phosphate complex used was also tested for its acid stability. It was determined that with a constant zeta potential of ∼ -20 mV, the phosphate functionality was able to remain stable in the acidic conditions simulating the environment of certain nuclear wastes. Overall SiO{sub 2} coated (PO)x-Fe{sub 3}O{sub 4} NPs show great promise for application in separation and removal of U in acid media. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Characterization of a Polyethylene Moderated Highly Enriched Uranium System
The polyethylene interstitial materials for the Class Foils experiment are one of the teaching tools used to teach criticality safety at the National Criticality Experiments Research Center (NCERC). This set of polyethylene plates is designed to provide the optimal H/{sup 235}U ratio on the critical mass curve allowing the experiment to have the minimum amount of {sup 235}U. This makes a great teaching tool to show that either additional {sup 235}U or additional moderator would increase the critical mass. The optimal H/{sup 235}U ratio and increased hydrogen density compared to the previously used Lucite plates has reduced the critical mass by 34%, to 997.9 ± 0.65 g. The robustness of this experiment makes it ideal for hands on training. The fuel foils consist of thin highly enriched uranium (93 wt% {sup 235}U) metal foils laminated in plastic; each foil weighs approximately 68 grams. The fuel is interleaved between interstitial plates to attain a critical configuration. The critical configuration requires 14.5 fuel foils. Rossi-α experiments have been proposed as a method of benchmarking kinetics properties given by neutronics codes such as MCNP. (authors)
07 ISOTOPE AND RADIATION SOURCES↗
Induced Ferromagnetism in Epitaxial Uranium Dioxide Thin Films
Abstract Actinide materials have various applications that range from nuclear energy to quantum computing. Most current efforts have focused on bulk actinide materials. Tuning functional properties by using strain engineering in epitaxial thin films is largely lacking. Using uranium dioxide (UO 2 ) as a model system, in this work, the authors explore strain engineering in actinide epitaxial thin films and investigate the origin of induced ferromagnetism in an antiferromagnet UO 2 . It is found that UO 2+ x thin films are hypostoichiometric ( x <0) with in‐plane tensile strain, while they are hyperstoichiometric ( x >0) with in‐plane compressive strain. Different from strain engineering in non‐actinide oxide thin films, the epitaxial strain in UO 2 is accommodated by point defects such as vacancies and interstitials due to the low formation energy. Both epitaxial strain and strain relaxation induced point defects such as oxygen/uranium vacancies and oxygen/uranium interstitials can distort magnetic structure and result in magnetic moments. This work reveals the correlation among strain, point defects and ferromagnetism in strain engineered UO 2+ x thin films and the results offer new opportunities to understand the influence of coupled order parameters on the emergent properties of many other actinide thin films.
36 MATERIALS SCIENCE↗
Emergence of Uranium as a Distinct Metal Center for Building Intrinsic X-ray Scintillators
The combination of high atomic number and high oxidation state in U VI materials gives rise to both high X-ray attenuation efficiency and intense green luminescence originating from ligand-to-metal charge transfer. These two features suggest that U VI materials might act as superior X-ray scintillators, but this postulate has remained substantially untested. Now the first observation of intense X-ray scintillation in a uranyl–organic framework (SCU-9) that is observable by the naked eye is reported. Combining the advantage in minimizing the non-radiative relaxation during the X-ray excitation process over those of inorganic salts of uranium, SCU-9 exhibits a very efficient X-ray to green light luminescence conversion. The luminescence intensity shows an essentially linear correlation with the received X-ray intensity, and is comparable with that of commercially available CsI:Tl. SCU-9 possesses an improved X-ray attenuation efficiency (E>20 keV) as well as enhanced radiation resistance and decreased hygroscopy compared to CsI:Tl.
Chemistry↗
A roadmap to uranium ionic liquids: Anti-crystal engineering
In the search for uranium-based ionic liquids, tris(N,N-dialkyldithiocarbamato)uranylates have been synthesized as salts of the 1-butyl-3-methylimidazolium (C 4 mim) cation. As dithiocarbamate ligands binding to the UO 2 2+ unit, tetra-, penta-, hexa-, and heptamethylenedithiocarbamates, N,N-diethyldithiocarbamate, N-methyl-N-propyldithiocarbamate, N-ethyl-N-propyldithiocarbamate, and N-methyl-N-butyldithiocarbamate have been explored. X-ray single-crystal diffraction allowed unambiguous structural characterization of all compounds except N-methyl-N-butyldithiocarbamate, which is obtained as a glassy material only. In addition, powder X-ray diffraction as well as vibrational and UV/Vis spectroscopy, supported by computational methods, were used to characterize the products. Differential scanning calorimetry was employed to investigate the phase-transition behavior depending on the N,N-dialkyldithiocarbamato ligand with the aim to establish structure–property relationships regarding the ionic liquid formation capability. Compounds with the least symmetric N,N-dialkyldithiocarbamato ligand and hence the least symmetric anions, tris(N-methyl-N-propyldithiocarbamato)uranylate, tris(N-ethyl-N-propyldithiocarbamato)uranylate, and tris(N-methyl-N-butyldithiocarbamato)uranylate, lead to the formation of (room-temperature) ionic liquids, which confirms that low-symmetry ions are indeed suitable to suppress crystallization. As a result, these materials combine low melting points, stable complex formation, and hydrophobicity and are therefore excellent candidates for nuclear fuel purification and recovery.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Characterization of uranium tetrafluoride (UF 4 ) with Raman spectroscopy
The Raman spectrum of uranium tetrafluoride (UF 4 ) is unambiguously characterized with multiple Raman excitation laser sources for the first time. Across different laser excitation wavelengths, UF 4 demonstrates 16 distinct Raman bands within the 50-400 cm -1 region. The observed Raman bands are representative of various F-F vibrational modes. UF 4 also shows intense fluorescent bands in the 325 – 750 nm spectral region. Comparison of the UF 4 spectrum with the ZrF 4 spectrum, its crystalline analog, demonstrates a similar Raman band structure consistent with group theory predictions for expected Raman bands. Additionally, a demonstration of combined scanning electron microscopy (SEM) and in situ Raman spectroscopy microanalytical measurements of UF 4 particulates shows that despite the inherent weak intensity of Raman bands, identification and characterization are possible for micron-sized particulates with modern instrumentation. The published well characterized UF 4 spectrum is extremely relevant to nuclear materials and nuclear safeguard applications.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Solubility of Uranium Hexafluoride in Liquid Metal Penta- and Hexafluorides
The existence of a linear dependence of the mutual solubility of the higher fluorides of group-V and –VI metals on the atomic number of the solvent metal was established. The solubility of uranium hexafluoride in liquid metal pentafluorides is shown to be a linear function of the parameter α/r {sup 6} of the solvent.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Swelling of Uranium Dioxide–Silumin Dispersion Fuel Composition in Experimental Fuel Elements of the SM Reactor
A variant of experimental dispersion fuel elements with a displacer and uranium dioxide-silumin fuel composition, which were proposed for modernizing the core of the SM reactor, was investigated. The fuel elements were irradiated in a wide spectrum of neutron- and thermophysical parameters of the reactor’s reflector channel. The fuel elements showed satisfactory radiation resistance at thermal flux density 5.8–8 MW/m{sup 2} and burnup to 45%. The swelling of the fuel composition was analyzed. It is shown that of three possible components of the swelling the one due to gaseous fission products makes the main contribution, approximately 3/4 of the total amount. The interaction of the fuel components results in compaction of the kernel and promotes some compensation of the swelling, increasing as the interaction increases. These investigations show that the depth of burnup at the achieved thermal flux density for fuel elements with a displacer is not the limit.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Calculation of the Present Value of Separative Work for Uranium Isotopes
An economics-mathematical model for performing analytical calculations of the present value of separative work for uranium isotopes in a separation plant currently being designed using gas centrifuge technology is examined. Analytical expressions are obtained for the present value of the separative work, the internal rate of return, and the payback period of the separation plant as a function of its main engineering and economics parameters – productivity (capacity), capital investment, and operating expenses. Calculations of these criteria for investment efficiency are presented for a wide range of initial data. It is shown that the calculation of the present value of separative work must be performed in a complex with other investment efficiency criteria in order to determine their optimal combination.
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Determination of initial fuel state and number of reactor shutdowns in archived low-burnup uranium targets
This article presents a method for destructive analysis of irradiated uranium (U) targets, with a focus on collection and measurement of long-lived (t 1/2 > ~10 years) and stable fission product isotopes of ruthenium and cesium. Long-lived and stable isotopes of these elements can provide information on reactor conditions (e.g. flux, irradiation time, cooling time) in old samples (> 5–10 years) whose short-lived fission products have decayed away. The separation and analytical procedures were tested on archived U reactor targets at Los Alamos National Laboratory as part of an effort to evaluate reactor models at low-burnup.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Combination of atomic lines and molecular bands for uranium optical isotopic analysis in laser induced plasma spectrometry
Through computer simulation on experimentally acquired optical spectra, uranium isotopic analysis by laser ablation molecular isotopic spectrometry and laser induced breakdown spectroscopy were studied. The use of only one spectral feature, either the strong UO band at 593.55 nm or the nearby U I 593.382 nm line, are similar in precisions (~ 1.5% in absolute 235 U abundances). Precision improves to 0.72% with the use of a group of U atomic lines from 591.6 to 596.5 nm. The use of both molecular bands and atomic lines further advances the precision to 0.42% and compares well with the U II 424.437 nm single-line benchmark (0.48% precision).
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Chlorination of uranium metal in molten NaCl-CaCl 2 via bubbling HCl
Molten chloride salt fast reactors (MCFRs) will require UCl 3 dissolved in molten salt mixtures as fuel for nuclear fission. For infusing the salt with UCl 3 , bubbling HCl into NaCl-CaCl 2 in contact with U metal was investigated. The reaction was run up to 9 h and yielded U concentration up to 0.652 wt.%. Open circuit potential between a W electrode and Ag/AgCl reference electrode yielded a potential consistent with uranium existing as U(III) in the salt. Furthermore, this demonstrates that HCl can be a very effective chlorinating agent to infuse MCFR fuel with UCl 3 starting from U metal.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Updated uranium reference material 231 Pa/ 235 U consensus model ages for nuclear forensics
Radiochronometry provides the model age of nuclear materials, which is useful for understanding the production history of materials found outside of regulatory control. Certified reference materials (CRMs) are important for radiochronometry to increase confidence in measurement quality; however, the absence of 231 Pa/ 235 U CRMs necessitates that nuclear forensic laboratories measure the 231 Pa/ 235 U model ages of preexisting uranium reference materials. Here, in this work, new consensus 231 Pa/ 235 U model ages are reported from three nuclear forensic laboratories for three reference materials using current analytical methods. These updated consensus values can be used for quality control of 231 Pa/ 235 U model age measurements.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Neutron capture signatures determined from gadolinium isotope compositions of uranium ore concentrates using MC-ICPMS
We present Gd isotope compositions on 25 well-characterized uranium ore concentrates (UOCs). About half the UOCs have isotope depletions in 157 Gd coupled with anticorrelated excesses in 158 Gd due to neutron capture effects. UOCs from older ore bodies and with higher U contents show larger neutron capture effects than UOCs from younger ore bodies with lower U contents. These Gd data are correlated with their previously measured Sm isotope compositions, and we use the Sm data to estimate the neutron fluence of these samples. In conclusion, this work demonstrates how Gd isotope signatures can be employed as a new tool for nuclear forensics.
Earth Sciences↗
Quantifying uncertainty in uranium concentration measurements via K-edge densitometry
This study quantifies the uncertainty in uranium concentration predictions of fluoride and chloride-based salts within a steel pipe using K-edge densitometry. Modeling and simulation was conducted with the Monte Carlo N-Particle Transport (MCNP) code. The quality of of this technique’s prediction in a pipe requires proper characterization of the pipe’s thickness, which is dependent on the source size and axial offset from the pipe centerline. The thickness was determined as either the center-line thickness seen by the X-ray source or an average value determined through random sampling. Generally, the predicted concentrations were slightly better at lower offset with the random sampling thickness and using the center-line thickness for the highest offsets. For a line-beam source and varying axial offsets, the relative error of concentration was within 1% of the true value but uncertainty increased by 2 orders of magnitude. Similarly, for no axial offset, the relative error was significantly less than 1% while no trend for uncertainty was found. However, at the largest possible offset for a given source size, the concentrations become erroneous and greater than the allowable 1% relative error. Furthermore, high offsets tended to increase the variance of the transmission spectra by 3 orders of magnitude.
Characterization and Analytical Technique↗
Characterizing microscale signatures in uranium ore concentrates using electron probe microanalyzer
Impurities in uranium ore concentrates (UOCs) serve as forensic signatures of processing history and origin. Here, this study utilizes Electron Probe Microanalyzer (EPMA) to characterize microscale compositional and textural features in individual UOC particles from both commercial and bench-scale production. At the particle scale, multiple internal phases with distinct morphologies, chemical signatures, and stoichiometries are documented. Our data shows that chemical impurities are heterogeneously distributed within single particles and among particles within a sample. These microscale heterogeneities correlate with known processing histories, indicating that microscale signatures of early fuel cycle materials can provide valuable information for nuclear forensic material analysis.
organic↗