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At least 73 records · Page 4

Uranium Carbide and Uranium-Metal Thermal Scattering Law Evaluations and Cross Sections [Slides]

New Uranium Carbide and Uranium Metal evaluations have been developed using the FLASSH platform. Ab initio LD/MD models converged electronic, magnetic, and dynamical properties and demonstrate good agreement with experimental data. Thermal scattering cross sections generate inelastic and elastic thermal neutron scattering libraries in FLASSH . New TSL evaluations occurred in the production of ENDF File 7 data for Uranium Carbide and Uranium Metal submitted to NNDC for ENDF/B-VIII.1 release.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Contribution of Uranium-Bearing Evaporites to Plume Persistence Issues at a Former Uranium Mill Site Riverton, Wyoming, USA

• Evaporites occur in an unsaturated silt layer, which is underlain by a sand and gravel aquifer. • These evaporites are rich in chloride across the site. • Uranium concentrations are higher in the evaporites that overlie the uranium contaminant plume. • Flooding can solubilize the evaporites in the silt layer and release chloride, sulfate (not shown), and uranium into the underlyingsand and gravel aquifer. • The uranium-rich evaporites can delay natural flushing, creating plume persistence near the Little Wind River.

54 ENVIRONMENTAL SCIENCES↗

Deformation Strengthening of Uranium and Dilute Uranium Alloys

The strength and ductility of uranium and dilute uranium alloys can be substantially improved by deformation strengthening. The yield strength of unalloyed uranium can be nearly doubled by rolling in the vicinity of 250°C. The embrittling effect of hydrogen is also overcome, eliminating the need for vacuum outgassing to obtain good ductility. Significant differences in longitudinal versus transverse tensile properties result, in part, from texture introduced by unidirectional rolling. Warm rolling of U-2.3%Nb results in both traditional strain hardening and a significant Bauschinger effect, resulting in differences between tensile and compressive yield strength. A similar combination of strain hardening and Bauschinger effect also occurs in deformation strengthened U-0.75%Ti. Warm rolling of U-0.75%Ti results in significantly better combinations of tensile yield strength and ductility than can be obtained by conventional age hardening. Warm rolling prior to aging also reduces the loss of ductility which typically accompanies conventional age hardening. Here, an approach is developed in which the effects of prior deformation on tensile and compressive yield strengths are analyzed in terms of texture, long-range dislocation, and Bauschinger effects. The Bauschinger effect is shown to vary in sign with the type of deformation, thus providing opportunities to tailor tensile and compressive properties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

In-Field Alpha Spectrometry to Assess Uranium Enrichment In Uranium Hexafluoride

A new In-Field Alpha Spectrometry (IFAS) system is being developed to allow quick turnaround measurements of uranium enrichment in uranium hexafluoride (UF6) samples. Samples are collected using specially-designed Single-Use Destructive Assay (SUDA) wafers which have an absorptive film of zeolite deposited onto a quartz or metal substrate. The SUDA samples, along with a special holder, are designed to be attached directly to a sampling tap at a gas centrifuge enrichment plant or a uranium conversion facility, allowing gaseous UF6 to come into direct contact with the zeolite. The zeolite absorbs this material and converts it into stable, safe UO2F2 within a few minutes. Once the sample has been collected it is transferred to the IFAS system where a solid-state, silicon alpha spectrometer is used to quantitatively measure the alpha emissions from 234U, 235U, and 238U in the sample. The IFAS system is a small, light-weight device that can be quickly turned on and put into use. The SUDA samples and IFAS hardware are designed so that thin-film spectra are produced, allowing a complete measurement with a final 235U:Utotal determination having a precision <±2% to be made in less than eight hours. This short time frame will allow an inspector to get results on-site within one working shift; further innovations may reduce this to even shorter times.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

In-Field Alpha Spectrometry to Assess Uranium Enrichment In Uranium Hexafluoride

A new In-Field Alpha Spectrometry (IFAS) system is being developed to allow quick turnaround measurements of uranium enrichment in uranium hexafluoride samples. Samples are collected using specially-designed Single-Use Destructive Assay (SUDA) wafers which have an absorptive thin film of zeolite deposited onto a quartz substrate. The SUDA samples, along with a special holder, are designed to be attached directly to a sampling tap at a gas centrifuge enrichment plant or a uranium conversion facility, allowing gaseous UF6 to come into direct contact with the zeolite. The zeolite absorbs this material and converts it into stable, safe UO2F2 within a few minutes. Once the sample has been collected it is transferred to the IFAS system where a solid-state, silicon alpha spectrometer is used to quantitatively measure the alpha emissions from 234U, 235U, and 238U form the sample. The SUDA samples are designed so that thin-film spectra are produced, and the SUDA samples and IFAS system are designed so that a complete measurement, with a final 235U:Utotal determination of <±2%, can be made in less than eight hours. This short time frame will allow an inspector to get results on-site within one working shift.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

In situ liquid SIMS analysis of uranium oxide

Trace analysis of nuclear materials in solid particles collected in the environment or particles in liquid slurry generated in nuclear material manufacturing processes can pinpoint elemental, organic, and isotopic signatures of nuclear fuel cycle activities and processes. Such information can support nuclear safeguards programs by increasing our ability to detect undeclared nuclear materials, routine activities for safeguarding at declared facilities, and illicit activities. However, trace radioactive material analysis in liquids and slurries is challenging using bulk approaches. For example, one drawback of sensitive analysis such as inductively coupled plasma mass spectrometry (ICP-MS) is that sample is consumed or destroyed as a result of the technical approach. We developed a vacuum compatible microfluidic interface to enable surface analysis of liquids and liquid-solid interactions using time-of-flight secondary ion mass spectrometry (ToF-SIMS). In this work, we illustrate initial results of liquid standards containing uranium using in situ liquid SIMS. Specifically a series of diluted uranium standards used for ICPMS analysis were studied and the limit of detection was estimated. Since the liquid SIMS analysis is almost nondestructive, the same sample can be analyzed by other more destructive approaches afterwards or saved for future references. Consequently, multimodal analysis is possible. Our results demonstrate that in situ liquid SIMS can be used as a new approach to analyze radioactive materials in liquid and slurry forms of relevance to the IAEA safeguards missions.

In situ liquid ToF-SIMS, uranium, limit of detecti↗

Challenges and opportunities to alloyed and composite fuel architectures to mitigate high uranium density fuel oxidation: Uranium mononitride

We see the challenges and opportunities to alloyed and composite fuel architectures designed and intended to mitigate oxidation of the fuel during a cladding breech of a water-cooled reactor are discussed in three review manuscripts developed in parallel, with the presented article focused on the oxidation performance of uranium mononitride. Several high uranium density fuels are under consideration for deployment as accident tolerant and/or advanced technology nuclear reactor fuels, including one on each: UN, U 3 Si 2 , UC and UB 2 . Presented here is the research motivation for the incorporation of additives, dopants, or composite fuel architectures to improve the oxidation/corrosion behavior of high uranium density nuclear fuels for use in LWRs. Furthermore, this review covers the literature on the degradation modes, thermodynamics, and oxidation performance of pure UN and UN-compounds as well as reported alloyed and composite architectures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Resilience of uranium mononitride/zirconium carbide composites and uranium-zirconium carbonitride in hot hydrogen for nuclear thermal propulsion

Nuclear thermal rockets require fuels capable of withstanding flowing hydrogen propellant up to 3200 K. Presently, there has not been a fuel type that reliably operates at these conditions. A promising candidate anticipated to endure this demanding environment is a ceramic-ceramic composite comprising of uranium mononitride and zirconium carbide. Further, this investigation assesses the behavior and resilience of variations of this composite and its resultant homogenized form (uranium-zirconium carbonitride) under two hot hydrogen conditions (2273 K and 3000 K). The findings revealed that composites that homogenize into UZrCN exhibit superior structural integrity in hydrogen compared to heterogeneous counterparts. Consequently, this study underscores the potential of homogenized uranium-zirconium carbonitride for enhanced performance in nuclear thermal propulsion applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Constraints in the Remediation of Uranium Former Uranium Mining Sites - 19586

Uranium mining and milling legacy sites still exist all over the world. Financial constraints play a key role in constraining the remediation of these sites, but a series of other factors must also be considered. The IAEA has been assisting its Member States in moving forward their remediation projects, and more specifically the Central Asian region has received dedicated attention in this aspect. In association with other international organisations such as the European Commission and European Bank of Reconstruction and Development among others in the scope of the CGULS initiative (Coordination Group of Uranium Legacy Sites), a series of activities have been put in place to assist the countries in that region. Through its Technical Cooperation Department, the IAEA has also supported other Member States to manage their legacies. The IAEA CIDER Project (Constraints in Decommissioning and Environmental Remediation) in its first phase investigated possible constraint to implementation of both decommissioning and environmental remediation projects, and collected successful experiences and lessons learned from remediation projects all over the world. It started with a survey in which almost 30 Member States participated. Constraints were examined in three main areas: i) Institutional Aspects (regulatory and policy); ii) Technological and iii) Social. These results have been published in a dedicated report available in the IAEA web page (also called the CIDER Baseline Report). Under the request of participating Member States, a second phase of CIDER has been initiated with a more focused (action oriented) character. In this regard experts developed a framework for helping countries in need under two major areas: Strategy Development and Implementation and Stakeholder Engagement Support. Two other initiatives under CIDER Phase II consisted of the Enhanced Capacity Building in Environmental Remediation (the so-called School of Environmental Remediation) and a database depicting the sites in and in need of remediation in a global perspective. This paper is intended to present and promote some aspects of the methodology conceived in CIDER Phase II to help countries establish remediation strategies that will facilitate overcoming some of the barriers mentioned above. Furthermore, it aims to discuss aspects that might be improved in the assistance provided by international organisations to countries in need of developing remediation projects, pointing out to some of the documented causes for not achieving more robust results. It is expected that the combination of different tools to share good practices e.g. web-based tools, e-Learning, webinars in addition to face-to-face training events, may enhance the chances of successful implementation of remediation of legacy sites, including former uranium production sites. This initiative opens a wide avenue for cooperation while providing a platform to bring together practitioners, regulators, contractors, funding organisations to enhance the support to be provided. By working together, more effective and sustainable results can be achieved and remediation of such sites implemented in a timely, safe and cost-effective way. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Challenges and opportunities to alloyed and composite fuel architectures to mitigate high uranium density fuel oxidation: uranium silicide

We report the challenges and opportunities to alloyed and composite fuel architectures designed and intended to mitigate oxidation of the fuel during a cladding breech of a water-cooled reactor are discussed in three review manuscripts developed in parallel, with the presented article focused on the oxidation performance of uranium silicide. Several high uranium density fuels are under consideration for deployment as accident tolerant and/or advanced technology nuclear reactor fuels, including UN, U 3 Si 2 , UC and UB 2 . Presented here are the literature for the U3Si2 degradation modes, thermodynamics, and oxidation performance of the pure compound and its reported alloyed and composite architectures. Furthermore, this review covers the materials and techniques for the incorporation of additives, dopants, or composite fuel architectures to improve the oxidation/corrosion behavior for high uranium density fuels for use in LWRs.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Revealing Disparate Chemistries of Protactinium and Uranium. Synthesis of the Molecular Uranium Tetroxide Anion, UO 4 –

The synthesis, reactivity, structures, and bonding in gas-phase binary and complex oxide anion molecules of protactinium and uranium have been studied by experiment and theory. The oxalate ions, An V O 2 (C 2 O 4 ) - , where An = Pa or U, are essentially actinyl ions, An V O 2 + , coordinated by an oxalate dianion. Both react with water to yield the pentavalent hydroxides, An V O(OH) 2 (C 2 O 4 ) - . The chemistry of Pa and U becomes divergent for reactions that result in oxidation: whereas Pa VI is inaccessible, U VI is very stable. The U V O 2 (C 2 O 4 ) - complex exhibits a remarkable spontaneous exothermic replacement of the oxalate ligand by O 2 to yield UO 4 - and two CO 2 molecules. The structure of the uranium tetroxide anion is computed to correspond to distorted uranyl, U VI O 2 2+ , coordinated in the equatorial plane by two equivalent O atoms each having formal charges of -1.5 and U-O bond orders intermediate between single and double. The unreactive nature of Pa V O 2 (C 2 O 4 ) - toward O 2 is a manifestation of the resistance toward oxidation of Pa V , and clearly reveals the disparate chemistries of Pa and U. The uranium tetroxide anion, UO 4 - , reacts with water to yield UO 5 H 2 - . Infrared spectra obtained for UO 5 H 2 - confirm the computed lowest-energy structure, UO 3 (OH) 2 -

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Electronic excitation of uranium atoms sputtered from uranium metal and oxides

Atoms sputtered from solids by energetic ion irradiation often partition across electronically excited states. We developed a resonance ionization method to measure the population of the uranium 5 K 5 state (620 cm -1 ) relative to the 6 L 6 ground state for atoms sputtered from metallic and oxide surfaces. A considerable fraction of sputtered atoms reside in the 5 K 5 state, and the fraction increases as the surface oxidizes. The effect is consistent across uranium metal, UO 2 , and U 3 O 8 , and is invariant with the departing velocity of the sputtered atom. The data are not sufficient to determine the excitation mechanism, however they are qualitatively consistent with resonant electron transfer from the surface to the departing atom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Trace Uranium Partitioning in a Multiphase Nano-FeOOH System

The characterization of trace elements in nanomaterials using extended X-ray absorption fine structure (EXAFS) spectroscopy constitutes a first step toward understanding how impurities or dopants affect the properties of the host phase. However, limitations to EXAFS interpretation complicate the analysis of trace concentrations of impurities that are distributed across multiple phases in a heterogeneous system. Ab initio molecular dynamics (AIMD)-informed EXAFS analysis was employed to investigate the immobilization of trace uranium associated with nanophase iron (oxyhydr)oxides, a model system for the geochemical sequestration of radiotoxic contaminants. The reductive transformation of ferrihydrite (Fe(OH)3) to nano-particulate iron oxyhydroxide minerals in the presence of uranyl (UO2)2+(aq) resulted in the preferential incorporation of U into goethite (a-FeOOH) over lepidocrocite (g-FeOOH), even though reaction conditions favored the formation of excess lepidocrocite. This unexpected result is supported by atomically resolved transmission electron microscopy. Using this model system, we demonstrate how AIMD-informed EXAFS analysis lifts the strict statistical limitations of traditional shell-by-shell EXAFS modeling, enabling the detailed analysis of the local bonding environment, charge compensation mechanisms, and oxidation states of polyvalent impurities in complex multi-phase nano-systems.

ab initio molecular dynamics↗

Startup Test Plan and Predictions for Highly Enriched Uranium to Low-Enriched Uranium Fuel Conversion at the University of Missouri Research Reactor

Nonpower reactors licensed by the U.S. Nuclear Regulatory Commission require a startup test plan as part of any facility modification to verify operability prior to resumption of operations. In order to support conversion of the University of Missouri Research Reactor from the use of highly enriched uranium to low-enriched uranium (LEU) fuel, a startup test plan has been devised to measure certain reactor physics parameters for the initial all-fresh LEU core licensing documentation that will be submitted. These parameters include the approach to critical, primary coolant void coefficient of reactivity, flux trap void coefficient of reactivity, determination of flux trap sample reactivity worth, radial and axial thermal neutron flux mapping, control blade worth calibration, primary and pool coolant temperature coefficient of reactivity, and flux mapping of experimental positions. Here, predictions for these parameters made using the Monte Carlo N-Particle Version 5 (MCNP5) radiation transport code are reported. These predictions will support the startup tests by providing a baseline set of expectations and additional insight into the performance of the LEU core.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗