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At least 73 records · Page 4

Assembly of MiniFuel Targets for Irradiation of U-Mo Fuel Specimens in the High Flux Isotope Reactor

To support the development of advanced low-enriched uranium for use in nuclear reactors, irradiation testing of U-Mo disk specimens was performed at the Oak Ridge National Laboratory (ORNL) High Flux Isotope Reactor (HFIR) to collect experimental irradiation data on this type of fuel at pressurized water reactor–relevant temperatures. U-Mo is a uranium alloy that has superior dimensional stability relative to alpha-phase uranium metal and has a substantially higher uranium density compared to UO 2 . U-Mo disks specimens were fabricated at Idaho National Laboratory and inserted into MiniFuel targets for HFIR irradiation. Three MiniFuel targets were successfully assembled, welded, tested, and delivered to HFIR, along with their quality assurance documentation. The targets were inserted into HFIR’s inner vertical experiment facility within the permanent beryllium reflector. Each target contains six disk specimens and will be irradiated in HFIR for three, four, and eight cycles, with target temperatures between 250 and 500°C. This report summarizes the experiment design, test matrix, pre-characterization of specimens, and experiment assembly.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Status of the n+ 234 U evaluation in the resolved resonance region (*), (**)

In natural uranium, the 234 U isotope represents only 0.0055%, however, this minor isotope can affect highly enriched uranium metal benchmark calculations. In fact, enriched uranium contains more 234 U than natural uranium as the result of the uranium enrichment process. Therefore, the n+ 234 U nuclear data evaluation is one of the milestones of the APPENDIX B within the Nuclear Criticality Safety Program (NCSP).

AMPX↗

Intentional Uranium Tagging for Material Provenance and Pathway Forensics (LA19-Intentional-Forensics-NDD3Bb): Final Project Report

This report summarizes the outcomes of a 3-year NA-22 exploratory project to research the feasibility of tagging uranium materials, especially nuclear fuels, for nuclear nonproliferation purposes. The experimental focus was on metallic uranium forms under prospective surface and bulk tagging manufacturing and detection scenarios. This study showed that a large number of tags (drawn from an even larger menu of options) could be successfully imparted and detected in both as-built and degraded conditions. These results pave the way for additional R&D studies of surface and bulk tagging of metallic forms of uranium.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

An Ab Initio Molecular Dynamics Study of Key Thermodynamic Input Parameters for Computer Simulation of U-6Nb Solidification

The key to metallic fuel development is the fabrication of uranium metal and alloys into fuel forms. U-Nb alloys are one of the best candidates for a metallic fuel alloy with high-temperature strength sufficient to support the core, acceptable nuclear properties, good fabricability, and compatibility with usable coolant media. Melt processing has been a key component of the metallic fuel cycle, and process models require thermophysical parameters at elevated temperatures, particularly above the melting temperatures, regarding which experimental data are scarce, for accurate simulations and process development. By means of ab initio density-functional theory (DFT) quantum molecular dynamics (QMD), we have calculated the main thermophysical parameters—the density, thermal expansion coefficient, specific heat, thermal conductivity, melting temperature, latent heat of fusion, and viscosity—used in the modeling of the U-6 wt.% Nb alloy casting. The melting temperature of the U-6 wt.% Nb alloy at ambient pressure is obtained by means of QMD simulations using the Z-method. The ambient volume change and latent heat of melting of U-6 wt.% Nb are also derived from QMD simulations in conjunction with analytical fitting for the energy and pressure. The thermal conductivity for the solid U-Nb alloy is calculated from the semi-classical Boltzmann transport equation combined with an estimate of the electron relaxation time obtained from DFT simulations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Demonstration of Electroreduction Technology to Convert GNF Uranium Oxide Powder to Metal

Global Nuclear Fuel – Americas LLC (GNF) has partnered with Argonne National Laboratory to demonstrate electroreduction of uranium oxides produced by deconversion of UF 6 to uranium metal through the Gateway for Accelerated Innovation in Nuclear (GAIN) program under the U.S. Department of Energy to accelerate the domestic production of metallic advanced reactor fuels. Electroreduction of uranium oxide was first demonstrated and patented by Argonne in the early 2000s as a technology to convert used oxide nuclear fuel from light water reactors to metal for further fuel reprocessing. More recently, electroreduction has been proposed as a front-end technology for metallization of uranium oxides produced by deconversion of UF 6 and for scrap recovery of oxide materials. During the electroreduction process, UO 2 powder is contained in a stainless-steel mesh basket with a cathode lead located in the center of the UO 2 bed. The basket is immersed in lithium chloride molten salt electrolyte containing 1 wt% lithium oxide along with a platinum anode and a nickel/nickel oxide (Ni/NiO) reference electrode. Current is applied to the cell between the cathode and anode to reduce the UO 2 to metallic uranium via a solid-state reduction reaction. Oxide ions released from the UO 2 during reduction are transported through the salt to the anode where oxygen gas is evolved. Once reduction is complete, the basket containing the metallicized uranium is removed from the salt and can be processed to remove the salt and consolidate the uranium into an ingot for use in metallic fuel fabrication. This project was performed to provide evidence of the electroreduction technology readiness level for metallization of UO 2 powder, identify and retire technical risks for industrialization of electroreduction, and accelerate the path to commercialization for metallic fast reactor fuel production. To that end, five electroreduction tests were performed with UO 2 provided by GNF and the resulting product was analyzed for the extent of conversion to metal and for impurity contents of the metal product to verify that electroreduction does not introduce impurities that would prevent use of the product in metallic fuel fabrication.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A chromatography chemistry for purifying $\mathrm{Pa}$ from $\mathrm{U-Nb}$ metal alloys

Here we present a chromatography chemistry for purifying protactinium from uranium metal alloys containing weight-percent concentrations of niobium. Niobium is precipitated in 9 M HCl without the co-precipitation of Pa as demonstrated by gamma-ray spectrometry. Protactinium is further purified using Bio-Rad™ anion resin AG® 1-X8 and 9 M HCl + 0.0128 M HF. A Pa/Nb separation factor of 85,000 and a 90% Pa recovery is demonstrated, which is amenable to 231 Pa concentration determination by isotope dilution and 231 Pa/ 235 U model age calculation for nuclear forensics.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

A new HALEU isotopic certified reference material

Candidate certified reference material (CRM) U196 was prepared by gravimetrically mixing and dissolving NNSA NRMP CRM 112-A (natural uranium metal) and CRM 116-A (highly enriched 93.2% 235 U metal) to achieve a high-assay low-enriched uranium (HALEU) isotopic abundance reference material. CRM U196 will be certified for the 233 U/ 238 U, 234 U/ 238 U, 235 U/ 238 U, and 236 U/ 238 U ratios. Gravimetrically determined uranium isotope amount ratios and values derived from the isotope data were calculated from the buoyancy corrected mass data and from certified values for the metal CRMs used to create the solution. The 235 U isotope amount fraction (·100) and expanded uncertainty is 19.5846 ± 0.0028. For attribute verification, total evaporation and modified total evaporation isotope ratio measurements were performed. In conclusion, the reference material is to be distributed as a unit containing 5 mg uranium as dry uranyl nitrate.

High-assay low-enriched uranium↗

A short tutorial on uranium electropolishing

Electropolishing of uranium metal is best performed in a simple aqueous solution of phosphoric acid. With +3 to +10 volts of bias potential applied to the uranium (anode) relative to a Pt counter electrode (cathode). As summarized in a Pourbaix stability diagram, these conditions yield dissolution of the U surface as UOX containing solution species without the possibility of injecting hydrogen into the metal surface. However, if the uranium is biased to negative potentials relative to the counter electrode then water may be reduced at the U surface and hydrogen gas becomes available for reaction with the U metal. The stability diagram may be modified if there are other complexing species present in solution and the potential scale shifted if a different metal is use for the counter electrode. These effects can be understood in a known way as long as solution and electrochemical cell conditions are recognized.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Dry Deactivation of Sodium Metal in a Molten LiCl-KCl-CsCl-NaCl System

An experimental study was performed with the objective of investigating and characterizing a dry technique for deactivation of sodium metal in a molten salt system. The study was performed in three parts. First, proof-of-principle testing of the technique was performed at bench scale. It involved loading and melting tens of grams of clean sodium metal atop a pool of LiCl-KCl-CsCl eutectic at ∼300°C and then adding ammonium chloride particles while mixing. The ammonium chloride reacted with sodium to form sodium chloride and nitrogen/hydrogen off-gases. The sodium chloride assimilated into the salt pool, forming a quaternary salt mixture of LiCl-KCl-CsCl-NaCl. The proof-of-principle testing repeatedly exhibited complete deactivation of the loaded sodium metal. Second, characterization of a LiCl-KCl-CsCl-NaCl system was performed using differential scanning calorimetry to produce a partial phase diagram of LiCl-KCl-CsCl eutectic versus NaCl, which identified the liquidus, solidus, and two-phase regions of the quaternary system. Third, the dry deactivation technique was demonstrated at kg-scale in an inert atmosphere radiological glovebox with sodium metal that was previously separated in the same glovebox from uranium metal in unirradiated blanket elements for the Fermi-1 nuclear reactor. The quaternary salt product at the end of the demonstration was sampled and showed complete deactivation of the sodium metal. Here, in short, this study qualified a technique to completely deactivate batches of sodium metal in the absence of air or water. While this study focused on the deactivation of sodium metal, including bond sodium from unirradiated blanket elements, the technique is applicable to other sources of sodium metal, such as sodium metal from batteries. Furthermore, the technique could also be extended to other alkali metal systems, including lithium, sodium, potassium, rubidium, cesium, and mixtures thereof.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Removal and Deactivation of Bond Sodium from Fast Reactor Blanket Materials

The disposition of sodium-bonded spent nuclear fuel and blanket materials in a repository is complicated by the presence of sodium metal that is used as a thermal bond between the uranium metal fuel and blanket slugs and their cladding. The concern is that the metallic sodium could react with water, producing explosive hydrogen gas, or could exhibit a pyrophoric character. Thus, experimental studies were performed to investigate and demonstrate the removal and deactivation of bond sodium from blanket material in a dry environment. Specifically, bond sodium was removed from unirradiated Fermi-1 blanket elements and an assembly via a melt-drain-evaporate process using elevated temperature and reduced pressure. The effectiveness of sodium metal removal from the blanket materials and their associated cladding was =99.9998%, based on post-test quantitative analyses. The separated sodium metal was collected and subsequently deactivated by reacting it in a molten state with a controlled addition of ammonium chloride particles atop a molten salt medium. In this process sodium chloride is formed and assimilates into the salt pool. The subsequent deactivation of the bond sodium produced a solid ingot of sodium chloride, potassium chloride, lithium chloride, and cesium chloride that was devoid of sodium metal based on post-test analyses of the salt product. Both the sodium removal and deactivation operations were conducted within a dry inert atmosphere enclosure. The results of this study substantiate a path forward for the disposition of sodium-bonded blanket materials, including 34 metric tons heavy metal in irradiated Fermi-1 blanket material currently stored at Idaho National Laboratory.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Method to produce salts containing actinide halides

A method of producing uranium halides is disclosed in which chlorine gas is introduced into a liquid uranium-nickel alloy. NaCl salt is surrounding the crucible containing the liquid uranium-nickel alloy, producing a eutectic mixture of NaCl—UCl3. Upon chlorination, the metal halide dissolves in the matrix salt forming a solution. Adding the reactant metal, uranium to the nickel, the alloy is able to remain molten throughout processing. The liquid metal alloy may be removed from the salt bath, while the halogen gas continues to enter the system through the sparge until the desired composition of NaCl—UCl3—UCl4 is achieved. The method and system can be used to produce other metal halide salts such as actinide, lanthanide or transition metal halides contained in a matrix salt consisting of alkali and/or alkaline earth halides.

Williamson, Mark A.↗

CHALLENGES IN THE DEVELOPMENT OF THE ELECTROREFINING PROCESS AT Y-12

In order to ensure future capabilities of the Y-12 site as older buildings retire, a new process was developed, the Metal Purification Process. The purpose of this new process is to provide a simpler and more efficient uranium metal purification that the previous multi-staged, complex chemical processes. The basis for this technology currently exists in the US DOE complex, but it has not been utilized on a large scale for uranium at higher enrichments. The system requires larger-geometry vessels and furnaces in order to meet the through-put requirements. The crux of the process is the electrorefining cell, consisting of several concentric liners and an unfavorable geometry cylindrical crucible. Within the crucible, a molten Li-CL-KCL-UCL3 salt electrolyte is present. ‘Dirty’ metal is placed into a loading basket and loaded into an electrorefining cell. Here, the metal reacts into the molten salt within the cell to form UCL3, while ‘clean’ metal simultaneously plates out from the salt electrolyte in the form of metal dendrites. These dendrites are then collected and removed from the cell. After removal from the cell, the dendrites are taken to a furnace to remove adhered salts. Then, the salt-free dendrites are moved to a separate furnace for consolidation into the final product form. The development of the Criticality Safety Evaluation for this complex system brought with it many NCS Challenges and lessons learned. These challenges include: design decisions for ensuring subcriticalty in the electrorefining cell during abnormal conditions, the interface of the main glovebox system with auxiliary systems such as the purification system and designated storage, implementation of mass tracking, and concerns from production and operation regarding the movement of material within the system.

36 MATERIALS SCIENCE↗

Addendum to ICSBEP Logbooks 12r, 13r, 14r and 15r for Polyethylene and Graphite Reflected HEU Metal Critical Experiments

This report documents the experimenters’ data sheets that were recently (2023) discovered for critical experiments with highly enriched uranium metal with polyethylene and graphite reflectors. These data sheets were produced at the time of the measurements, when the dimensional inspection reports for the polyethylene and graphite were available. However, at this writing, those inspection reports are not available but may be in unmarked storage for the Y-12 National Security Complex. However, the data sheets presented herein contain sketches of the experimental configurations and other additional information that is not in the logbooks, such as dimensions and masses of the graphite measurements. This report reproduces the experimental data sheets that complement the logbooks. Some of the data on these sheets and the logbooks can be used to infer the dimensions and masses that are not documented. Some obvious mistakes in the logbook and data sheets have been corrected. In the reproduced data sheets, some of the information is not clearly visible: some information, such as average values, can be obtained from other data in the sheets or logbook. This report should be sent to the International Criticality Safety Benchmark Program at Idaho National Laboratory to complement the existing Oak Ridge Critical Facility logbooks there.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Uranium Dust Cloud Combustion: Burning Characteristics and Absorption Spectroscopy Measurements

This study characterized uranium metal dust cloud combustion using absorption spectroscopy, imaging, and broadband emission measurements. Other metals were similarly combusted to establish correlations between results from this study and those found in the literature. It was determined that the burn temperature of uranium was limited to the volatilization temperature of uranium dioxide. Combustion behavior was similar to that of other refractory metals in terms of burn time and the observation of exploding particle behavior.

42 ENGINEERING↗

Uranium droplet core nuclear rocket

Uranium droplet nuclear rocket is conceptually designed to utilize the broad temperature range ofthe liquid phase of metallic uranium in droplet configuration which maximizes the energy transfer area per unit fuel volume. In a baseline system dissociated hydrogen at 100 bar is heated to 6000 K, providing 2000 second of Isp. Fission fragments and intense radian field enhance the dissociation of molecular hydrogen beyond the equilibrium thermodynamic level. Uranium droplets in the core are confined and separated by an axisymmetric vortex flow generated by high velocity tangential injection of hydrogen in the mid-core regions. Droplet uranium flow to the core is controlled and adjusted by a twin flow nozzle injection system.

Anghaie, Samim↗

Electrorefiner Speciation and Phase Model for Prediction of Operation Lifetime

The Mk IV electrorefiner (ER) at Idaho National Laboratory has recovered uranium metal from used nuclear fuels for 27 years. Thus, large quantities of fission product chlorides more electropositive than uranium have accumulated in the ER salt, increasing the complexity of phase equilibria and salt speciation. Importantly, the melt temperature of the salt increases with ER operation and will ultimately exceed design limits without intervention. Methods to remove fission products from molten chloride salt are known, but their implementation at scale is not yet demonstrated. In this work, historical ER composition and differential scanning calorimetry (DSC) are utilized to develop coupled speciation and chloride salt solution thermochemistry models, which enable accurate present-day analysis of ER salt as well as forecast its future disposition. The developed thermochemical models are applicable to chloride salts generally and have been made available in the Molten Salt Thermal Properties Database – Thermochemical.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Verification of Subcritical Limits in ANSI/ANS-8.1-2014

The first edition of the current American National Standards Institute (ANSI)/American Nuclear Society (ANS) standard ANSI/ANS-8.1-2014, “Nuclear Criticality Safety in Operations with Fissionable Materials Outside Reactors,” was published in 1964 as ASA N6.1-1964, “Safety Standard for Operations with Fissionable Materials Outside Reactors.” In 1969, that standard was revised as ANSI N16.1-1969, “Nuclear Criticality Safety in Operations with Fissionable Materials Outside Reactors.” ANSI N16.1-1969 includes a variety of subcritical limits (SCLs) for uniform aqueous solutions and metals containing fissile nuclides of 233 U, 235 U, and 239 Pu. Furthermore, SCLs are also included for uranium-water lattices. In the 1983 version of ANSI/ANS-8.1 (a revision of ANSI N16.1-1975), the suite of SCLs in the standard was expanded to include 235 U enrichment limits for homogeneous uranium-water mixtures and dry/damp oxides, uniform aqueous solutions of low-enriched uranium, and uniform aqueous mixtures of Pu(NO 3 ) 4 containing 240Pu in addition to the SCLs included in ANSI N16.1-1969. The SCLs have changed little in subsequent revisions (ANSI/ANS-8.1-1998 and ANSI/ANS-8.1-2014). The ANSI/ANS-8.1-2014 standard is currently being revised to include new SCLs (uranium metal and compounds with enrichments up to 20 wt% 235 U) and possible updates to the current SCLs already in the standard, although these new/updated SCLs will not be available to the nuclear criticality safety (NCS) community for a number of years. The original bases for these SCLs were documented in papers in journals such as Nuclear Science and Engineering and in ANS meeting transactions; however, these bases are ambiguous enough that sites and regulators in the United States have not widely endorsed them for safety purposes. Overall, the purpose of this paper is to present the results of a comparison study for the SCLs in the ANSI/ANS-8.1-2014 standard using modern codes (SCALE and MCNP) and cross sections (ENDF/B-VIII.0) to provide some assurance about their quality (bias and bias uncertainty) for use in NCS applications and for consideration by the ANS-8.1 Working Group as a reference for future revisions.

42 ENGINEERING↗

Electrochemical Deposition with Redox Replacement of Lanthanum with Uranium in Molten LiCl-KCl

Electrochemical recovery of dilute concentrations of actinides from spent nuclear fuel would reduce the longevity of storing high-level nuclear waste. Electrochemical deposition with redox replacement (EDRR) is used in a molten salt medium for the selective electrochemical recovery of uranium in the presence of excess concentrations of lanthanum. In each EDRR cycle, after a short electrodeposition pulse, the deposited lanthanum is spontaneously replaced by uranium at open circuit. After repeated cycles, uranium metal was obtained on a tungsten electrode immersed in LiCl-KCl melt that contained 1 wt.% lanthanum chloride – 0.15 wt.% uranium 4+ chloride. Here, scanning electron microscopy and energy dispersive X-ray spectroscopy analysis revealed uranium particles approximately 0.5 - 1 μm with well-defined rectangular shapes; and with 20 – 60 times more uranium recovered on the surface of the electrode than lanthanum.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗