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Reveal of Uranium Bioremediation Mechanisms by Bacillus Species through Proteomics Studies

Radionuclides, such as Uranium (U) and heavy metals continue to pose threats to the ecosystem health and processes at the Department of Energy (DOE) managed, Savannah River Site (SRS), located along the Savannah River near Aiken, SC. Such co-contaminated environments are difficult to remediate using conventional excavation and disposal or pump-and-treat approaches. Globally, more than 109 tons of uranium contaminated areas pose a long term threat to human and ecological health. Even with presented low concentrations in the brain, central nervous effects are still observed. Uranium and depleted uranium (DU) have long term effects on the kidneys. Some small general health effects include severe headaches and breathing problems. Uranus ions are toxic to living cells because they inhibit metabolism of carbohydrates by blocking ATP binding sites. Bioremediation by microorganisms represents an alternative solution, which is advantageous because of the possibility of biosorbent regeneration, cost-effectiveness, increased metal removal and easy recovery of some valuable metals. Bacillus sp. bacterium was previously used in the bioremediation of heavy metals in coal mine run off waters of SRS. However, its ability to bioremediate uranium was unknown so far. Hence, in the present study, uranium bioremediation by Bacillus sp. bacterium was investigated. The mechanism of bioremediation was also revealed through proteomics studies. Heavy metals contamination poses a serious threat to water, soil and human health. Soil and water are contaminated due to excessive exploitation of uranium mines for generation of nuclear energy and weaponry. It is not degradable easily and persist in soil and water for a long period of time due to its long half- life. Savannah river site (SRS) is one of the uranium contaminated sites. The physical or chemical remediation techniques are costly and complex. Microbial system approaches with competent bacteria has received increased attention due to its adaptability in various environmental matrices and cost effectiveness. However, even though there are multiple suggested pathways (F1), the specific mechanisms that drive this behavior are still unclear, especially with popular microorganisms such as Bacillus species. In a previous research (Ibeanusi et al, 2003) Bacillus sp. was shown to detoxify and precipitate a variety of heavy metals in coal pile runoff waters of SRS site. Additionally, genomic analysis demonstrated that this microorganism posses multiple attributes for chemical transport regulation and metabolic pathways. U remediation occurs during the first 20 hours of exposure. During this time period, Bacillus sp. may work primarily under two mechanisms - sorption and accumulation. These two mechanisms simultaneously work to protect the microorganism from high concentrations. Figure 10 demonstrates that certain proteins are up regulated and down regulated under extreme stressful conditions. Membrane fraction proteins were up regulated. Cytosolic fraction proteins were down regulated. This protein information coincides with the adsorption behavior. Bacillus sp. is a good candidate for U remediation at various concentrations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Development of a Convolutional Neural Network Classifier for Data Starved Spectra - 20199

The Institute for Clean Energy Technology (ICET) at Mississippi State University is exploring the utility of machine learning in augmenting its mobile radiation surveying platforms, which are currently being developed as means to survey depleted uranium contaminated areas in support of remediation and decommissioning efforts. Mobile survey platforms provide a means to efficiently scan large areas of interest while reducing human exposure to radiation and other hazards. The survey platforms can also be used for scanning for any gamma emitting isotope in addition to depleted uranium. The spectral data that the platforms collect may be data starved with relatively low counts and poorly defined spectral features depending on the speed of the platforms and scintillation detector selection. Such data-starved spectra are difficult to use for isotope identification, requiring advanced knowledge of the possible radionuclides that could be present and environmental factors that could attenuate signals or introduce background noise. These factors in combination with the volume of survey data increases the time it takes to perform analysis of survey data when the source type is unknown. There are a number of algorithms in the field of machine learning that can be used to classify data that would be challenging and time-consuming for a human to identify. Supervised machine learning algorithms train models based on extensive amounts of human-labeled training data. Once sufficiently trained, these models can be used to quickly make high-fidelity predictions on new data. Convolutional neural networks are machine learning algorithms that excel in learning representations of 'shapes'. They do this by taking numerical input data and convolving them with spatial feature detectors referred to as filters. These filters are incrementally adjusted to reduce the prediction error on the data during the backpropagation step of training. Discussed in this paper is the development of a convolutional neural network classifier (CNNC) that can utilize spectral survey data for source discrimination and isotope identification. Bench-top laboratory experiments data using LaBr{sub 3}(Ce) scintillation detectors were used to train and evaluate the performance of the developed CNNC. The CNNC is capable of discriminating a variety of gamma emitting source types, differentiating different forms of uranium (depleted vs. natural), and estimating the amount of uranium for a known geometry. The discussed CNNC may be useful in scenarios where survey systems are deployed in situations where hazardous radioactive material maybe present, but the type is unknown. When used in remediation applications the CNNC can be used to screen-out false positives, helping reduce remediation costs. (authors)

07 ISOTOPE AND RADIATION SOURCES↗

Delayed Neutron Temporal Signatures for Uranium Enrichment Measurement NA-241 SGTech (Final Report)

Nondestructive determination of uranium enrichment is a core capability for nuclear material accounting and control (NMAC) and safeguards verification measurements; however, traditional gamma spectroscopy-based techniques for enrichment measurement rely on significant assumptions of material composition and geometry, precluding their use in scenarios where a heterogeneous spatial distribution of enrichments is encountered. As an alternative, we are developing a technique to use delayed neutron temporal signatures for the measurement of uranium enrichment. Each uranium isotope has unique delayed neutron group yields, resulting in a unique delayed neutron decay time profile which can be analyzed to determine enrichment without the need for calibration sources. As part of this effort, we performed a series of measurement campaigns in which we used an active well coincidence counter (AWCC) retrofitted with commercial D-D and D-T generators to evaluate the operational characteristics of this method in response to a set of uranium enrichment and mass standards, as well as representative diversion scenarios in which either “concealed” enriched uranium is shielded by depleted uranium or declared enriched uranium is “hollowed out” and replaced with a central region of depleted uranium. A standard operating procedure and best practices were compiled to facilitate the use of delayed neutron-based enrichment measurements for international safeguards inspections.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Enhancing isotope mixing in U-10Mo downblend castings with electromagnetic stirring

Uranium alloyed with 10 wt percent molybdenum (U-10Mo) is the proposed fuel for use in the United States’ high-performance research reactors. The U-10Mo fuel is fabricated by a two-step casting process that downblends highly enriched uranium with depleted uranium (DU) and/or natural uranium (NU) and subsequently alloys the resulting high-assay low-enriched uranium (HALEU) with Mo. Currently, a two-step casting process is needed to meet the ingots’ U-235 enrichment homogeneity specifications. This work demonstrates the ability to provide more homogeneous U-235 distributions during downblend casting by using zirconia for crucibles rather than graphite. When graphite is used as a crucible, the electromagnetic field produced by the induction heater couples directly with the graphite. Zirconia is nonconducting in this study, and therefore does not couple with the field. The induction field couples directly with the metal, and causes electromagnetic stirring (EMS) in the molten metal pool. Eight downblend casting experiments were carried out in this work. Four were performed with zirconia crucibles and four with graphite crucibles. The U-235 enrichment was measured at nine discrete points in each casting using laser ablation multi-collector inductively coupled mass spectrometry (LA-MC-ICP-MS). The enrichment homogeneity was approximately eight times better in zirconia crucible castings than in graphite crucible castings as measured by the plate enrichment range and enrichment coefficient of variation. The results show a single casting step could be used to meet USHPRR enrichment specifications if electromagnetic stirring is present during casting. A related investigation was carried out to determine whether it is appropriate to measure enrichment on as-cast ingots or whether heat treated specimens should be used to accurately characterize enrichment. The results show that the as-cast microstructure plays a significant role in enrichment homogeneity. It is recommended that all enrichment measurements be done after the homogenization heat treatment typical of U-10Mo processing.

36 MATERIALS SCIENCE↗

ZPPR-15 Small Reactivity Worth Experiments

In addition to measuring the worth of sodium voiding and the worth of simulated control rods, the ZPPR staff measured the Doppler worth of four standard samples, the worth of axial expansion and the worth of radial bowing in ZPPR-15. Doppler sample worths were measured in ZPPR-15A, ZPPR-15B and ZPPR-15D. The Doppler samples were natural UO 2 , depleted uranium metal, depleted U-10Zr alloy and 33% enriched UO 2 . These samples were placed in a sample capsule in the inner core of ZPPR-15 and heated to various temperatures between 300 K and 1100 K. The resulting changes in reactivity relative to the reference configuration were measured to determine the Doppler worths of the samples. Special segmented drawers were constructed to measure the worth of axial expansion in ZPPR15. The segments were connected to each other, and the back segment was connected to a spring-loaded cable. Pulling the cable introduced small gaps between drawer segments to simulate axial expansion, and releasing the cable eliminated those gaps. The worth of this simulated axial expansion was measured in ZPPR-15A, ZPPR-15B and ZPPR-15D. The worth of radial bowing was measured in ZPPR-15, but the experimenters regarded the result as unsatisfactory. Radial bowing was measured by two methods in ZPPR-17A, so the ZPPR-17A bowing measurements were analyzed in place of the unpublished ZPPR-15 radial bowing measurement. The first ZPPR-17A measurement consisted of rearranging the plates in 96 core drawers at the core-radial blanket boundary to simulate outward motion of the fuel during bowing. The second ZPPR-17A measurement used a new bowing oscillator to move the core plates a small distance vertically in a special drawer. The published uncertainties for the Doppler worth, axial expansion worth and radial bowing worth measurements are the statistical uncertainties in the measurements. In reality, the published uncertainty for each of these measurements is just one component of the total uncertainty. There are additional uncertainties specific to each measurement and a common uncertainty related to conversion from the natural measurement units, cents, to pcm for calculations. A full uncertainty analysis was performed for each measurement. The significant uncertainties were quantified, and a total uncertainty was determined for each measurement. The ZPPR-15 and ZPPR-17A experimental records were used to create detailed as-built Monte Carlo models of the Doppler worth, axial expansion and radial bowing measurement configurations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Removal of Bond Sodium from Full-Length Unirradiated Fermi-1 Blanket Elements and Assembly via Melt-Drain-Evaporate Process

Equipment was designed, fabricated, tested, and operated in an inert atmosphere radiological glovebox at Idaho National Laboratory to demonstrate the removal of bond sodium from full-length unirradiated Fermi-1 radial blanket elements and an entire radial blanket assembly using a Melt-Drain-Evaporate process. A series of three runs was performed with individual and multiple radial Fermi-1 blanket elements, and a fourth run was conducted with an entire Fermi-1 radial blanket assembly. After each run, the depleted uranium alloy slugs in every element slid out of its cladding, mechanically exhibiting the effectual absence of bond sodium. Quantitative and further qualitative analyses of the treated Fermi-1 material revealed the substantive, if not complete, absence of sodium metal in blanket element components. Indeed, entire columns of depleted uranium alloy slugs and associated cladding from select treated elements were separately contacted with water to react with residual sodium metal on the element surfaces, forming hydrogen gas. Samples of the resultant gas were analyzed to quantify the hydrogen concentration, which correlated to a residual sodium metal content for the treated element. Accordingly, no detectable sodium metal (<7 µg) was found on the surfaces of multiple depleted uranium alloy slugs after removal from its cladding. Detectable sodium metal, ranging from 14 to 30 µg, was found on the surfaces of one separated column of slugs and two separated full-length cladding segments. Each element originally contained ~25 g of bond sodium, resulting in quantitative sodium metal removal efficiencies of =99.9998%. The remaining separated uranium alloy slugs and cladding segments from the four runs were piece-wise immersed in alcohol while videorecording possible gas bubble formation as an additional qualitative analysis for residual sodium metal on treated surfaces, which identified the predominant absence of sodium reactivity on the balance of treated Fermi-1 blanket material. The results of this demonstration substantiate a path forward for treatment and disposal of 34 metric tons heavy metal of irradiated sodium-bonded Fermi-1 blanket material currently stored at Idaho National Laboratory.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

R-Value Measurements Performed on Uranium Targets Irradiated with Fission Spectrum Neutrons FY 2021 for F2019 Project

The separation and characterization of two irradiated uranium targets, a depleted uranium (DU) and a highly enriched uranium (HEU) target, was conducted in April of 2021. The two targets were assembled at Los Alamos National Laboratory (LANL) and irradiated using the critical assembly at the National Criticality Experiments Research Center (NCERC). Splits of the dissolved targets were received by Pacific Northwest National Laboratory (PNNL) after which the PNNL and LANL teams chemically separated the solutions using independent separation schemes and analyzed the separated fractions for short lived actinides and fission products. Chemical separations at PNNL were traced with stable or radioactive tracers to allow for the determination of chemical yields, analyzing using either inductively coupled plasma optical emission spectroscopy (ICP-OES), inductively coupled plasma mass spectrometry (ICP-MS) or gamma emission analysis (GEA) depending on the nature of the tracer. Several other analytical techniques were used by PNNL including kinetic phosphorescence analysis (KPA) and thermal ionization mass spectrometry (TIMS) depending on the analyte’s need. Comparisons were made between current and historical PNNL and LANL, as well as literature values. Overall, there was agreement between the two laboratories for the bulk of analytes, with some notable exceptions such as 111 Ag, and 141,143,144 Ce. Included in these comparisons were the short-lived actinides 237 U, 239 Np, the fission products 89 Sr, 91 Y, 95/97 Zr, 99 Mo, 111 Ag, 115/115 mCd, 136/137 Cs, 140 Ba, 141/143/144 Ce, 147 Nd, 153 Sm, 156 Eu, and 161 Tb, providing both total atoms as well as the R-values. The data presented in this report represents the sixth NCERC irradiation of HEU and DU (FY13, FY14, FY15, FY17, FY18, FY21), and their subsequent separation and analysis.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

R-Value Measurements Performed on Actinide Targets Irradiated using the GODIVA IV Critical Assembly in FY22

The separation and characterization of two irradiated uranium targets, a depleted uranium (DU) and a highly enriched uranium (HEU) target as well as a plutonium (Pu) target, was conducted in April of 2022. The three targets were assembled at Los Alamos National Laboratory (LANL) and irradiated using the GODIVA critical assembly at the National Criticality Experiments Research Center (NCERC). Splits of the dissolved targets were received by Pacific Northwest National Laboratory (PNNL) after which the PNNL and LANL teams chemically separated the solutions using independent separation schemes and analyzed the separated fractions for short lived actinides and fission products. Chemical separations were traced with stable or radioactive tracers to allow for the determination of chemical yields, analyzing using either inductively coupled plasma optical emission spectroscopy (ICP-OES), inductively coupled plasma mass spectrometry (ICP-MS) or gamma emission analysis (GEA) depending on the nature of the tracer. The Pu target solution was traced with stable elements at LANL to follow elemental fractionation during a Pu removal step. Many analytical techniques were used by PNNL including kinetic phosphorescence analysis (KPA), ICP-OES, ICP-MS, GEA, and thermal ionization mass spectrometry (TIMS) depending on the analyte’s need.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A novel protocol to recycle zirconium from zirconium alloy cladding from used nuclear fuel rods

A potential new zirconium recycling protocol has been demonstrated using unirradiated Zircaloy-based claddings and depleted uranium oxide for the chemical removal of zirconium alloy cladding in used nuclear fuel (UNF) rods from light water reactors. This protocol is based on the application of three new scientific findings. First, a new lower temperature chlorination reaction of zirconium with sulfur monochloride is described. Second, the high solubility of zirconium chloride in thionyl chloride is used to separate it from uranium oxide fuel and fission and activation contaminants. Finally, in the third step, the zirconium chloride is purified by simple recrystallization from thionyl chloride. Utilizing sulfur chloride solvents for a lower temperature liquid-based chemical digestion and purification of zirconium alloy claddings reduces technical complications experienced by current high temperature gas phase chlorination strategies, such as contamination of product streams. This novel protocol has been demonstrated on a 3–50 g scale of unirradiated zirconium alloy, with no significant change in the time required for complete chlorination (3–4 h). This zirconium chlorination protocol has also been performed in the presence of depleted uranium oxide pellets. The depleted fuel pellets do not affect zirconium chlorination, and the chlorination protocol does not chemically or physically alter the fuel pellets. Finally, a preliminary description of an industrial protocol to recycle nuclear grade zirconium from UNF rods is presented.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Panel Session 90: US DOE Mixed Waste: Proposals for Dealing with Problematic Waste Streams and Policy Changes

This panel focused on generation and management of low level and mixed low-level radioactive wastes, challenges for disposition, innovative solutions applied at DOE sites, and collaboration among sites to ensure that waste disposition pathways are understood. In addition, potential policy initiatives were discussed including depleted uranium, elemental mercury, and treatment of legacy mixed waste components. As part of the introduction, Theresa Kliczewski provided an overview of why this panel is relevant: problematic mixed waste streams still exist across the DOE cleanup complex. Theresa noted that the DOE EM Headquarters Office of Waste and Materials Management (EM-4.2), for which she is employed with, continues to work with the DOE cleanup sites on a path forward for these problematic mixed waste streams. As part of this effort, EM-4.2 requested that the Energy Facility Contractors Group (EFCOG) perform a review of all the DOE sites problematic mixed waste streams. Panelists with presentations: Challenging Waste Streams: Disposition of Depleted Uranium Oxide Conversion Product (Douglas Tonkay); EFCOG WMWG Challenging Waste Subgroup (Tammy Monday); Mercury Waste Challenges (John Wrapp); Legacy Large Mixed Waste Components (Kalli Shupe)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Raising Nuclear Thermal Propulsion (NTP) Technology Readiness Above 3

NTP development is currently supported by the NASA program office "Advanced Exploration Systems". The concept is a main propulsion option being considered for human missions to Mars in the 2030's. Major NTP development took place in the 1960's and 1970's under the Rover/NERVA program. The technology had matured to TRL 6 and was preparing to go to TRL 7 with a prototype flight engine before the program was cancelled. Over the last 40 years, a variety of continuations started, but only lasted a few years each. The Rover/NERVA infrastructure is almost all gone. The only remains are a few pieces of hardware, final reports and a few who worked the Rover/NERVA. Two types of nuclear fuel are being investigated to meet the current engine design specific impulse of 900 seconds compared to approximately 850 seconds demonstrated during Rover/NERVA. One is a continuation of composite fuel with new coatings to better control mid-band corrosion. The other type is a CERMET fuel made of Tungsten and UO2. Both fuels are being made from Rover/NERVA lessons learned, but with slightly different recipes to increase fuel endurance at higher operating temperatures. The technology readiness level (TRL) of these current modified reactor fuels is approximately TRL 3. To keep the development cost low and help mature the TRL level past 4 quickly, a few special non-nuclear test facilities have been made to test surrogate fuel, with depleted uranium, as coupons and full length elements. Both facilities utilize inductive heating and are licensed to handle depleted uranium. TRL 5 requires exposing the fuel to a nuclear environment and TRL 6 requires a prototype ground or flight engine system test. Currently, three different NTP ground test facility options are being investigated: exhaust scrubber, bore hole, and total exhaust containment. In parallel, a prototype flight demonstration test is also being studied. The first human mission to Mars in the 2030's is currently 2033. For an advanced propulsion concept to be seriously considered for use, the engine development plans need to show it is feasible and affordable to reach TRL 8 by 2027 and can be qualified for human mission use.

Gerrish, Harold P., Jr.↗

Uranium Solubility and Supernate Enrichment Testing for Accelerated Basin De-Inventory Discards to Concentration, Storage, and Transfer Facilities

After future Accelerated Basin De-inventory (ABD) enriched uranium discards into sludge batches (SB), portions of supernate decants during SB preparation will be blended into salt batches (StB) and the resulting feeds must meet the nuclear safety requirements for the Salt Waste Processing Facility (SWPF). During previous SB10 sampling and testing, which involved H-Canyon material containing enriched uranium being mixed with Tank 51 sludge shortly after the H-Canyon stream was neutralized, it was identified that the uranium isotopic enrichment in the supernate deviated from the uranium isotopic enrichment in the slurry. The higher uranium isotopic enrichment in the supernate introduced the risk of challenging the feed requirements of SWPF. The ABD material added to SB11 was isotopically diluted with depleted uranium, mitigating any downstream impacts. However, H-Canyon desires to eliminate or minimize future depleted uranium additions in order to meet the mission schedule.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Active Interrogation of the Snyder Shells using a SEA-7 Betatron

The shielded highly enriched uranium (HEU) problem is one that still needs to be addressed. As a first step towards a solution, the Snyder shells (depleted uranium) were actively interrogated with a SEA-7 betatron in various configurations using an MC15 as a detector. These configurations include masses from 0.55 to 5.1 kg, as well as 5.1 kg in a steel container. A strong electromagnetic field (EMF) background was identified in previous work, but the results in this work show all configurations produce a signal well above the background. An initial simulation capability was developed that produces the expected flux profile from the SEA-7 betatron, but further work needs to be done to determine the magnitude of the flux via a combination of experiment and simulation validation. Depleted uranium generally produces more neutrons than HEU, so additional future work will need to include similar measurements of HEU to confirm similar performance of the technique. Additionally the EMF background needs to be better characterized as a function of distance and angle from the SEA-7 source and mitigation techniques explored.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Gamma ray collimator

A gamma ray collimator including a housing having first and second sections is disclosed. The first section encloses a first section of depleted uranium which is disposed for receiving and supporting a radiation emitting component such as cobalt 60. The second section encloses a depleted uranium member which is provided with a conical cut out focusing portion disposed in communication with the radiation emitting element for focusing the emitted radiation to the target.

Casanova, Edgar J.↗

Gamma ray collimator

A gamma ray collimator including a housing having first and second sections. The first section encloses a first section of depleted uranium which is disposed for receiving and supporting a radiation emitting component such as cobalt 60. The second section encloses a depleted uranium member which is provided with a conical cut-out focusing portion disposed in communication with the radiation emitting element for focusing the emitted radiation to the target.

Casanova, Edgar J.↗

The Nuclear Cryogenic Propulsion Stage

Nuclear Thermal Propulsion (NTP) development efforts in the United States have demonstrated the technical viability and performance potential of NTP systems. For example, Project Rover (1955 - 1973) completed 22 high power rocket reactor tests. Peak performances included operating at an average hydrogen exhaust temperature of 2550 K and a peak fuel power density of 5200 MW/m3 (Pewee test), operating at a thrust of 930 kN (Phoebus-2A test), and operating for 62.7 minutes in a single burn (NRX-A6 test). Results from Project Rover indicated that an NTP system with a high thrust-to-weight ratio and a specific impulse greater than 900 s would be feasible. Excellent results were also obtained by the former Soviet Union. Although historical programs had promising results, many factors would affect the development of a 21st century nuclear thermal rocket (NTR). Test facilities built in the US during Project Rover no longer exist. However, advances in analytical techniques, the ability to utilize or adapt existing facilities and infrastructure, and the ability to develop a limited number of new test facilities may enable affordable development, qualification, and utilization of a Nuclear Cryogenic Propulsion Stage (NCPS). Bead-loaded graphite fuel was utilized throughout the Rover/NERVA program, and coated graphite composite fuel (tested in the Nuclear Furnace) and cermet fuel both show potential for even higher performance than that demonstrated in the Rover/NERVA engine tests.. NASA's NCPS project was initiated in October, 2011, with the goal of assessing the affordability and viability of an NCPS. FY 2014 activities are focused on fabrication and test (non-nuclear) of both coated graphite composite fuel elements and cermet fuel elements. Additional activities include developing a pre-conceptual design of the NCPS stage and evaluating affordable strategies for NCPS development, qualification, and utilization. NCPS stage designs are focused on supporting human Mars missions. The NCPS is being designed to readily integrate with the Space Launch System (SLS). A wide range of strategies for enabling affordable NCPS development, qualification, and utilization should be considered. These include multiple test and demonstration strategies (both ground and in-space), multiple potential test sites, and multiple engine designs. Two potential NCPS fuels are currently under consideration - coated graphite composite fuel and tungsten cermet fuel. During 2014 a representative, partial length (approximately 16") coated graphite composite fuel element with prototypic depleted uranium loading is being fabricated at Oak Ridge National Laboratory (ORNL). In addition, a representative, partial length (approximately 16") cermet fuel element with prototypic depleted uranium loading is being fabricated at Marshall Space Flight Center (MSFC). During the development process small samples (approximately 3" length) will be tested in the Compact Fuel Element Environmental Tester (CFEET) at high temperature (approximately 2800 K) in a hydrogen environment to help ensure that basic fuel design and manufacturing process are adequate and have been performed correctly. Once designs and processes have been developed, longer fuel element segments will be fabricated and tested in the Nuclear Thermal Rocket Element Environmental Simulator (NTREE) at high temperature (approximately 2800 K) and in flowing hydrogen.

Houts, Michael G.↗

U Metal Oxidation with Steam (U)

The Savannah Rive National Laboratory 9SRNL) is evaluating a method to produce uranium oxide (UO 2 ) from uranium metal using steam. The typical methods for making UO 2 yield powders with particle-size ranges of 1 to 50 micron. The goal of the steam oxidation is to produce a depleted uranium (DU) product with a larger particle size that can be used as a surrogate for testing physical and mechanical process techniques to refine uranium and/or plutonium bearing residues. Several studies in the literature indicated that reactions between uranium metal and steam will yield UO 2 as fine powders in the 160 to 500 °C range, but granular materials form above 500°C. Above 880 °C, a hard compact scale forms on the U metal. Furthermore, sintering of UO 2 occurs at about 1300 °C, but it has been stated that the presence of steam enhances the sintering characteristics of UO 2 . Initial studies into the oxidation of DU metal in an atmosphere of argon and steam have been completed. Oxidation of depleted uranium metal in Ar/steam at 600, 710, 700, and 830 °C yielded at UO 2 product with little or no impurity at each temperature. Although not enough sample was available to perform sieve analysis for particle size distribution, SEM images reveal that a significant volume fraction of the products at 710, 770, and 830 °C exceeds 100 microns. The material produced at 600 °C was too fine for programmatic needs. Questions associated with the UO 2 include morphology of product, mechanical strength of the particles, and performance in milling operations. The size of the samples produced in these tests did not allow for quantitative assessment of particle size of mechanical strength. A qualitative assessment of the particles formed at 710, 770, and 830 °C was that the samples produced at 710 and 770 °C were friable, and the sample produced 830 °C had more mechanical strength. Sintering of the samples in Ar/steam at 970 °C appeared to increase the strength of the particles without changing their general particle size characteristics. Due to the small sample sizes, the increase in strength could not be quantified. If the sintering at 970 °C is inadequate, higher sintering temperatures in Ar/steam can be evaluated. Future work will increase scale of the steam oxidation conditions which yield the most-favorable particle-size distributions with sufficient mechanical strength for programming usage. Further consideration will be given to oxidation temperature, steam addition to the reaction vessel, U metal pretreatment, and sintering conditions after oxidation. The UO 2 production could involve a two-step process where particles are formed in steam at lower temperatures (700-850 °C) and then sintered in Ar/steam at elevated temperatures (950-1200 °C). Larger samples (50-100 g each) will provide sufficient UO 2 product for sieve analysis and assessment of mechanical strength relatives to subsequent milling operations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hot Hydrogen Testing of Tungsten-Uranium Dioxide (W-UO2) CERMET Fuel Materials for Nuclear Thermal Propulsion

CERMET fuel materials are being developed at the NASA Marshall Space Flight Center for a Nuclear Cryogenic Propulsion Stage. Recent work has resulted in the development and demonstration of a Compact Fuel Element Environmental Test (CFEET) System that is capable of subjecting depleted uranium fuel material samples to hot hydrogen. A critical obstacle to the development of an NCPS engine is the high-cost and safety concerns associated with developmental testing in nuclear environments. The purpose of this testing capability is to enable low-cost screening of candidate materials, fabrication processes, and further validation of concepts. The CERMET samples consist of depleted uranium dioxide (UO2) fuel particles in a tungsten metal matrix, which has been demonstrated on previous programs to provide improved performance and retention of fission products1. Numerous past programs have utilized hot hydrogen furnace testing to develop and evaluate fuel materials. The testing provides a reasonable simulation of temperature and thermal stress effects in a flowing hydrogen environment. Though no information is gained about radiation damage, the furnace testing is extremely valuable for development and verification of fuel element materials and processes. The current work includes testing of subscale W-UO2 slugs to evaluate fuel loss and stability. The materials are then fabricated into samples with seven cooling channels to test a more representative section of a fuel element. Several iterations of testing are being performed to evaluate fuel mass loss impacts from density, microstructure, fuel particle size and shape, chemistry, claddings, particle coatings, and stabilizers. The fuel materials and forms being evaluated on this effort have all been demonstrated to control fuel migration and loss. The objective is to verify performance improvements of the various materials and process options prior to expensive full scale fabrication and testing. Post test analysis will include weight percent fuel loss, microscopy, dimensional tolerance, and fuel stability.

Hickman, Robert↗