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At least 91 records · Page 5

UZrCN Synthesis via Arc Melting - A Novel Synthesis Study

The next generation of nuclear reactors for both power production and space nuclear propulsion require fuel that is more durable, thermally stable, and more thermally conductive to support rapid heat transfer. High temperature gas reactors (HTGR), advanced gas reactors (AGR), and space-based nuclear thermal propulsion (NTP) are advanced reactor concepts that require a fuel type that can withstand high temperatures (1000-2900K) and flow of corrosive gas coolants such as helium, hydrogen, and carbon dioxide. One fuel with the potential to meet these demanding requirements is uranium-zirconium-carbonitride (UZrCN). UZrCN has many favorable fuel qualities compared to other eligible fuel forms such as uranium dioxide (UO2) and uranium mononitride (UN) that could support the aforementioned reactor concepts. UZrCN has an exceptionally high operating temperature and thermal conductivity which are highly desirable to improve reactor economics and safety. It far exceeds the properties of UO2 which is the most common fuel form in the United States. UZrCN also surpasses UN in terms of thermal conductivity and operating temperature by eliminating the dissociation problem UN has at 1700K. UZrCN could improve gas reactor performance and enable NTP technologies; however, it is an under-researched fuel that lacks rigorous scientific study. In recent efforts by the Idaho National Laboratory, a variety of novel methods to produce this fuel composition have been explored. One such method is via arc melting of uranium, zirconium, and carbon under a nitrogen atmosphere. Alloy fabrication using arc melting has been utilized for close to 150 years now and is well-understood as a method for rapid alloy prototyping. This process will be used to perform in-situ nitriding to form UZrCN.

36 MATERIALS SCIENCE↗

Alloys for inert matrix fuel compositions, and methods of making the same

In one embodiment, an alloy includes: Zr; Fe; Cu; Ta in an amount from about 1 wt % to about 3 wt %; and one or more optional constituents selected from: Ti, Be, and Nb; and wherein the alloy comprises a ductile phase and a nanoprecipitate hard phase. According to another embodiment, a method of forming an inert matrix nuclear fuel includes: packing a hollow structure with fuel pellets and alloy precursor pellets; heating the fuel pellets and the alloy precursor pellets to at least a melting temperature of an alloy to be formed by melting the alloy precursor pellets; and solidifying the alloy into a matrix surrounding the fuel pellets. The alloy precursor pellets independently comprise: Zr; Fe; Cu; Ta present in an amount from about 1 to about 3 wt %; and one or more optional alloy constituents selected from: Ti, Be, and Nb.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Production and Chemical Analysis of NaCl-KCl-UCl 3 Salts

Thermochemical and thermophysical properties of several molten salt systems of interest to molten salt reactor (MSR) developers are being measured at Argonne National Laboratory. These properties are needed by developers to design, license, and operate their reactors. Thermochemical properties being measured at Argonne include thermal transitions, phase behavior, and heat capacity. Thermophysical properties being measured at Argonne include liquid density, surface tension, volumetric thermal expansion of the liquid phase, thermal diffusivity, thermal conductivity, and viscosity. Properties of the ternary NaCl-KCl-UCl 3 system that may be used as a fuel bearing salt are being measured. Low-melting eutectic salt compositions are of interest to developers owing to the thermal efficiency. Using salts with low melting temperatures allow reactors to be operated at a lower temperature to improve operation and decrease safety concerns. Confirming low melting behaviors are maintained during composition changes that occur during fission is also an important factor. It is essential to any molten salt reactor developer utilizing a fuel bearing salt to have a complete understanding of the behavior of that fuel salt at a variety of compositions near the eutectic composition they plan to use. This kind of stability is indicated on a phase diagram by low liquidus slopes at compositions bordering the eutectic. Therefore, a thermodynamic model was constructed to determine what compositions of the ternary NaCl, KCl, and UCl 3 system should be studied to support MSR developers.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Management of the Three Mile Island Unit 2 Accident Corium and Severely Damaged Fuel Debris (Rev. 2)

The Three Mile Island, Unit Two (TMI-2) pressurized water reactor core underwent a significant meltdown in 1979 due to an untimely combination of maintenance problems that led to a loss of feedwater, followed by a series of operational misunderstandings and errors. Primary coolant discharging through a malfunctioning valve represented what was analyzed as a “small-break” loss-of-coolant accident (LOCA) and ultimately became a full core meltdown. The melted core recovery process required the development of a wide array of tools. After approximately three years of water management and other cleanup actions, the first views of the core revealed a much higher degree of damage than previously expected. Approximately 62 metric tons of the core had melted, leaving only 42 of the 177 fuel assemblies standing with fuel rods intact. The core to be recovered was composed of loose, gravel-like and granular particulate material and a central solidified mass of formerly molten fuel. Molten fuel had also penetrated some of the pressure vessel internals and resolidified below the main core support structure. Robotic tools that had been designed for the task were of limited effectiveness due to the range of material types and phases.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Management of the Three Mile Island Unit 2 Accident Corium and Severely Damaged Fuel Debris (Rev. 2)

The Three Mile Island, Unit Two (TMI-2) pressurized water reactor core underwent a significant meltdown in 1979 due to an untimely combination of maintenance problems that led to a loss of feedwater, followed by a series of operational misunderstandings and errors. Primary coolant discharging through a malfunctioning valve represented what was analyzed as a “small-break” loss-of-coolant accident (LOCA) and ultimately became a full core meltdown. The melted core recovery process required the development of a wide array of tools. After approximately three years of water management and other cleanup actions, the first views of the core revealed a much higher degree of damage than previously expected. Approximately 62 metric tons of the core had melted, leaving only 42 of the 177 fuel assemblies standing with fuel rods intact. The core to be recovered was composed of loose, gravel-like and granular particulate material and a central solidified mass of formerly molten fuel. Molten fuel had also penetrated some of the pressure vessel internals and resolidified below the main core support structure. Robotic tools that had been designed for the task were of limited effectiveness due to the range of material types and phases.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Prediction of Ablation Rates from Solid Surfaces Exposed to High Temperature Gas Flow

A mathematical model and a solution algorithm is developed to study the physics of high temperature heat transfer and material ablation and identify the problems associated with the flow of hydrogen gas at very high temperatures and velocities through pipes and various components of Nuclear Thermal Rocket (NTR) motors. Ablation and melting can be experienced when the inner solid surface of the cooling channels and the diverging-converging nozzle of a Nuclear Thermal Rocket (NTR) motor is exposed to hydrogen gas flow at temperatures around 2500 degrees Kelvin and pressures around 3.4 MPa. In the experiments conducted on typical NTR motors developed in 1960s, degradation of the cooling channel material (cracking in the nuclear fuel element cladding) and in some instances melting of the core was observed. This paper presents the results of a preliminary study based on two types of physics based mathematical models that were developed to simulate the thermal-hydrodynamic conditions that lead to ablation of the solid surface of a stainless steel pipe exposed to high temperature hydrogen gas near sonic velocities. One of the proposed models is one-dimensional and assumes the gas flow to be unsteady, compressible and viscous. An in-house computer code was developed to solve the conservations equations of this model using a second-order accurate finite-difference technique. The second model assumes the flow to be three-dimensional, unsteady, compressible and viscous. A commercial CFD code (Fluent) was used to solve the later model equations. Both models assume the thermodynamic and transport properties of the hydrogen gas to be temperature dependent. In the solution algorithm developed for this study, the unsteady temperature of the pipe is determined from the heat equation for the solid. The solid-gas interface temperature is determined from an energy balance at the interface which includes heat transfer from or to the interface by conduction, convection, radiation, and ablation. Two different ablation models are proposed to determine the heat loss from the solid surface due to the ablation of the solid material. Both of them are physics based. Various numerical simulations were carried out using both models to predict the temperature distribution in the solid and in the gas flow, and then predict the ablation rates at a typical NTR motor hydrogen gas temperature and pressure. Solid mass loss rate per foot of a pipe was also calculated from these predictions. The results are presented for fully developed turbulent flow conditions in a sample SS pipe with a 6 inch diameter.

Akyuzlu, Kazim M.↗

A critical review of the history of fabricating monolithic U-Mo fuel plates

The fabrication of monolithic uranium-molybdenum alloy fuels, specifically those developed for high-performance research and test reactors, began in the early 2000s. The primary fuel form consists of uranium alloyed with 10-wt% molybdenum in a thin foil coated with zirconium and encapsulated in aluminum-6061 cladding. Over the years, the process has evolved with different types of casting, heat treatments, rolling schedules, and cladding applications. This review examines the history of these fabrication processes and their impact on microstructure and fuel-swelling performance. Even though various fabrication methods were used, we found little correlation between fabrication variation and fuel swelling. This insensitive relationship between fabrication variation and fuel swelling is primarily due to inhomogeneous microstructures that formed during casting and grain refinement that occurred during rolling. We conclude that the fabrication processes we examined produced similar microstructures, indicating that the fuel microstructure is somewhat insensitive to the fabrication parameters evaluated. However, the relatively small amount of historic data, such as those for grain sizes, limited this analysis. More recently fabricated materials, such as those from ongoing irradiation experiment, Mini-Plate-1 and Mini-Plate-2, were also excluded from this analysis and are intended to be reviewed separately. The findings, that fuel microstructure is somewhat insensitive to the fabrication parameters, do not imply that any fabrication method is acceptable, given the uncertainties in data and fuel-swelling observations. For example, only arc melting and vacuum induction melting casting processes were previously explored in the historic fabrication efforts. In conclusion, the findings should not be extrapolated to other casting processes.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Hot Hydrogen Exposure of U x Zr 1-x C y Nuclear Fuel: The Influence of Composition and Density

Refractory carbide nuclear fuel has been one of the most promising fuel candidates for space nuclear propulsion due to its high melting point, temperature stability, and compatibility in a hot hydrogen environment. In this study, U x Zr 1-x C y fuel was produced by means of a carbothermic reduction process in different UC compositions including 5,10, 20, and 30 at.% UC in the fuel compound. The powder feedstock was consolidated via direct current sintering with densities up to 97% of the theoretical density. The samples with different U x Zr 1-x C y compositions were exposed to hot hydrogen at 2600 K for a cumulative time of 300 min. The samples were characterized by SEM, XRD, density, and measured for mass losses. The high-density samples displayed improved performance in hot hydrogen by minimizing porous sites and reducing areas of direct contact with hydrogen gas, leading to reduced mass losses. Variations in sample density proved to induce large changes in mass loss rates, increasing them up to 90%. The compositions with higher UC content reported the largest mass losses in the study. The loss of uranium occurred primarily at the surfaces exposed to the hot hydrogen where changes in the lattice constant confirmed losses exceeding 50% of the initial UC content in higher compositions, specifically to U 0.3 Zr 0.7 C y . XRD analyses revealed the presence of UH 3 in U 0.3 Zr 0.7 C y suggesting that metallic uranium formed inside the sample as a product of carbon losses. High-density U x Zr x-1 C y fuel with UC concentrations at or below 20 at.% UC exhibited stability and negligible density changes in a high temperature hydrogen environment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Material Interactions in Severe Accidents – Benchmarking the MELCOR V2.2 Eutectics Model for a BWR-3 MARK-I Station Blackout: Part I – Single Case Analysis

Here in this analysis, the two material interaction models available in the MELCOR code are benchmarked for a severe accident at a BWR under representative Fukushima Daiichi boundary conditions. This part of the benchmark investigates the impact of each material interaction model on accident progression through a detailed single case analysis. It is found that the eutectics model simulation exhibits more rapid accident progression for the duration of the accident. The slower accident progression exhibited by the interactive materials model simulation, however, allows for a greater degree of core material oxidation and hydrogen generation to occur, as well as elevated core temperatures during the ex-vessel accident phase. The eutectics model simulation exhibits more significant degradation of core components during the late in-vessel accident phase – more debris forms and relocates to the lower plenum before lower head failure. The larger debris bed observed in the eutectics model simulation also reaches higher temperatures, presenting a more significant thermal challenge to the lower head until its failure. At the end of the simulated accident scenario, however, core damage is comparable between both simulations due to significant core degradation that occurs during the ex-vessel phase in the interactive materials model simulation. A key difference between the two models’ performance is the maximum temperatures that can be reached in the core and therefore the maximum ΔT between any two components. When implementing the interactive materials model, users have the option to modify the liquefaction temperature of the ZrO 2 -interactive and UO 2 -interactive materials as a way to mimic early fuel rod failure due to material interactions. Through modification of the liquefaction of high melting point materials with significant mass, users may inadvertently limit maximum core temperatures for fuel, cladding, and debris components.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

High-temperature thermal imaging to inform the arc-melt synthesis of nuclear materials

The advancement of nuclear energy technology necessitates the development of novel materials and synthesis methods to produce materials which enable new fuel cycles. Alongside the maturation of R&D scale technologies to produce these materials, there is an ongoing effort to develop in situ monitoring capabilities to reduce the time to the discovery and development of these fuels. Monitoring data can be leveraged in artificial intelligence platforms to detect phenomena which lead to varied macro- and microstructural features which impact the application and performance of samples synthesized. The present study presents early-stage findings of the implementation of high-temperature, high-frame-rate infrared thermal imaging to monitor the arc-melt synthesis of novel fuels and compounds relevant to advanced nuclear reactors. The study illustrates both the challenges and opportunities of this methodology, highlighting the importance of internal standards while determining emissivity and transmission values as well as visualizing volatilization during melt synthesis.

Stone, Jordan↗

Ab Initio Evaluation of Plutonium Dioxide $S(α,β)$ and Thermal Neutron Cross Sections

Plutonium Dioxide (PuO 2 ) is an advanced fuel-cycle nuclear fuel material for thermal and fast reactors, with a melting point at 3261.8 K and thermal conductivity above 3 Wm -1 K -1 for temperatures below 1500 K. Plutonium from spent UO 2 is reprocessed to form chemically stable mixed oxide (MOX) fuel. In contrast to metallic fuels, the low PuO 2 conductivity results in high thermal gradients between fuel center and surface, resulting in structural annealing and efficient fission product migration over burnup. Crystal binding affects the doppler broadening of epithermal resonances for nuclear fuels and scattering behavior of thermal neutrons. Currently, there is no ENDF/B Thermal Scattering Law, i.e., $S(α,β)$, evaluation for PuO 2 , only free atom cross sections for Plutonium and Oxygen, respectively, which neglect lattice contributions to total cross section. Herein, ab initio lattice dynamics (AILD) techniques are employed to calculate the phonon density of states (DOS) using spin-orbit-coupling density functional theory (DFT) to predict the PuO2 paramagnetic ground-state structure. These results highlight the evaluation of $S(α,β)$ for Plutonium and Oxygen, respectively in PuO 2 and consequential generation of thermal neutron scattering cross sections for high fidelity criticality safety analysis and reactor calculations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Scoping studies for low-temperature melting ZnO–Bi 2 O 3 –(B 2 O 3 , SiO 2 ) binder glass

In this work, low melting point glass systems were explored as candidates for binders of solid oxide nuclear wastes which include volatile elements such as radioactive iodine. The base glass systems considered were ZnO-Bi 2 O 3 -B 2 O 3 and ZnO-Bi 2 O 3 -SiO 2 , with specific compositions selected for synthesis trials based on available phase diagrams and a desire to explore the whole glass-forming region. Ten compositions were synthesized by melt quenching. Promising candidate glass binders were selected based on absence of crystallization and favorable thermal properties, including low glass transition temperature (T g ) combined with a high crystallization onset temperature. These thermal properties indicate stable glass forming which would lead to sintering behavior needed for glass binding. Compositional effects include: higher Bi 2 O 3 content lead to lower Tg values, high ZnO content generally led to crystallization on quench, and high SiO 2 content resulted in requirements for excessively high melting temperature. 25ZnO-15Bi 2 O 3 -60B 2 O 3 was down-selected for some detailed crystallization versus time and temperature studies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Modeling Internal Material Melting

The purpose of the SEED LDRD was to create new functionality to model internal material melting and solidification inside the state-of-the-art nuclear fuel performance simulation code BISON.

97 MATHEMATICS AND COMPUTING↗

Safely probing the chemistry of Chernobyl nuclear fuel using micro-focus X-ray analysis

Detailed chemical analysis of the solidified molten fuel still residing in the stricken Chernobyl reactor unit 4 are inferred using multi-modal micro-focus X-ray analysis of a low-radioactivity proxy. A fascinating mixture of molten UO 2 , nuclear fuel cladding, concrete, stainless steel and other nuclear reactor components, these materials behaved like lava, solidifying to form a complex, highly radioactive glass-ceramic. Using element-specific chemical probes (micro-X-ray fluorescence and X-ray absorption spectroscopy), coupled with micro-diffraction analysis, the crystalline phase assemblage of simulants of these heterogeneous materials was established, which included “chernobylite” and a range of compositions in the (U 1-x Zr x )O 2 solid solution. Novel insight to nuclear accident fuel chemistry was obtained by establishing the oxidation state and local coordination of uranium not only in these crystalline phases, but uniquely in the amorphous fraction of the material, which varied depending on the history of the nuclear lava as it flowed through the reactor. This study demonstrates that micro-focus X-ray analysis of very small fractions of material can yield rich chemical information, which can be applied to nuclear-melt down materials to aid decommissioning and nuclear fuel management at nuclear accident sites.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

SOLID SOLUTION CARBIDES ARE THE KEY FUELS FOR FUTURE NUCLEAR THERMAL PROPULSION

Nuclear thermal propulsion uses nuclear energy to directly heat a propellant (such as liquid hydrogen) to generate thrust for space transportation. In the 1960 s, the early Rover/Nuclear Engine for Rocket Propulsion Application (NERVA) program showed very encouraging test results for space nuclear propulsion but, in recent years, fuel research has been dismal. With NASA s renewed interest in long-term space exploration, fuel researchers are now revisiting the RoverMERVA findings, which indicated several problems with such fuels (such as erosion, chemical reaction of the fuel with propellant, fuel cracking, and cladding issues) that must be addressed. It is also well known that the higher the temperature reached by a propellant, the larger the thrust generated from the same weight of propellant. Better use of fuel and propellant requires development of fuels capable of reaching very high temperatures. Carbides have the highest melting points of any known material. Efforts are underway to develop carbide mixtures and solid solutions that contain uranium carbide, in order to achieve very high fuel temperatures. Binary solid solution carbides (U, Zr)C have proven to be very effective in this regard. Ternary carbides such as (U, Zr, X) carbides (where X represents Nb, Ta, W, and Hf) also hold great promise as fuel material, since the carbide mixtures in solid solution generate a very hard and tough compact material. This paper highlights past experience with early fuel materials and bi-carbides, technical problems associated with consolidation of the ingredients, and current techniques being developed to consolidate ternary carbides as fuel materials.

Panda, Binayak↗

Melt Crystallization of CsF from Alkali Fluorides

Fractional melt-crystallization is a technique used to separate components in a multicomponent liquid mixture through controlled cooling. In fiscal year (FY) 2023, this technique was successfully used to separate CsCl from LiCl-KCl. This demonstrated a potential route for concentrating electrorefiner fission product waste streams in pyrochemical fuel cycles, building on previous work that developed the melt-crystallization system for fission product removal from LiCl-based electrolytes used for oxide reduction. This work investigated whether a thermally controlled process of a solid-liquid separation process could effectively remove CsF from LiF-NaF-KF (FLiNaK)-CsF salt for MSR fuel cycle applications. The designed process aimed to recover purified LiF-NaF-KF salt as solid precipitates while concentrating CsF to a remaining salt heel. This concentrated CsF can then be immobilized during a salt waste stream treatment operation, minimizing waste volume.

36 MATERIALS SCIENCE↗

Metabolic engineering of β-oxidation to leverage thioesterases for production of 2-heptanone, 2-nonanone and 2-undecanone

Medium-chain length methyl ketones are potential blending fuels due to their cetane numbers and low melting temperatures. Biomanufacturing offers the potential to produce these molecules from renewable resources such as lignocellulosic biomass. Here, we designed and tested metabolic pathways in Escherichia coli to specifically produce 2-heptanone, 2-nonanone and 2-undecanone. We achieved substantial production of each ketone by introducing chain-length specific acyl-ACP thioesterases, blocking the β-oxidation cycle at an advantageous reaction, and introducing active β-ketoacyl-CoA thioesterases. Using a bioprospecting approach, we identified fifteen homologs of E. coli β-ketoacyl-CoA thioesterase (FadM) and evaluated the in vivo activity of each against various chain length substrates. The FadM variant from Providencia sneebia produced the most 2-heptanone, 2-nonanone, and 2-undecanone, suggesting it has the highest activity on the corresponding β-ketoacyl-CoA substrates. We further tested enzyme variants, including acyl-CoA oxidases, thiolases, and bi-functional 3-hydroxyacyl-CoA dehydratases to maximize conversion of fatty acids to β-keto acyl-CoAs for 2-heptanone, 2-nonanone, and 2-undecanone production. In order to address the issue of product loss during fermentation, we applied a 20% (v/v) dodecane layer in the bioreactor and built an external water cooling condenser connecting to the bioreactor heat-transferring condenser coupling to the condenser. Finally, using these modifications, we were able to generate up to 4.4 g/L total medium-chain length methyl ketones.

2-Heptanone↗

Data for Metabolic Engineering of β-Oxidation to Leverage Thioesterases for Production of 2-Heptanone, 2-Nonanone, and 2-Undecanone

Medium-chain length methyl ketones are potential blending fuels due to their cetane numbers and low melting temperatures. Biomanufacturing offers the potential to produce these molecules from renewable resources such as lignocellulosic biomass. In this work, we designed and tested metabolic pathways in Escherichia coli to specifically produce 2-heptanone, 2-nonanone and 2-undecanone. We achieved substantial production of each ketone by introducing chain-length specific acyl-ACP thioesterases, blocking the β-oxidation cycle at an advantageous reaction, and introducing active β-ketoacyl-CoA thioesterases. Using a bioprospecting approach, we identified 15 homologs of E. coli β-ketoacyl-CoA thioesterase (FadM) and evaluated the in vivo activity of each against various chain length substrates. The FadM variant from Providencia sneebia produced the most 2-heptanone, 2-nonanone, and 2-undecanone, suggesting it has the highest activity on the corresponding β-ketoacyl-CoA substrates. We tested enzyme variants, including acyl-CoA oxidases, thiolases, and bi-functional 3-hydroxyacyl-CoA dehydratases to maximize conversion of fatty acids to β-keto acyl-CoAs for 2-heptanone, 2-nonanone, and 2-undecanone production. In order to address the issue of product loss during fermentation, we applied a 20% (v/v) dodecane layer in the bioreactor and built an external water cooling condenser connecting to the bioreactor heat-transferring condenser coupling to the condenser. Using these modifications, we were able to generate up to 4.4 g/L total medium-chain length methyl ketones.

Metabolic Engineering↗