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Multimetallic Layered Composites (MMLCs) for Rapid, Economical Advanced Reactor Deployment (Final Report)

This project focused on the development of multi-metallic layered composites (MMLCs) for advanced fission reactor technologies. There are many instances where one alloy or material simply cannot meet all the demands thrown at it by a reactor system, or cannot allow it to perform as strongly as one would like. Instead of focusing all our effort on developing one perfect alloy, we seek to leverage the design principle of “separation of functionality,” used in many other arenas in design, to boost performance beyond single alloys alone. One illustrative example shows the power of this approach for molten salt-cooled reactors: A three meter tall, three meter diameter reactor vessel made of Incoloy 800 was quoted at $\$$500k in 2018. A Hastelloy N vessel was quoted at $\$$5M. An MMLC vessel, in which a layer of Hastelloy N would be weld-overlaid onto Incoloy 800, was quoted at $\$$700k, and it would achieve the same performance. The potential economic gains of leveraging this approach are therefore substantial. At a minimum, each MMLC would contain one core structural layer and one coolant-facing corrosion-resistant layer. Sometimes, MMLCs required buffer layers, as the structural and corrosion-resistant layers were metallurgically incompatible. In other words, they didn’t always play nice, thus separating layers compatible with both functioned as intermediaries to keep the composite together. However, in doing so we inevitably produce new interfaces, where new issues can arise. Therefore, this project focused on what happens at these interfaces from a combination of high temperatures, irradiation, corrosion, and time. After all, a reactor makes money when it is operating, and outages of any kind erode its economic viability. First, we set out to experimentally prove that MMLCs for at least two advanced reactor systems can be made, today, in US domestic facilities. In this respect we were successful – one MMLC (a Ni-201/Incoloy 800H composite) was successfully made and drawn into two-inch coolant piping. Others were attempted, though new issues relating to cracking in vanadium layers for one and radiation damage performance of the corrosion-resistant layer in another prevented us from moving further in those specific arenas – these are engineering problems which deserve continued focus after this project. Additional experimental work focused on long-term corrosion testing of the outermost layers of the salt-cooled and liquid lead-cooled MMLC concepts, which would then be fed into predictions of how long the MMLCs could last. Next, computational (thermodynamics and atomistic) simulation studies studied how much we expect the interfaces to “blend,” due to the mixing action of neutron irradiation. This eats into both the margin for the structural layer of each MMLC, as dilution from the corrosion-resistant layer into the structural layer would decrease the total load-bearing capacity of an MMLC of finite size. On the other hand, dilution of the corrosion-resistant layer into the structural layer further reduced the margin of corrodible material, reducing the lifetime of the MMLC or necessitating extra thickness to be imparted to the MMLC to meet its functional requirements. Work here focused on irradiation-induced segregation to predict new phases which may embrittle the MMLCs, as well as quantifying irradiation-induced mixing at each interface. The results showed that mixing is expected, but it is both steady and therefore predictable, and not lifetime-limiting for most MMLC concepts – it simply has to be accounted for in calculations of reactor performance when utilizing an MMLC. Then, full-core simulations using the experimentally-derived corrosion data, the computationally discovered irradiation-induced mixing data (partially validated by experiment), and existing, benchmarked core designs for large and small sized reactor concepts (one salt-cooled, one lead-cooled) were conducted to quantify any expansion of reactor operating envelopes achieved by utilizing these MMLCs. This new framework, called REX (Reactor Envelope Expansion), incorporates a combination of core neutronics, thermal hydraulics, and the material performance data derived from this project to see how using an MMLC expands advanced fission reactor operating envelopes. It was discovered that in some cases, MMLC utilization does indeed increase the maximum operating temperatures and cycle lengths of reactor concepts, while in other cases it does not. Finally, our tech-to-market (T2M) strategy was not necessarily to create specific embodiments of MMLCs for immediate sale (because getting into the nuclear market is incredibly slow and laden with regulation, this is a long-term goal), but rather immediate stimulation of US industry using the design approach of MMLCs derived from this project. In this respect we were successful, as one of the PhD students funded on this project co-founded Allium Engineering, Inc., which created a stainless steel / low-alloy steel MMLC to function as chloride corrosion-resistant rebar for embedding into concrete structures. Allium Engineering continues to be successful, having recently opened their first factory as of this writing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Unraveling the Early-Stage Ordering of Krypton Solid Bubbles in Molybdenum: A Multimodal Study

Self-organization of defects such as fission gas bubbles in materials can lead to high inventory capacity for fission gas storage and help mitigate swelling caused by fission gases in nuclear fuel materials under radiation in nuclear reactors. Here, we report the physical mechanism of self-organization of krypton (Kr) gas bubbles in molybdenum (Mo) under ion implantation. The ion fluence and temperature-dependent formation of Kr solid bubble superlattice (SBS) in Mo were investigated by using both synchrotron-based small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM). Early stage self-organization of gas bubbles is observed at a fluence of 2.5 × 10 16 ions/cm 2 at temperatures of 300–400 °C. The bubble lattice constant increases with increasing implantation temperature from 300 to 400 °C. Both experiments and atomic kinetic Monte Carlo modeling indicate that the Kr solid bubbles are weakly ordered in comparison to previously studied helium (He) gas bubble superlattice (GBS) while the lattice constant are relatively smaller for Kr SBS compared to that of He GBS. The irradiation conditions suggest that spinodal decomposition, which is a form of phase separation, probably precedes gas bubble ordering in Mo. Altogether, our work sheds light on the formation mechanism of noble gas superlattice toward the development of radiation-tolerant materials which are important for the design of advanced nuclear reactors.

36 MATERIALS SCIENCE↗

Advanced Modeling and Simulation to Characterize Advanced Boiling Water Reactor Source Terms to Support a Regulatory Approval Pathway for Right-Sized Emergency Planning Zone. Advanced Boiling Water Reactor (A-BWR) Project Phase 2

The United States Department of Energy (US DOE) is currently supporting the development of various small modular reactor (SMR), microreactor and advanced reactor designs. These reactors have improved safety features as compared to conventional Large Light Water Reactors (LLWRs), which include features that improve potential reduction of radiological source terms in the event of design and beyond-design basis accidents. Specifically, some reactors feature a relatively smaller containment volume with respect to the available surface area for fission product deposition; these include Integrated Pressurized Water Reactors (iPWRs), such as the NuScale SMR and SMR-type Boiling Water Reactors (BWRs) such as General Electric-Hitachi’s BWRX-300 design.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

The porosity surrounding carbides and second phase stringers in monolithic U-10Mo fuel plate after irradiation

Post-irradiation microstructure characterization plays an important role in qualifying the low-enriched uranium (LEU) monolithic U-10 wt%Mo plate-type fuel for United States high-performance research reactors (USHPRRs) program. Inhomogeneous features resulting from manufacturing and irradiation processes, including carbides, second phase stringers, and extensive void spaces caused by the combining of small porosities, may increase the risk of heat concentration in local regions of the fuel plate over the operating conditions. In this study, characteristics of carbides, stringers, and porosity after multiple levels of irradiation at varying fission densities were studied by electron microscopes to decipher the morphology of pores and the porosity evolution in U-10 wt%Mo. For carbides, the result shows that porosities start forming on UMo grain boundaries, then on UMo/carbides interfaces as the burn-up going higher. However, the porosities surrounding carbides grow larger than the ones on UMo grain boundaries. The porosities around the uranium carbides could interconnect to form larger void space. The study revealed that the void spaces larger than 5 µm were found around uranium carbides after high burnup, while no evidence was observed to support the similar voids formed near second phase stringers even though the size of the stringers (> 50 µm) was much larger than uranium carbides (< 20 µm). The evolution of porosities suggests that the formation of second phase stringers may not create more significant porosities compared to regular uranium carbides regions during fuel operating conditions.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Investigation of neutron noise in a micro-scale, natural circulation molten salt fission battery system

The Molten Salt Reactor (MSR) concept is a rapidly evolving Generation IV design that has recently attracted favorable attention due to the potential for reducing waste generation, realizing passive safety features, and seizing on the opportunity for cost effective economics. A specific novel micro-MSR, natural circulation, battery design concept involves placing all primary components within a single reactor vessel containment without the need of primary forced pumping. This small modular, integral design presents potential cost savings while producing safety, reliable, and transportable carbon-free power for decades. This investigation evaluates the neutron noise induced by density and flow fluctuations in a natural circulation MSR battery concept being developed at the University of Idaho. This study finds numerical solutions to the one-dimensional, one-group, coupled diffusion equations for a bare, homogeneous core, and evaluates neutron flux and delayed neutron precursor concentration noise due to core flow and fuel salt density perturbation sources. Noise analysis shows both point kinetic and space-dependent behavior is present despite the small size, low-flow, closely-coupled nature of the natural circulation MSR concept. Analysis shows that the low flow of the convective system results in noise behavior typically representative of a larger forced-circulation MSR system. Finally, noise techniques may also be useful in MSR core diagnostics as a non-invasive, low-cost radiological option to traditional monitoring schemes.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Fluid structural interaction simulation of the MP-1 plate performance irradiated in the advanced test reactor

Due to the high neutron fluxes they generate and increased heat transfer performance, plate type fuels are used in the U.S. high-performance research reactors. During irradiation, a significant amount of fission energy (i.e., ~200 MeV per atom) is released by the U-235 chain reaction that is carried away by the coolant. Through thermal hydraulic analysis, the coolant’s heat transfer capability is investigated to ensure that the desired fuel temperature can be maintained. At high temperatures, the plate undergoes elastic/plastic deformation, creep, and swelling as a result of both the temperature gradients and the fission gas production within the fuel. These effects are studied via fuel performance analysis. When the plate deformation is small enough that the coolant flow remains relatively unchanged, conducting these two types of analyses independently will suffice. But at high fuel burnups, the swollen plates may encroach into the coolant channels that separate the fuel plates from each other and cause these channels to narrow. Large reductions in channel gap size imperil cooling performance, causing fuel temperatures to rise. Further, if the plate deformation is asymmetric, the fuel centerline will shift toward one side of the channel, causing an uneven reduction in coolability. In addition, a boehmite (oxide) layer will, over time, grow on the plate surface, further obstructing the heat transfer process. To precisely predict fuel temperatures/deformation, a complete coupled analysis that considers coolant flow, heat transfer, oxide growth, elastic/plastic deformation, creep, and swelling is needed; however, this type of analysis method is not available in the literature. To fill the gap, this research developed a fluid structure interaction (FSI) approach to the fuel plate analysis, then successfully applied it to the Mini-Plate (MP)-1 experiment, which was irradiated in the Advanced Test Reactor (ATR) for both one and two cycles. The complete analysis coupled STAR-CCM+, a computational fluid dynamic (CFD) software for calculating flow, with Abaqus, a finite element analysis code for calculating plate deformation. Improvements in the results were found when comparing the fully coupled analysis to the independently conducted analyses but they were not significant due to the miniature size of the plates and the relatively short irradiation time. In the future, the fully coupled approach presented herein will be applied to full-size fuel plates with longer irradiation cycles once additional experiments become available.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Benefits of using multiple Raman laser wavelengths for characterizing defects in a UO 2 matrix

Abstract Raman spectroscopy is one of the most useful techniques for studying the structure of UO 2 and changes due to specific defects caused by doping, changes in stoichiometry, irradiation, or heating under oxidizing conditions. In this paper, we illustrate several aspects of the application of Raman techniques to the study of UO 2 , including the use of wavelength‐dependent excitation (455, 532, and 785 nm) to assess the effects of doping (Nd, Th, and Zr), ion irradiation, and in situ heating and oxidation (UO 2 to U 3 O 8 ). Additionally, we show examples of how correlative microscopy is possible using electron backscatter diffraction combined with Raman maps of specific vibration bands or of laser‐induced luminescence generated by rare‐earth dopants in the matrix. For each of these applications, we suggest optimal excitation wavelengths that vary depending on the desired data. Blue (455 nm) excitation tends to promote oxidation even at low powers, but because Raman spectra change little with doping, irradiation‐induced changes are easier to observe. Green (532 nm) excitation is optimal for observing electron–phonon resonance effects in UO 2 and offers a good compromise for high‐temperature oxidation experiments, delivering high‐quality spectra for both UO 2 and U 3 O 8 . Infrared (785 nm) excitation is best for observing “defect” bands associated with doping in UO 2 , as changes with irradiation are small. Raman spectroscopy is particularly suited for studying the stability of UO 2 towards oxidation in the presence of dopants simulating fission products, where electron–phonon resonant effects, dopant ion luminescence, and mapping can be used together to investigate structural rearrangement as a function of temperature. These techniques can offer insight into microstructural changes in UO 2 fuels at higher burnups envisioned in future reactors.

42 ENGINEERING↗

Nuclear Safety [Vol. 32, No. 1, January-March 1991]

Nuclear Safety is a review journal that covers significant developments in the field of nuclear safety. Its scope includes the analysis and control of hazards associated with nuclear energy, operations involving fissionable materials, and the products of nuclear fission and their effects on the environment. Primary emphasis is on safety in reactor design, construction, and operation; however, the safety aspects of the entire fuel cycle, including fuel fabrication, spent-fuel processing, nuclear waste disposal, handling of radioisotopes, and environmental effects of these operations, are also treated. Table of Contents for this issue follows. GENERAL SAFETY CONSIDERATIONS: 1 The Safety Review and Approval Process for Space Nuclear Power Sources, G. L. Bennett; 19 Report on the American Nuclear Society International Topical Meeting: "The Safety, Status, and Future of Non-Commercial Reactors and Irradiation Facilities", E. G. Silver; 35 Book Review: Fission Product Transport Processes in Reactor Accidents, Proceedings to the International Centre tor Heat and Mass Processes T. S. Kress; 38 Fast Reactor Technology in the 1990s: A Summary of the 1990 International Fast Reactor Safety Meeting, A. E. Levin; ACCIDENT ANALYSIS: 56 Effects of Chemical Phenomena on LWR Severe Accident Fission Product Behavior, A. P. Malinauskas and T. S. Kress; CONTROL AND INSTRUMENTATION: 65 Technical Note: Safety Parameter Display Systems—10 Years Later, R. J. Eckenrode; 68 Potential Application of Neural Networks to the Operation of Nuclear Power Plants, R. E. Uhrig; DESIGN FEATURES: 80 Twenty-First DOE/NRC Nuclear Air-Cleaning Conference, R. R. Bellamy, D. W. Moeller, and M. W. First; 91 Impact of an Apparent Radiation Embrittlement Rate on the Life Expectancy of PWR Vessel Supports, R. D. Cheverton, G. C. Robinson, W. E. Pennell, and R. K. Nanstad; ENVIRONMENTAL EFFECTS: 103 Technical Note: The Impact of Offsite Factors on the Safety Performance of Small Nuclear Power Plants, Yu. D. Baranaev and A. N. Viktorov; WASTE AND SPENT FUEL MANAGEMENT: 109 Activities Related to Waste Management, Compiled by E. G. Silver; OPERATING EXPERIENCES: 118 Reactor Shutdown Experience, Compiled by J. W. Cletcher; 121 Selected Safety-Related Events, Compiled by G. A. Murphy; 123 Operating U.S. Power Reactors, Compiled by E. G. Silver; RECENT DEVELOPMENTS: 140 General Administrative Activities, Compiled by E. G. Silver; 150 Reports, Standards, and Safety Guides, D. S. Queener; 155 Status of Power-Reactor Licensing Activities, Compiled by E. G. Silver; 157 Proposed Rule Changes as of Sept. 30, 1990; ANNOUNCEMENTS: 79 MIT Offers Summer Program on Nuclear Power Reactor Safety; 108 Harvard School of Public Health Offers Several Short Courses; 139 Short Course and Workshop on Nuclear Criticality Safety at University of New Mexico; 160 SCK/CEN Announces Training Course on Emergency Planning and Response; 161 The Authors; 164 Indexes to Nuclear Safety, Volume 31

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Site specific porosity-thermal performance correlations in neutron irradiated U-10Zr fuel

In this work, we present a site-specific three-dimensional analysis of porosity evolution in neutron-irradiated U–10Zr metallic fuel using high-resolution synchrotron X-ray tomography. Focused ion beam cubic lift-outs from four radial positions—fuel center, middle, edge, and fuel-cladding interaction (FCCI) zones—were imaged, reconstructed, and segmented to quantify pore volume, density, morphology, and pore connectivity. Porosity increased modestly from 5.5% at the center to 10.5% at the edge, yet pore number density increased by over two orders of magnitude in the fuel portion near the FCCI interface (from 4.8 x 10 4 to 6.0 x 10 6 pores/mm 3 ). Morphological classification revealed a progression from small spherical pores at the center to equiaxed and tortuous networks at the periphery, with enhanced orientation along the radial direction. Connectivity and permeability analysis reveal that the FCCI region maintains dense, highly interconnected pores despite a moderate volume fraction, enabling rapid fission gas transport and lanthanide migration. Effective thermal conductivity models incorporating sodium logging confirm that these site-specific pore features critically influenced heat transport during reactor irradiation. These findings demonstrate that pore topology—not just porosity fraction—controls thermal performance and thermal pathways in U–10Zr fuels, impacting fuel thermal performance in a reactor.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Using X-ray spectrum imaging to quantify fission gas in high-burnup UO2 fuel

Analysis of fission gas bubbles (FGBs) in light-water reactor (LWR) fuel is needed to improve the understanding and predictive capability of fuel evolution under normal- and transient conditions. One of the most important parameters of a FGB is the pressure of the gas, primarily Xe, inside it. Bubble volume and location (inter- vs. intragranular) are important considerations as well. However, experimental analysis of such bubbles is challenging due to their small size and embedded nature, and usefulness of the data requires large numbers be analyzed. This paper proposes a method to measure the pressure of Xe bubbles using X-ray spectrum imaging (XSI) in scanning transmission electron microscopy (STEM). From X-ray generation and instrumental parameters, the number of Xe atoms yielding a given number of Xe L-series X-ray counts is estimated, and then from the estimated volume of the bubble the Xe density is estimated, which can then be converted to pressure via an equation-of-state. We apply the method to XSI datasets from high burnup (HBu) fuel from North Anna 1 reactor in as-irradiated and post-LOCA-test conditions and find Xe pressures in the FGBs clustered around 1 GPa.

Parish, Chad [ORNL] (ORCID:0000000312097439)↗

Scaled up Process Report – Apparatus and Model

Advanced voloxidation with NO 2 is a proposed process for used nuclear fuel head-end reprocessing scheme that converts UO 2 to higher oxides, and it also converts partitioning volatile fission products into the gas phase, thus facilitating fuel dissolution and actinide recovery. NO 2 voloxidation is being studied on small batches of UO 2 Simfuel, but the real test of process feasibility will be when it is scaled up to work with >100 g of irradiated material. This report discusses the aspects of scale-up that must be considered for NO 2 voloxidation, including development of a stirred reactor to promote agitation of the mixture during processing, online process monitoring, and automation controls. Brief details on parallel efforts are also provided in this report, including (a) demonstration of iodine release from Simfuel made by Spark Plasma Sintering, and (b) development of an order-of-magnitude scale-up to react 100 g of UO 2 Simfuel in a metal reactor.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nuclear fuel irradiation testbed for nuclear security applications

The nuclear security community has long been interested in the identification and quantification of nuclear material signatures to understand a material’s provenance, use, and ultimate application. New forensics signatures and methods intended for non-traditional or advanced nuclear fuel applications require fuel irradiation experiments to demonstrate viability and validity. Integral fuel irradiations have historically required significant costs and long timelines to design, irradiate, and characterize. This paper describes how a recently developed nuclear fuel irradiation testbed can be used to provide a low cost, rapid turnaround, modular test environment for irradiation and evaluation of nuclear fuel specimens for nuclear security applications. The irradiation testbed houses six small ‘MiniFuel’ samples within hermetically sealed capsules inside targets that can be removed in between each ∼25-day operating cycle of the High Flux Isotope Reactor (HFIR). As many as nine targets can be irradiated using a single irradiation position (reflector region) in HFIR, allowing for varying irradiation temperatures and burnups. A suite of hot cell capabilities have been established to perform post-irradiation examination for measuring performance (e.g., fuel swelling, fission gas release) and facilitating experiment disassembly for subsequent property measurements, microstructural analysis, or chemical assay. This new testbed allows fuel irradiations to be conducted on an accelerated timeframe to enable rapid proof of concept testing and to provide reference material for nuclear fuel security applications. Recent applications using this testbed include the testing of isotopic taggants in UO 2 fuel (intentional forensics), testing of U-10Mo fuel for down-conversion of highly enriched uranium–fueled reactors, and the production of irradiated UO 2 fuel material for signature analysis of its isotopic composition (plutonium, fission gases, etc.).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

H 2 generation by the 10 B(n,α) 7 Li reaction in high temperature water

H 2 produced in water from the 10 B(n,α) 7 Li fission reaction has been measured up to 300 °C. Thermal energy neutrons from the Rhode Island Nuclear Science Center's 2 MW reactor interact with boric acid-containing water in temperature-controlled high-pressure cells made from tubing of either titanium or zirconium alloy. After exposure for a minimum of 1 h, the solution sample is extracted and sparged with argon. The H 2 entrained by the sparging gas is sampled with a small mass spectrometer. A small amount of sodium is included in the boric acid solution so that after sparging, samples can be collected for 24 Na activation measurements in a gamma spectrometer to determine the neutron exposure and thus the total energy deposited in solution. The G-value (μmol/J) for H 2 production is obtained for water at a pressure of 25 MPa, over a temperature range from 20 °C to 300 °C. The weak temperature dependence of this yield between 150 °C and 200 °C demonstrates that the bimolecular reaction of pairs of e$^{–}_{aq}$ is a very minor source of H 2 in high LET tracks.

10B↗

Post Examination of Candidate NpO 2 Targets for 238 Pu Production

Four targets composed of sintered NpO 2 pellets enclosed in Zircaloy cladding were irradiated in the High Flux Isotope Reactor for 2 to 4 cycles to determine if an oxide pellet and Zircaloy cladding would be usable candidates for 238 Pu production. The pellets were sintered to a high fraction of theoretical density (TD) and melt wires were placed in small holes that had been drilled in the center of selected pellets to determine if the pellet centers exceeded desirable operating temperatures. After irradiation, the targets were punctured to determine the internal target pressure and the fission gas release. None of the targets had excessive pressure, and fission gas release was in the range of 4 to 38%. The targets were then cut into segments for radiochemical analysis, and metallography (MET) mounts were created to examine the pellet microstructure and to search for the melt wires to determine if they had melted. Three of the four targets resulted in successful MET mounts; the two-cycle pellets were too friable to be handled. No signs of pellet melting were noted, and unfortunately, none of the melt wires could be recovered. The results indicate that this pellet/clad design offers a practical option for 238 Pu production.

36 MATERIALS SCIENCE↗

Realizing "2001: A Space Odyssey": Piloted Spherical Torus Nuclear Fusion Propulsion

A conceptual vehicle design enabling fast, piloted outer solar system travel was created predicated on a small aspect ratio spherical torus nuclear fusion reactor. The initial requirements were satisfied by the vehicle concept, which could deliver a 172 mt crew payload from Earth to Jupiter rendezvous in 118 days, with an initial mass in low Earth orbit of 1,690 mt. Engineering conceptual design, analysis, and assessment was performed on all major systems including artificial gravity payload, central truss, nuclear fusion reactor, power conversion, magnetic nozzle, fast wave plasma heating, tankage, fuel pellet injector, startup/re-start fission reactor and battery bank, refrigeration, reaction control, communications, mission design, and space operations. Detailed fusion reactor design included analysis of plasma characteristics, power balance/utilization, first wall, toroidal field coils, heat transfer, and neutron/x-ray radiation. Technical comparisons are made between the vehicle concept and the interplanetary spacecraft depicted in the motion picture 2001: A Space Odyssey.

Williams, Craig H.↗

Extraction of Pm-147 from savannah river site nuclear material management programs

The Savannah River Site (SRS) processes used-nuclear fuel to recover uranium. There are many interesting fission products lost in the raffinate from this separation including 147 Pm. Here, the goal of this work was to recover 147 Pm from SRS waste solutions. A radiochemical separation method typically used for the determination of 147 Pm and 151 Sm was modified to purify significant quantities of 147 Pm from the H Canyon waste solutions. The developed scheme was tested on a small aliquot of waste solution from the processing of used fuel from the High Flux Isotope Reactor at Oak Ridge National Laboratory.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Bubble Mass Transport Measurement in the Large-Scale Test Loops at Oak Ridge National Laboratory

Molten salts are complex fluids that incorporate multi-phase behavior depending on the chemistry and the physical properties of the entrained components. These components include the carrier salt, the actinide fuel, and fission, activation, and corrosion products, the concentrations of which depends on the burnup history of the salt. Radionuclide transport from the salt into the cover gas / off-gas system depends on volatility as predicted by thermochemistry, but data from the Molten Salt Reactor Experiment (MSRE) conducted in the late 1960s suggest that bubble formation and transport are also important. Anomalously high fractions of noble metals were found in the off-gas system and were attributed to transportation with parent salt aerosols and their association with rising noble gas bubbles. The prediction of such phenomena requires coupled neutronic, thermal hydraulic, and chemical equilibrium calculations, the framework of which is being developed within the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program supported by the US Department of Energy (DOE) Office of Nuclear Energy (NE). However, separate effects tests and models of experiments using tools such as SAM and Thermochimica can guide model developers through important processes. Conversely, model development guides the choice of experiments and systems to provide data that are relevant for validation. This report describes several experiments that tracked gas transport in molten salts, ranging from small-scale systems to large-scale loops. Gas transportation in a molten salt, LiCl-KCl, has been studied using the shadowgraph technique. Sensors such as residual gas analysis, Raman spectroscopy, and laser-induced breakdown spectroscopy have been tested for off-gas measurements. These data were used to interpret how the gases move through the upstream salt / cover gas and the interface between them. Differential pressure measurements were able to detect individual gas bubbles as they popped at the liquid–gas interface. Salt aerosols were collected on a cascade impactor. Their formation was also observed directly via the shadowgraph method, and most of these aerosols were launched ballistically into the cover gas. Fine mists could also be observed. Convection currents through the salt were visualized and can be used to calculate the thermophysical properties of the salt itself. The apparatuses described in this report and in a previous work (McFarlane et al. 2023) have been commissioned and are available for use in making further measurements of salt/surrogate fission product behavior. Novel approaches using neutron imaging are planned for the study of fluoride salts, which cannot be contained in quartz, so shadowgraph visualization is not available. Bubble transport in convective flow and in a slow-moving salt column are planned. The mobile laser-induced breakdown spectroscopy (LIBS) system is available for several applications, including iodine capture in a molten hydroxide scrubber, H2 transport though molten salts to complement Raman analysis, and online tracking of salt aerosol generation, transport, and deposition. This report summarizes the findings from FY24 and the plans for FY25. The work completes milestone M2AT-24OR0702013 of the DOE-NE Advanced Reactor Technology, Molten Salt Reactor Campaign, DOE-NE-5.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Irradiation Testing of Ultrasonic Transducers

Ultrasonic technologies offer the potential for high accuracy and resolution in-pile measurement of numerous parameters, including geometry changes, temperature, crack initiation and growth, gas pressure and composition, and microstructural changes. Many Department of Energy-Office of Nuclear Energy (DOE-NE) programs are exploring the use of ultrasonic technologies to provide enhanced sensors for in-pile instrumentation during irradiation testing. For example, the ability of single, small diameter ultrasonic thermometers (UTs) to provide a temperature profile in candidate metallic and oxide fuel would provide much needed data for validating new fuel performance models. Other efforts include an ultrasonic technique to detect morphology changes (such as crack initiation and growth) and acoustic techniques to evaluate fission gas composition and pressure. These efforts are limited by the lack of existing knowledge of ultrasonic transducer material survivability under irradiation conditions. To address this need, the Pennsylvania State University (PSU) was awarded an Advanced Test Reactor National Scientific User Facility (ATR NSUF) project to evaluate promising magnetostrictive and piezoelectric transducer performance in the Massachusetts Institute of Technology Research Reactor (MITR) up to a fast fluence of at least 1021 n/cm2 (E> 0.1 MeV). This test will be an instrumented lead test; and real-time transducer performance data will be collected along with temperature and neutron and gamma flux data. By characterizing magnetostrictive and piezoelectric transducer survivability during irradiation, test results will enable the development of novel radiation tolerant ultrasonic sensors for use in Material and Test Reactors (MTRs). The current work bridges the gap between proven out-of-pile ultrasonic techniques and in-pile deployment of ultrasonic sensors by acquiring the data necessary to demonstrate the performance of ultrasonic transducers

Daw, J.↗