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At least 325 records · Page 18

Modeling of fission and activation products in molten salt reactors and their potential impact on the radionuclide monitoring stations of the International Monitoring System

Molten Salt Reactors (MSRs) are one of six Generation IV reactor designs currently under development around the world. Because of the unique operating conditions of MSRs, which include molten fuel and the continuous removal of gaseous fission products during operation, work was performed to analyze the potential impact of emissions on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). Simulations were performed to predict the production of IMS-relevant radionuclides in four MSR designs operating under two scenarios – (1) a sealed reactor with releases only during operational shutdown and (2) continuous reprocessing or sparging of the fuel salt. From these production estimates the radioxenon and radioiodine signatures were extracted and compared to three current reactor designs (PWR, BWR, RBMK). In the cases where continuous reprocessing of the fuel salt occurred both the radioxenon and radioiodine signatures are nearly indistinguishable from a nuclear explosion. Estimates were also made of the potential emission rate of radioxenon for three reactor designs and it was found that MSRs have the potential to emit radioxenon isotopes at a rate of 1015 – 8×1016 Bq/d for 133Xe if no abatement is used. An assessment was also made of activation products using a candidate fuel salt (FLiBe) mixed with corrosion products for the Thorium Molten Salt Reactor (TMSR-LF1)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Uranium Processing Signatures for Nuclear Forensics (NA22 End of FY23 Report)

A vacuum induction melting (VIM) furnace was used to produce an ~120 kg depleted uranium (DU) rod in November 2021 from well characterized feedstock to investigate the separation of thorium (Th) and protactinium (Pa) from uranium (U) during U metal casting and quantify the behavior of the 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry systems. This work suggested that while 234 Th, measured by gamma spectrometry, appears to segregate to the top and surface of the rod, the concentration of 230 Th determined by isotope dilution mass spectrometry (IDMS) in drill turnings from multiple locations in the rod, including the hot top, is relatively consistent. To evaluate whether Th is potentially enriched at only the very outer surface of the cast DU rod relative to the bulk material in the cast rod, thin surface samples were collected from the cast DU rod. Locations sampled included the inner diameter (ID) and outer diameter (OD) of the bottom of the casting and the ID, OD, and top face of the hot top (very top of the casting). The locations are shown in Figure 1. Four samples were taken from each location at different depths in the cast material. Each cut took approximately 0.03 – 0.05” off of the casting.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Disposition Options for Sodium Cooled Fast Reactor (A White Paper)

The sodium-cooled fast reactor (SFR) design concept is one of the six classes of nuclear reactors in the GenIV initiative. SFRs are uranium or plutonium-fueled reactors operating in the fast neutron spectrum using liquid sodium as the coolant. SFRs can be designed as a breeder reactor or actinide-burning reactor in addition to operating the thorium fuel cycle. While having different fuel designs, the anticipated waste streams, and the necessary management strategies for spent nuclear fuel (SNF) and radioactive wastes from SFRs are very similar. This includes the SNF, activated sodium coolant, in-core stainless-steel components, piping, resins and filters, solidified liquid waste, contaminated equipment, and other radioactive wastes. Modern SFR designs are based on a long and rich operating history of several liquid-metal-cooled fast reactors with sodium coolant. Several of these reactors have been shut down, the fuel has been placed in safe storage, and they have undergone some degree of decommissioning. As such, there is significant experience in the management of the SNF and radioactive wastes associated with operating these reactors. This white paper will identify the definitions and regulations that apply to the safe and secure management, storage, and disposal of radioactive waste and identify the key radioactive waste streams from SFRs. Idaho National Laboratory has significant experience in the management of the SNF from the SFR predecessors. This experience should form the basis for the management and disposition efforts of the radioactive waste from any new SFR-type small modular reactor or microreactor intended for deployment at the Idaho National Laboratory Site

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Assessment of Technical Information Needs and Considerations for Front-End Activities for Molten Salt Fuel Types

This report details an assessment of the hazards and safety impacts related to front-end operations of molten salt reactors (MSR) as well as an assessment of existing safety guidance. Publicly available information was evaluated to make recommendations to the U.S. Nuclear Regulatory Commission (NRC) for guidance development and information gathering needs. Five different MSR technologies were evaluated along with information from 1960’s about the Atomic Energy Commission programs for the Aircraft Reactor Experiment and Molten Salt Reactor Experiment. Primary areas of evaluation include fuel cycle facilities, transportation and at reactor fuel mixing operations up to reactor startup. In general, there was difficulty synthesizing publicly available information due to the early stage of the MSR development and proprietary information associated with the reactor technology companies analyzed. There are a few specific recommendations from this report. One overarching paradigm shift that the NRC needs to evaluate is the possibility of collocating fuel cycle facilities with operating MSRs. Although there is no specific prohibition to this in the NRC regulations, the collocation of the fuel cycle facilities with the operating MSR presents a novel approach compared to the light water reactor baseline. More guidance and research into thorium operations and regulation is needed. The hazards associated with the stability of stored fuel constituents need to be evaluated. Some reactor fuel cycles use beryllium, and its use and the associated hazards need further analysis. NRC-approved designs for transportation packages for shipping molten salt fuels and factory-built and fueled reactors are not available.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Documentation of Air Emissions Source Term for Radionuclide NESHAP Compliance: TA-53 Building 0984 Isotope Production Facility

This paper will document the air emissions source term for the TA-53 Building 0984 Isotope Production Facility (IPF). The facility has historically been managed as a minor source under Radionuclide NESHAP regulations, but began using a wider variety of irradiation targets and a higher beam current. To support expanded generation of actinium-225 for medical diagnostic and therapeutic uses, IPF is now irradiating thorium targets and the beam current is planned to increase from 250 microamperes up to 600 microamperes. These changes merit a review of the anticipated source term under the new proposed operational conditions. The end result of the review indicates the main stack (Exhaust Stack ES-1) needs to be managed as a major source with continuous emissions monitoring. No additional advance notifications or permitting is required as a result of these operational changes.

54 ENVIRONMENTAL SCIENCES↗

SCALE Analyses of Scenarios in the Molten Salt Reactor Fuel Cycle

In support of the US Nuclear Regulatory Commission non-light-water reactor fuel cycle demonstration project, the capabilities of SCALE 6.3.1 for radionuclide characterization, criticality, and shielding were demonstrated through several scenarios in a molten salt reactor (MSR) nuclear fuel cycle. Three scenarios were selected for this study, with the molten salt breeder reactor (MSBR) serving as the reference design. The original thorium-based fuel salt used in MSBR was replaced with a 235 U-enriched fuel salt to better reflect anticipated future MSR concepts. The first scenario focused on the fuel salt preparation stage. Criticality analyses, using SCALE/CSAS-Shift and SCALE/SAMPLER, examined potential critical configurations in the fresh fuel salt container based on variables such as 235 U enrichment, UF 4 molar fraction, temperature, and container geometry. The second scenario explored the release of fission products during reactor operation in which the tritium buildup in the primary fuel salt was quantified through depletion calculations using SCALE/TRITON with continuous fuel makeup and fractional fission product removal. This scenario also assessed radioactivity levels in the off-gas system (OGS), quantifying radiotoxic nuclides that could be released into the environment. SCALE/SAMPLER was employed to perform uncertainty quantification to identify key operating parameters influencing the buildup of radiotoxic nuclides in the OGS. Additionally, radiation dose rates were calculated using SCALE/MAVRIC to estimate the maximum exposure levels within the reactor cell complex during operation. The final scenario evaluated the decay heat and radioactivity of the primary fuel salt collected in the drain tank, as well as the radiation dose rate outside the building from the presence of the drain tank. Overall, the application of SCALE’s various capabilities for radionuclide inventory generation, criticality analysis, and shielding in MSR fuel cycles was successfully demonstrated across these scenarios.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Characterization of MC&A for the Molten Salt Fuel Cycle

Advanced reactor developers are exploring diverse reactor designs, including molten salt reactors (MSRs). These advanced reactors are considered for wider applications and a range of deployment locations, including supporting the integration of renewable energy sources in the grid. There are three main types of MSRs: (1) reactors in which the fuel salt freely circulates within the core; (2) reactors with the fuel salt contained within vented fuel tubes; and (3) reactors that use molten salt solely as a coolant, with the fuel in a separate, solid form. In this document, the term MSR refers specifically to the first two types, which use fuel salt—special nuclear material (enriched uranium, plutonium, and 233 U) in chloride or fluoride form mixed with chloride- or fluoride-based carrier salt in a peritectic mixture—as the primary medium for fission. The composition of fuel salt, both at startup and for makeup or refueling, varies depending on the MSR design and the chosen fuel cycle approach, which can be either once-through or closed. For MSRs, a variety of fuel cycle approaches (e.g., U, U–Pu, U–Pu–TRU, U–Th, U–Pu–Th) are being considered. Fuel in MSRs is much different than traditional solid fuel, including its preparation. The uniqueness warrants investigation into characterizing fuel preparation processes, known as fuel salt synthesis . This effort characterized major fuel preparation and synthesis processes, identifying temperature, equipment, and environmental requirements for uranium-, plutonium-, and thorium-based fuel preparation and synthesis. Because MSR fuel salt synthesis facilities handle special nuclear material in loose, bulk form, a material control and accounting plan will be required for licensing from the US Nuclear Regulatory Commission or under the US Department of Energy authorization. This effort serves as a foundation to investigate material control and accounting approaches for synthesis facilities, including determining measurement points and techniques. Because several MSR developers are planning demonstration facilities in the coming years, this effort will support stakeholders with preparing or reviewing material control and accounting plans for providing assurance that all special nuclear material is accounted for at fuel salt synthesis facilities. This report was produced for Materials Protection, Accounting, and Control Technologies (MPACT) program under the US Department of Energy (DOE), Office of Nuclear Energy, Nuclear Fuel Cycle and Supply Chain.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Exploring Actinide Nanocrystal Growth towards Defining 5f Surface Chemistry (Final Technical Report)

When particles are very small, down to the nanometer length scale, they display unusual properties not typical of larger materials. Most of the atoms in these structures are at the surface of the particles, which give them different electronic properties. While these unusual properties have been studied in most of the periodic table, little is known about how the electronic properties of the actinides, such as neptunium and plutonium, behave when they become so small. This planned research will study growth pathways of actinide nanoscale particles. Interestingly, the shapes of the particles change depending on the specific actinide species, spanning from thorium through americium, despite having otherwise identical arrangements of atoms. This project will use differences in the shapes and growth pathways of different actinide particles to learn about trends in electronic properties at surfaces across the actinide row. Growth pathways will be determined using a combination of synthesis and the use of advanced X-ray characterization tools. These X-ray characterization tools can provide information about electronic properties and also local bonding characteristics. This project will also inform how to make unprecedented actinide oxide nanoparticles using very small quantities of material. This will enable safe working with radioactive materials and the study of materials that never before have been made into nanoparticles. Meanwhile, students will be trained in working with these exotic materials.

36 MATERIALS SCIENCE↗

Metallic Coating of Cerium Oxide Microspheres

The ability to remove heat is paramount to nuclear fuel performance and longevity. Retaining fission product and separating fuel from reactor coolant and the environment is also necessary to prevent radiological contamination. Conventional nuclear fuel for commercial light water reactors and radioisotope power systems (RPS) is composed of oxide powders pressed into a pellet (cm-scale) and then sealed into a metal cladding to confine the fuel. What typical fuels lack is a method to surround each particle of nuclear fuel in metal, thus providing a more intimate protection layer for accident tolerance and boosting the thermal extraction from the fuel element. In such a way, metal-coated fuel particles increase heat extraction efficiency over clad-pellet designs while increasing the accident tolerance of the fuel. Metal oxide microspheres have wide-ranging applications, including the realm of fuels for nuclear reactors and RPS. Microspheres of uranium oxide/uranium carbide, mixed uranium/plutonium oxides, transuranics, and thorium fuels have been extensively studied. Pacific Northwest National Laboratory has also demonstrated the production of 238 PuO 2 microspheres for RPS applications. Metal-coated oxide microsphere fuels may also be attractive for other applications such as nuclear thermal rockets, future nuclear reactor designs, and catalysts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Refining a Novel Process Monitoring Method to Safeguard Continuously Cycling Designs Using Isotopic Ratios

In advanced reactor (AR) designs, a common feature is continuous chemical processing and circulation of the nuclear material. This work bridges a significant measurement gap in safeguarding reactors with circulating fuel or continuous refueling by leveraging and building on the isotope ratio method first developed by our team under an FY21 Advanced Reactors International Safeguards Engagement (ARISE) project (Uribe et al. 2021). In circulating fuel designs, the radioisotope inventory changes from traditional effects (e.g., radioactive decay, fission) but also includes material transport due to pressure and temperature gradients. Such designs may also require regular or continuous additions or removals during operation, which significantly increases the rate of inventory change compared to traditional pressurized water reactor (PWR)s. Thus, directly tracking the nuclear inventory is ineffective since the isotopes are continuously added and removed. The isotope ratio method instead focuses on detecting changes to the input and output flows of radioisotopes. Previous work showed that for well-chosen pairs of isotopes, the isotopic ratio provides a sensitive and lasting indicator of deviation from normal conditions (e.g., startup, shutdown, diversion). The isotope ratio method is a process monitoring method with potential for application in for forward-looking approaches to International Atomic Energy Agency (IAEA) safeguards. The original process monitoring method was developed for a specific case—the decay tank of a thorium-fueled molten salt breeder reactor. In this expanded work, we explored other types of reactors and processes with nonstationary (e.g., flowing) nuclear material, which are difficult to safeguard with traditional methods because of the transient nature of the systems. The goal of the present work is to generalize the isotope ratio method for use in processes with continuously flowing nuclear material. All continuous processes have an average time for isotopes to be replaced in the system. The isotope ratio method works by choosing radioisotopes with half-lives both above and below the processing time. The present work seeks to explore which isotopes are suitable for the method by simulating the nuclear inventory, radioisotope emissions, and detector responses for several classes of advanced reactors. While the method can in principle be applied to other processes (e.g., enrichment or reprocessing facilities), the present work limits scope to ARs with continuously flowing fuel. Section 2 details the mathematics supporting the isotope ratio method, and Section 3 introduces the representative ARs selected for this work. Section 4 discusses how each reactor was analyzed, and Section 5 showcases the results for each representative reactor. Finally, Section 6 provides concluding remarks and suggests pathways for further analysis.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Best Methods for Fluoride Fuel Salt Dissolution and Digestion

This report serves as the deliverable for Milestone M4FT-26AN080502015 (Report on methodology for elemental/isotopic analysis of fluoride fuel salts). The review within this document is a summary of the current literature identified by Argonne regarding fluoride salt dissolution and digestion methods and provides guidance on selecting optimal fluoride dissolution and digestion methods for future fuel salt qualification studies. Methods are compared based on completeness of digestion, chemical hazards, and tradeoffs such as equipment needs or potential to introduce impurities. Recommendations are provided for best dissolution and digestion methods for uranium- and thorium-bearing salts, and ideas for key future experiments are described.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluation of Candidate Theranostics for 227 Th/ 89 Zr Paired Radioimmunotherapy of Lymphoma

227 Th is a promising radioisotope for targeted α-particle therapy. It produces 5 α-particles through its decay, with the clinically approved 223 Ra as its first daughter. There is an ample supply of 227 Th, allowing for clinical use; however, the chemical challenges of chelating this large tetravalent f-block cation are considerable. Using the CD20-targeting antibody ofatumumab, we evaluated chelation of 227 Th 4+ for α-particle–emitting and radiotheranostic applications. Methods: We compared 4 bifunctional chelators for thorium radiopharmaceutical preparation: S-2-(4-Isothiocyanatobenzyl)-1,4,7,10-tetraazacyclododecane tetraacetic acid (p-SCN-Bn-DOTA), 2-(4-isothicyanatobenzyl)-1,2,7,10,13-hexaazacyclooctadecane-1,4,7,10,13,16-hexaacetic acid (p-SCN-Bn-HEHA), p-isothiacyanatophenyl-1-hydroxy-2-oxopiperidine-desferrioxamine (DFOcyclo*-p-Phe-NCS), and macrocyclic 1,2-HOPO N-hydroxysuccinimide (L804-NHS). Immunoconstructs were evaluated for yield, purity, and stability in vitro and in vivo. Tumor targeting of the lead 227 Th-labeled compound in vivo was performed in CD20-expressing models and compared with a companion 89 Zr-labeled PET agent. Results: 227 Th-labeled ofatumumab-chelator constructs were synthesized to a radiochemical purity of more than 95%, excepting HEHA. 227 Th-HEHA-ofatumumab showed moderate in vitro stability. 227 Th-DFOcyclo*-ofatumumab presented excellent 227 Th labeling efficiency; however, high liver and spleen uptake was revealed in vivo, indicative of aggregation. 227 Th-DOTA-ofatumumab labeled poorly, yielding no more than 5%, with low specific activity (0.08 GBq/g) and modest long-term in vitro stability (<80%). 227 Th-L804-ofatumumab coordinated 227 Th rapidly and efficiently at high yields, purity, and specific activity (8 GBq/g) and demonstrated extended stability. In vivo tumor targeting confirmed the utility of this chelator, and the diagnostic analog, 89 Zr-L804-ofatumumab, showed organ distribution matching that of 227 Th to delineate SU-DHL-6 tumors. Conclusion: Commercially available and novel chelators for 227 Th showed a range of performances. The L804 chelator can be used with potent radiotheranostic capabilities for 89 Zr/ 227 Th quantitative imaging and α-particle therapy.

227Th↗

Thermodynamics Modeling for Actinide Monocarbides and Mononitrides from First Principles

The high-temperature thermodynamical properties for the actinide monocarbides and mononitrides ThC, ThN, UC, UN, PuC, and PuN are calculated from first-principles electronic-structure theory. The electronic structure is modeled with density-functional theory (DFT) and is fully relativistic, including the spin-orbit interaction. Furthermore, the DFT is extended to account for orbital–orbital interactions, by means of a parameter-free orbital-polarization (OP) technique, that has proven to be essential for the 5f electrons in plutonium. Strong anharmonicity and the temperature dependence of the lattice vibrations are captured with the self-consistent ab initio lattice dynamics (SCAILD) method. The calculated free energies and heat capacities are compared to published results from quasi-harmonic (QH) theory, and experiments, where available. For the uranium and plutonium compounds, we make use of CALPHAD assessments to help evaluate the theory. Generally, our anharmonic relativistic approach compares well with both CALPHAD and experiments. For the thorium compounds, our theory is in good accord with QH modeling of the free energy at lower temperatures but for the heat capacity the comparison is less favorable.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗