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Development Results on Replacement Materials for Current Scarce or High Supply Chain Risk Materials

In September 2020, the U.S. government issued an executive order to address the threat to the domestic supply chain from its reliance on critical minerals (CMs) from foreign competitors and to support the domestic mining and processing industry. The Advanced Materials and Manufacturing Technology (AMMT) program is addressing this executive order by evaluating advanced manufacturing (AM) and its impact on the demands of CMs for energy production in general and how the deployment of AM in nuclear energy will support the projected goals of the Paris Accord and further a net-zero carbon economy (NZE) by 2050. Three strategic reports were previously prepared by the AMMT program to date and identified two areas for more detailed exploration: (1) the replacement of high-risk CMs such as cobalt and niobium by more abundant minerals and (2) the minimization and utilization of CM waste streams. The design of nuclear materials without critical elements as alloying elements, is a part of the nuclear materials strategy to overcome the critical minerals scarcity. In this report, two approaches are evaluated namely (1) replacement of critical elements as alloying elements in nuclear materials, and (2) the design of a new alloys that does not contain critical minerals as an alloying element.

36 MATERIALS SCIENCE↗

Control Boundary Analysis for Liquid-Fueled Molten Salt Reactors

The US Nuclear Regulatory Commission (NRC) will likely require license applicants for liquid-fueled molten salt reactors (MSRs) with circulating fuel to submit a nuclear material control and accounting (MC&A) plan or provide a detailed MC&A program description for the facility. In liquid-fueled MSRs with special nuclear material (SNM) in bulk form (i.e., not in discrete items) and with rapidly changing quantities due to fuel transmutation and depletion, a novel MC&A approach is needed because traditional nuclear material accounting methods with material balance evaluations will not be sufficient. This report details the continued efforts carried out at Oak Ridge National Laboratory (ORNL) during FY 2025 to develop a distinct MC&A approach suitable specifically for domestic safeguards of the first-of-a-kind MSRs. These efforts are built on previous ORNL efforts reported in ORNL/SPR-2023/3181 and ORNL/SPR-2024/3555.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Krypton-85 chronometry of spent nuclear fuel

We describe the use of the radionuclide 85 Kr, which is produced by nuclear fission and has a half-life of 10.76 years, to determine the age of spent nuclear fuel. The method is based on mass-spectrometric measurement of the relative abundance of fissiogenic Kr isotopes extracted from a fuel sample, and we show that it can be applied to micron-scale particles of spent fuel that are analogous to particles that have been released into the environment from various nuclear facilities in the past. 85 Kr chronometry is potentially valuable for identifying and attributing nuclear materials, grouping samples into collections of common origin that can be used to reconstruct the origin and irradiation history of the material, and verifying declared nuclear activities in the context of international monitoring programs.

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↗

Application of Hybrid K-Edge Densitometry in Reprocessing Facilities

During reprocessing operations, accurately determining the elemental concentrations of uranium and plutonium is critical for nuclear security. Reprocessing facilities processes hundreds of tons of nuclear material annually, requiring accurate measurements to ensure effective nuclear material control and accountability. Hybrid K-edge densitometry (HKED) system combines K-edge absorption densitometry with x-ray fluorescence to measure actinide elemental concentrations with a low uncertainty. This system uses high-purity germanium gamma-ray detectors and advanced signal processing equipment to detect x-ray accurately. This document provides guidance on how to achieve effective performance from an HKED system for measuring uranium and plutonium concentrations in reprocessing facilities. It includes best practices for the setup and operation of an HKED system, while highlighting factors influencing uncertainties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Understanding Formation of Irradiation-Induced Defects through 4D-STEM, Electron Tomography, and WBDF-STEM

A major challenge in advancing nuclear materials for next-generation fission and proposed fusion reactors is to comprehensively understand the formation of irradiation-induced defects. Here it is essential to correlate the evolution of irradiation-induced defects and the degradation of mechanical properties, as they collectively dictate the material's lifespan and ensure nuclear safety. Scanning transmission electron microscopy (STEM) based techniques have emerged as indispensable tools for irradiation-induced defect characterization, offering high spatial resolution imaging and chemical analysis, such as electron energy loss spectroscopy (EELS) and energy dispersive X-ray spectroscopy (EDXS). These techniques have been effectively used to obtain an atomic-scale view of the defect structure. Recent advances in electron microscopy, particularly in 4D-STEM, offer detailed insight into microstructural evolution by capturing full 2D diffraction patterns at every pixel position. Using high-speed direct electron detectors, this technology generates a four-dimensional dataset, overcoming the limitations of traditional STEM imaging.

36 MATERIALS SCIENCE↗

Detection of uranium-photofission neutrons with a 4 He scintillation detector

The use of photon active interrogation to detect special nuclear material has held significant theoretical promise, as the interrogating source particles, photons, are fundamentally different from one of the main signatures of special nuclear material: neutrons produced in nuclear fission. However, neutrons produced by photonuclear reactions in the accelerator target, collimator, and environment can obscure the fission neutron signal. These (γ, n) neutrons could be discriminated from fission neutrons by their energy spectrum, but common detectors sensitive to the neutron spectrum, like organic scintillators, are typically hampered by the intense photon background characteristic of photon-based active interrogation. In contrast, high-pressure 4 ⁢He-based scintillation detectors are well-suited to photon active interrogation, as they are similarly sensitive to fast neutrons and can measure their spectrum, but show little response to gamma rays. Here, in this work, a photon active interrogation system utilizing a 4 ⁢He scintillation detector and a 9 MeV linac-bremsstrahlung x-ray source was experimentally evaluated. The detector was shown to be capable of operating in intense gamma-ray environments and detecting photofission neutrons from 238 ⁢U when interrogated by this x-ray source. The photofission neutrons show clear spectral separation from (γ, n) neutrons produced in lead, a common shielding material.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

The effect of gamma ray irradiation on few layered MoSe2: A material for nuclear and space applications

In recent years, emerging two-dimensional (2D) materials, such as molybdenum diselenide (MoSe2), have been at the center of attention for many researchers. This is due to their unique and fascinating physicochemical properties that make them attractive in space and defense applications that include shielding harsh irradiation environments. In this study, we examined the effects of gamma (γ) rays at various doses on the structural, chemical, and optical properties of MoSe2 layers. After the samples were exposed to intense gamma radiation (from a 60Co source) with various exposure times to vary the total accumulated dosage (up to 100 kGy), Raman and photoluminescence spectroscopies were used to study and probe radiation-induced changes to the samples. When compared to pristine materials, very few changes in optical properties were typically observed, indicating good robustness with little sensitivity, even at relatively high doses of gamma radiation. The imaging using scanning electron microscopy revealed a number of nano-hillocks that were connected to substrate alterations. X-ray photoelectron spectroscopies revealed that Mo’s binding energies remained the same, but Se’s binding energies blueshifted. We associated this shift with the decrease in Se vacancies that occurred after irradiation as a result of Mo atoms creating adatoms next to Se atoms. When compared to pristine materials, very few changes in optical, chemical, and structural properties were typically observed. These findings highlight the inherent resilience of MoSe2 in hostile radioactive conditions, which spurs additional research into their optical, electrical, and structural characteristics as well as exploration for potential space, energy, and defense applications.

Materials Science↗

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↗

Updated uranium reference material 231 Pa/ 235 U consensus model ages for nuclear forensics

Radiochronometry provides the model age of nuclear materials, which is useful for understanding the production history of materials found outside of regulatory control. Certified reference materials (CRMs) are important for radiochronometry to increase confidence in measurement quality; however, the absence of 231 Pa/ 235 U CRMs necessitates that nuclear forensic laboratories measure the 231 Pa/ 235 U model ages of preexisting uranium reference materials. Here, in this work, new consensus 231 Pa/ 235 U model ages are reported from three nuclear forensic laboratories for three reference materials using current analytical methods. These updated consensus values can be used for quality control of 231 Pa/ 235 U model age measurements.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Peridynamic modeling of cementitious materials for nuclear waste management

Radioactive and hazardous waste generated from fuel processing plants, nuclear reactors, and hospitals, requires effective management strategies. Cementitious materials are widely applied for these needs, serving as structural materials, reactive barriers, or waste forms. In these applications cracking poses a significant risk to performance, driven by inconsistent shrinkage of the components and the varying strength and permeability of their interfaces. Traditional modeling approaches face challenges in representing the complex fracture behavior of cementitious materials due to the reliance on spatial derivatives and difficulties with mesh generation. Here, to overcome these limitations, we employ peridynamics, a novel continuum mechanics formulation that uses integrals to describe mechanical equilibrium, avoiding discontinuities associated with traditional methods. Through incorporation of a bi-linear softening model and quasistatics, an experimentally validated model for Portland cement concrete samples was created. Mechanical parameters, including compressive strength and elastic modulus were validated and variation due to aggregate packing was evaluated. Additionally, sensitivity analysis of the peridynamic parameters to the bulk material properties was established. The results lay the groundwork for evaluating the impact of unique conditions of cementitious waste forms that can be assessed to improve the reliability of waste management strategies.

Aggregates↗

Influence of helium bubbles on the bulk equation of state of gold under static compression

Nuclear materials often evolve into two-phase systems comprising a bulk matrix with dispersed inert-gas bubbles. The presence of these bubbles can have consequences to the thermomechanical response of materials and is a key life-limiting factor in some nuclear fuel forms. Understanding the behavior of these two-phase, bubble-matrix systems is, thus, important to improved predictive models and frameworks for many nuclear materials applications. While temperature excursions of these two-phase systems have been characterized, fewer studies have focused on the evolution of inert-gas bubbles under pressure. Here, in this paper, we use x-ray tools to interrogate a He-implanted gold foil to determine the pressure-dependent evolution of the individual components (Au matrix + bubbles), and we compare that total pressure dependence to theoretical equation-of-state descriptions based on mixing rules.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Neutron Total Scattering Analysis of Materials for the Nuclear Fuel Cycle

Here, this paper reviews recent experimental efforts at the University of Tennessee and Oak Ridge National Laboratory to comprehensively characterize the structural details of materials relevant for the nuclear fuel cycle by employing advanced neutron scattering techniques. For the study of nuclear ceramics, neutron scattering offers distinct advantages over traditional laboratory or synchrotron X-ray diffraction, including enhanced sensitivity to elements with a low atomic mass, such as oxygen, nitrogen, and carbon. The key to these efforts is the recent advancement in the neutron scattering infrastructure at the high-flux diffractometers at the Spallation Neutron Source. The high neutron flux at these instruments enables neutron total scattering, a nondestructive bulk technique that simultaneously captures both short-range structural effects through pair distribution function analysis and long-range order through diffraction pattern analysis. This approach is particularly important for a comprehensive description of defective, disordered, or amorphous nuclear materials. The case studies presented here include analyses of the local defect structure in hyperstoichiometric uranium oxides and short-range order of ion-irradiated ceramics. This advanced analytical methodology will improve our understanding of the behavior of materials in extreme environments and contribute to the development of more resilient nuclear materials.

Neutron scattering↗

Alternative Analysis and Prioritization of Department of Energy “TBD” Materials with No Identified Disposition Pathway

The Department of Energy (DOE) complex manages a significant inventory of excess nuclear materials for which disposition pathways have not been identified, commonly referred to as "To Be Determined" (TBD) items. The Disposition Pathways Program, initiated in FY2018, provides a standardized framework for identifying viable disposition pathways for these materials. In 2023, the program undertook a comprehensive review and systematic analysis of the remaining TBD material groups, updating the assessment from the 2020 TBD Study using the 2022 fiscal year-end Nuclear Material Inventory Assessment (NMIA) as the primary data source. This effort aimed to utilize quantitative analysis to down-select from a wide range of potential disposition options and prioritize the remaining pathways to facilitate informed, risk-based decision-making for future programmatic funding and execution. This paper details the alternative analysis methodology used for screening and prioritization, highlighting the key criteria, ranking process, and resultant recommendations. The study successfully narrowed fifty-two potential disposition options down to nineteen, providing a focused path forward for addressing a longstanding challenge within the DOE complex.

Ramsey, Catherine [Savannah River National Laborat↗

Evaluation of material accountancy techniques for 233 Pa from thorium nuclear fuels

Thorium is a promising alternative to uranium as nuclear fuel with advantages such as higher abundance, lower production of long-lived transuranic elements, and potentially better proliferation resistance. However, thorium presents a potential pathway for proliferation where produced 233 Pa can be diverted for the clandestine production of safeguarded 233 U. To prevent this, the ability to detect and measure 233 Pa must be assessed. This paper reviews several nuclear material accountancy techniques to determine their suitability for detecting 233 Pa extracted from irradiated thorium fuel. Hybrid K-edge densitometry and passive gamma spectroscopy have been found to be the best options based on technology maturity, cost, accuracy, and acquisition time. Thorium can be used in various reactor designs such as pressurized water reactors (PWRs), Canada deuterium uranium (CANDU) reactors, and molten salt reactors (MSRs). Therefore, thorium-uranium oxide fueling was modeled for three representative reactors (PWR, CANDU, MSR), burning the fuel to 47 GWd/MTHM for PWR, 19 GWd/MTHM for CANDU, and at a steady power of 52.711 MW/MTHM for MSR. Within each model, the protactinium element in the used fuel was extracted and its isotopic content analyzed. Simulated results indicated that 233 Pa can be detected using passive gamma spectroscopy in each fuel type at all decay times (0–300 days) following separation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Use of a deuterium-deuterium neutron generator for the Add-A-Source waste matrix correction technique

Neutron generators offer an alternative to radioactive sources in the application of active techniques for nondestructive assay of nuclear materials. The Add-A-Source technique has enabled improvements in the ability to accurately measure waste bearing nuclear materials by measuring and correcting for the non-nuclear matrix effect. The technique has historically been performed with a Cf-252 spontaneous fission source. Here, in this work, we have demonstrated the use of a Deuterium-deuterium neutron generator in place of the Cf-252 source. A DD generator enables operational advantages and allows the simplification of the instrument design, while offering equivalent corrective performance as a Cf-252 source.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA/DOE/DOD nuclear propulsion technology planning: Summary of FY 1991 interagency panel results

Interagency (NASA/DOE/DOD) technical panels worked in 1991 to evaluate critical nuclear propulsion issues, compare nuclear propulsion concepts for a manned Mars mission on a consistent basis, and to continue planning a technology development project for the Space Exploration Initiative (SEI). Panels were formed to address mission analysis, nuclear facilities, safety policy, nuclear fuels and materials, nuclear electric propulsion technology, and nuclear thermal propulsion technology. A summary of the results and recommendations of the panels is presented.

Clark, John S.↗