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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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DOE OSTI2022

The Impact of Increased Requirements for Verification Measurements of Category III and IV Receipts

As part of the regular nuclear material accounting and control process, sites that have accountable nuclear material regularly perform measurements of the material in their possession. The expectation for the type of measurements and their frequency is set out in Department of Energy (DOE) Order 474.2, and further detailed in each site’s respective material control and accountability (MC&A) plan and associated controlling documents. The measurements of interest in this report are those performed on external (between DOE sites) transfer receipts of Category III or IV accountable materials. In 2020, a revision of DOE Order 474.2 was proposed that would significantly increase the requirement that measurements be performed upon receipt of material, and further, that those measurements be quantitative verification (rather than qualitative confirmatory) measurements. A survey was performed of DOE sites to discuss the impact on their MC&A measurements program if more rigorous verification measurements requirements for Category III and IV receipts were implemented. An assessment of nondestructive assay (NDA) measurement instruments to meet those needs was also performed. Across the board, sites indicated that personnel and budget would cause the largest impact. Sites which are qualified as Category I/II indicated a reduced impact as these sites already have the measurement capabilities and some personnel but would require the acquisition of additional measurement systems. Category III/IV sites indicated a much larger impact as these sites generally have smaller MC&A programs. A few smaller sites stated a measurement program would need to be created to handle the demand. Calorimetry, quantitative gamma spectroscopy and neutron coincidence counting systems were identified as common systems that could meet the verification measurement requirements. The other, and perhaps larger issue is the need for calibration standards for the calorimetry and neutron coincidence counting systems. It is proposed that a comparative study be performed for ISOCS and ISOTOPICS, qualification of a COTS calorimetry system be performed, and development of an AWCC system that uses a neutron generator.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2025

An In Situ Feed Monitoring System for Molten Salt Reactors with Fast Neutron Energy Spectrum Molten Salt Reactor Applications

Molten salt reactors (MSRs) are one of the six promising advanced reactor technologies selected for further research and development by the Generation IV International Forum. More than twenty MSR designs are actively being developed around the world. Several of these designs are liquid-fueled and intended for operation within the fast neutron energy spectrum.1 National regulations will require liquid-fueled MSRs to control and account for nuclear material within licensed facilities. Additionally, states with comprehensive safeguards agreements with the International Atomic Energy Agency (IAEA) are obligated to declare nuclear material quantities within facilities. In return, the IAEA Department of Safeguards independently verifies these quantities and provides assurance that the nuclear material and facility are being used only for peaceful purposes. One key distinction of liquid-fueled MSRs compared with other types of reactors is that in portions of the facility, the nuclear material is in bulk form rather than discrete items. Traditional nuclear material accounting techniques such as physical item counting and verification of serial numbers on fresh fuel assemblies do not translate directly to all process streams within liquid-fueled reactors. Liquid-fueled MSRs are typically designed with low excess reactivity. This feature provides safety benefits but also means that most MSRs require the addition of makeup fuel salt while a reactor is operational. The nuclear material in the initial fuel salt and in any makeup fuel salt must be quantified. Additionally, distinct nuclear material diversion and reactor misuse scenarios form the basis of the detection methods and monitoring systems developed for liquid-fueled MSRs. For example, the IAEA provides assurance that fuel salt containing nuclear material is not being diverted from the system, that the feed salt matches the reported actinide concentrations and uranium enrichment, and that no additional fertile material is being introduced into the system. Measurement systems currently used for nuclear material control and accounting are not directly applicable to achieving MSR safeguards goals. This paper concerns a system being designed to account for the nuclear material added to liquid-fueled MSRs and monitor for diversion and misuse scenarios related to MSR feed systems.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Nuclear Materials Process Modeling at the Y-12 National Security Complex

The Y-12 National Security Complex (Y-12) has implemented process modeling for various accountable nuclear materials operations that are performed throughout the plant. Using a discrete, event-based dynamic simulation program, key nuclear material streams are modeled, allowing Y-12 to effectively manage numerous points of interest within the plant’s production operations. Integration of the various material processes into a single, interdependent supply and demand model is one of the ongoing focuses within Y-12’s process modeling effort. The primary purpose of using dynamic simulation modeling is to allow for analysis of the nuclear materials inventories and forecasted supplies based on future demands. Analysis of these inventories includes capacity evaluation, bottleneck mitigation, and assessments of individual pieces of equipment to inform future facility investment decisions and associated project schedules. Modeling of the nuclear materials processes throughout the complex also allows for incorporation of changes relevant to production capabilities such as the upcoming transition of specific operations to the new Uranium Processing Facility. Prior to implementation of process modeling, Y-12 forecasted supply and demand of accountable nuclear materials streams using Microsoft Excel. With deterministic models such as Microsoft Excel, the annual forecasts, generated within data input condition parameters, can only provide a fixed point of data. Fixed data cannot simulate integrated material streams and account for the possibility of occurrences and other changes that dynamic simulations take into consideration. Y-12’s dynamic process modeling allows integrated simulations of multiple accountable nuclear materials processes, including supply and demand forecasting and analysis, and is a coordinated effort involving many steps of verification and validation (V&V), site briefings, testing, reporting, data mining, planning, and documentation that spans various programs throughout the Y-12 complex.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2024

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↗
DOE OSTI2023

Nuclear Material Control & Accounting for Pebble Bed Reactors (FY 2023 Summary Report)

This report discusses the work done under the US Department of Energy NE-5 Advanced Reactor Safeguards and Security Program during FY 2023. It provides a summary of material control and accounting (MC&A) for pebble bed reactors (PBRs) and addresses some of the main challenges with current PBR MC&A approaches that will inform safeguards and security by design efforts. The efforts to date have focused on tristructural isotropic (TRISO) pebble fuel material accounting and control including working with partners in industry, loss and production of nuclear material as part of reactor operations, burnup modeling and measurements, uncertainty quantifications for such modeling and measurements, statistical approaches needed, and measurement methods. The unique fuel management and utilization in a PBR, where the fuel in spherical form is introduced and circulates through the reactor, poses special challenges for MC&A. This contrasts with traditional water-cooled reactors in which the fuel is contained in large assemblies and can be easily identified and counted. Even online fueled reactors, such as the CANDU reactors (none of which operate in the United States), are significantly different because the fuel is still contained in relatively large assemblies, is uniquely identified, and the number of assemblies that pass through the core on an annual basis is much fewer than the hundreds of thousands that circulate in a PBR, none of which are uniquely identified. Additionally, the nature of the TRISO fuel results in very low heavy metal loading with each pebble containing less than 10 g of uranium and on the order of less than 1 g of fissile material. This low fuel density and the robustness of the TRISO particles are major features of the TRISO fuel from a safety basis as each TRISO particle and pebble acts as a containment for the nuclear material and fission products during normal and accident conditions. This also results in very low plutonium loading per pebble during normal operations, which is on the order of 0.1 g at full burnup. A major feature of PBRs is that they will allow for significantly higher burnup, on the order of 160 GWd/THM compared to the burnup of traditional LWRs, which is on the order of 45 GWd/THM. This is achieved by monitoring the pebbles as they circulate through the reactor and allowing them to be reintroduced into the core until the desired burnup is achieved and they are removed from the reactor and enter the spent fuel storage areas.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2024

An Assessment of the Safeguards Implications of Particle and Alloy Formation in MSRs

Molten salt reactors (MSRs) present unique challenges for applying safeguards measures and differ significantly from traditional nuclear reactors. Although the special fissionable materials within MSRs principally exist as dissolved species within the fuel salt, key actinides of interest may also be converted to solid phases including alloys and precipitated oxides via chemical and electrochemical reactions. These solid-phase components will complicate the nuclear material accounting and control (NMAC) approaches that have, so far, primarily targeted measurements of the liquid salt itself. For example, most of the proposed monitoring and characterization methods for MSRs are reliant on homogeneity of the salt and the ability to maintain accountable materials in solution. Solid deposits and particulates could invalidate the assumption of homogeneity and necessitate the use of new models and measurement tools to permit a full accounting of all nuclear material in an MSR. To address this, the likelihood of solids formation in MSRs, estimated the rate at which these solids could form, and assessed the monitoring tools that are available to account for the presence of these materials were examined. Specifically, three solid forming mechanisms were investigated, including (1) the accumulation of actinides within the MSR’s structural materials due to alloying, (2) the accumulation of actinides within noble metal fission product particulates, and (3) the generation of actinide oxides from interactions with salt impurities. These modeling-informed studies were completed with considerations to both fluoride- and chloride-containing salts. It was determined that, although measurable amounts of special fissionable material were expected to alloy with the structural elements and fission products, the predicted amounts were below levels considered as significant quantities (SQ) by the International Atomic Energy Agency (IAEA). However, it was determined that sufficiently large oxygen concentrations could potentially lead to significant quantities of special fissionable material being converted to solid oxide phases. As such, a comparative study of technologies that are commercially available to assist in monitoring and accountancy of this material was presented. Policy implications, design recommendations, and suggestions for follow-on experimental work were also presented to further assist reactor vendors in designing and controlling the fuel salt chemistry to address potential safeguards considerations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2024

Survey of prospective techniques for molten salt reactor feed monitoring

Safeguards verification measurements of nuclear material content in fresh fuel salt for liquid-fueled molten salt reactors (MSRs) are likely to be required as part of nuclear material accountancy for International Atomic Energy Agency safeguards. Here, this paper presents a comprehensive review and evaluation of 18 potential candidate techniques to quantify total uranium and 235 U for input accountancy measurements for liquid-fueled MSRs. As part of an overall screening and down-selection effort to identify the most promising techniques for further development for an MSR feed monitoring system, this paper defines eight figures of merit (FOMs): reasonably achievable measurement uncertainty, measurement time required, capital cost, burden upon the facility operator, maintenance intensity, technological maturity, human capital requirements for operation, and whether the technique introduces a path for potential material removal. Each candidate technique is then evaluated across these FOMs to identify the techniques with the highest potential for future development for fresh fuel accountancy measurements in MSRs. Our findings indicate that no single technique or combination thereof currently has the requisite technological maturity for immediate implementation in nuclear material accountancy at a liquid-fueled MSR facility. While several promising techniques are identified, there is a critical lack of experimental data for most systems in the context of molten salt applications.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

New Capability at ORNL: High Precision Uranium Titration

Destructive analytical measurements establish a nuclear facility’s nuclear material inventory and inventory differences for Nuclear Material Accountancy and Control. A nuclear laboratory’s ability to perform accurate high-precision analytical measurements is key for tracking large inventories within a facility’s material balance areas and during production to track material movement through dynamic processes. For uranium, these measurements are made by using several established high-precision measurement protocols. These include isotope dilution mass spectrometry, gravimetry, and potentiometric titrations. Whatever measurement technique a nuclear lab chooses to use, reference materials (RMs) with certified attributes and accompanying uncertainties are used to calibrate measurement systems, and are the cornerstone for accurate results. In addition to calibration, RMs provide for metrological traceability, are used for method development and validation, and thus provide critical evaluations of the appropriateness and performance of analytical processes used. Evaluations may include validation that a method is fit-for-purpose, quantification of systematic and random biases, and the evaluation of long-term and short-term performance metrics. High-precision measurement techniques require that measured attributes be certified to a high degree of precision in the RMs used—ultimately, to a higher degree than that of the measurement technique itself. The US authority on the production of special nuclear material Certified Reference Materials is the NBL Program Office (NBLPO), formally known as New Brunswick Laboratory (NBL). The NBLPO is responsible for the sales and distribution of existing NBL certified reference materials (CRMs) and for the production of the next generation of nuclear RMs. To accomplish its mission, NBLPO is establishing key base capabilities within the DOE laboratory complex that formerly existed at the NBL laboratory. The Nuclear Analytical Chemistry (NAC) section within the Chemical Sciences Division (CSD) at Oak Ridge National Laboratory (ORNL) is currently working with NBLPO to set up laboratory and measurement capabilities to provide measurements and capabilities for production and/or recertification of existing and future CRMs for uranium assay. The NBL-developed high-precision titration (HPT) method is a critically-evaluated, extremely precise and accurate primary method utilized for the determination of uranium content in a variety of uranium materials. The HPT method, combined with detailed balance weighing protocols, provides for an analytical methodology that is unsurpassed in precision and one in which all sources of error have been evaluated, a requirement of CRM certification. HPT capability within the United States was lost with the closure of the labs at NBL. The NAC has been collaborating with NBLPO to stand up and demonstrate the capability to perform uranium assay via HPT at ORNL. HPT can produce results with an expanded uncertainty of approximately 0.01% for pure uranium compounds, with typical precisions of <0.006%. The major tasks required to stand up the method at ORNL were the refurbishment of a dedicated lab and equipment setup, procedure development, analyst training, establishing method-specific quality assurance, and qualification of an analyst to perform the method. This report summarizes these tasks, outlines the documents drafted, and gives the outcome of the qualification titrations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗