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Idaho National Laboratory Nuclear Fuel Cycle Separations Capabilities presentation for the Critical Minerals Town Hall 2023, December 1, 2023.
Idaho National Laboratory’s (INL) nuclear fuel cycle capabilities enable the deployment of technologies that sustain the current reactor fleet, support demonstration and deployment of new advanced reactors, and facilitate management and disposition of existing and future radiological waste materials. INL focuses on deploying nuclear energy systems with confidence by decreasing proliferation risk through research that demonstrates process transparency and supports safeguards and security by design. An example of these capabilities is the Beartooth test bed, set to begin operations toward the end of fiscal year 2026. Beartooth will include a cascade of centrifugal contactors, glove box lines, and solidification and dissolution equipment to aid in the progression of novel separation techniques and to provide hands-on experience to cultivate and maintain a robust workforce of experts. To support Beartooth’s enhanced instrumentation and monitoring equipment needs, several nontraditional sensors are being considered for future deployment. The non-traditional sensors include accelerometers, acoustic microphones, and infrared cameras. These nontraditional sensors have the potential to not only help monitor the process but also enhance nuclear safeguards.
Deployment of advanced nuclear reactors will inevitably introduce new challenges for devising and implementing an efficient, safe, and economical nuclear fuel cycle that meets society’s need for clean energy and expectations for environmental stewardship. The growing urgency for decarbonizing the US and global economies makes such technological challenges all the more compelling. The Office of Materials and Chemical Technologies within US Department of Energy’s Office of Nuclear Energy stewards the capabilities and knowledge relied upon by government policy makers to make informed decisions regarding nuclear fuel cycle options. Such decisions in turn rely on the development of efficient and economical separation methods that can accept the used nuclear fuel containing actinides and fission products (FPs) to recycle selected actinides, recover valuable by-products, and deliver waste streams that are suitable for disposal. To help guide the future direction of fuel cycle separations research, taking into account emerging technologies, the Office of Materials and Chemical Technologies sponsored the Innovative Separations R&D Needs for Advanced Fuel Cycles workshop, held virtually August 30–September 1, 2021. Based upon 60 contributed white papers, 6 plenary lectures, and 3 days of discussions, the outcome of the workshop and subsequent deliberations was the generation of this report identifying seven future research directions (FRDs) plus three crosscutting areas of research.
Reprocessing is an important step in the nuclear fuel cycle where usable nuclear materials are extracted from used fuel for recycling. The separation of materials for reuse simultaneously reduces not only the volume of nuclear waste, but its decay time to radioactivity levels similar to that of the originating uranium ore. As part of an initiative to steward research, development, and innovation into the nuclear fuel cycle, Idaho National Laboratory is designing and constructing a solvent extraction testbed named Beartooth. This testbed will allow researchers to refine separation processes, test innovative extraction processes, and give early career scientists opportunities to gain skills in performing separations chemistry utilizing centrifugal contactors. In addition, the Beartooth testbed is being uniquely designed to enable novel technologies including machine learning capabilities for the characterization of chemical process operations in near real-time. To aid in the design of Beartooth, a team of researchers are installing a variety of atypical sensors into a system of contactors for signal discovery. The team will implement machine learning methods on acquired sensor data to extract signal features. The goal is to provide a process operator with a deeper understanding of the chemical process and equipment usage. This work will summarize sensors utilized and preliminary results from an infrared camera.
Reprocessing is an important step in the nuclear fuel cycle where usable nuclear materials are extracted from spent fuel for recycling. The extraction of materials for reuse simultaneously reduces not only the volume of nuclear waste, but its decay time to radioactivity levels similar to that of the originating uranium ore. As part of an initiative to steward research, development, and innovation into the nuclear fuel cycle, Idaho National Laboratory is designing and constructing a solvent extraction testbed named Beartooth. Beartooth will allow researchers to refine extraction processes, test innovative extraction processes, and give early career scientists opportunities to gain skills in performing separations chemistry that uses centrifugal contactors. In addition, the Beartooth testbed is being uniquely designed to enable novel technologies including machine learning capabilities for the characterization of chemical process operations in near real-time. To aid in the design of Beartooth, a team of researchers are installing a variety of atypical sensors into a system of contactors for signal discovery. The team will implement machine learning methods on sensor data to determine signal features with the goal of providing a process operator with a deeper understanding of the chemical process and equipment usage. This work will summarize sensors utilized and preliminary results from an infrared camera.
The current need to rapidly and substantially expand clean power production combined with limited capability for domestic uranium enrichment results in a U.S. nuclear power production planning environment similar to that of the first nuclear era. The U.S. thermal-spectrum molten-salt breeder reactor (TS-MSBR) program emerged during the first nuclear era as means to support rapid nuclear power expansion while minimizing demand on fissile resources. The primary reasons that the TS-MSBR program was discontinued in the 1970s were the comparatively large amount of required effort to mature its technology sufficiently for commercial deployment and the access to separated fissile material provided by the design of its integrated fuel cycle. The slowdown in U.S. electrical load growth after 1980 and the abundance of inexpensive fossil fuels inhibited reconsideration of TS-MSBR development for decades. The purpose of this discussion is to re-examine the value and technical challenges of TS-MSBRs with integrated fuel salt chemical processing considering the renewed need for rapid expansion of clean energy production worldwide, the current state of technology, the challenge of actinide wastes, and the continuing need to maintain a high degree of proliferation resistance and to integrate safeguards into the design.
Idaho National Laboratory is designing and constructing a solvent extraction test bed, Beartooth, as part of a nuclear fuel cycle stewardship initiative. The test bed will provide facilities and equipment for testing novel extraction processes and give early career scientists opportunities to gain skills in performing separations chemistry. The test bed is being uniquely designed to enable machine learning capabilities for the characterization of chemical process operations. One of the intentions of incorporating machine learning methods is to provide process operators with enhanced situational awareness for the optimization of separations techniques and possible detection of a diversion event. As a result, the objective of this Laboratory Directed Research and Development project is to develop a multi-sensor data collections system and implement machine learning techniques on signals from an existing centrifugal contactor cascade to identify equipment usage and process events. This presentation will provide an overview of sensors used and experiments conducted to date.
The U.S. Department of Energy’s Nuclear Energy Advanced Modeling and Simulation program aims to develop predictive capabilities using computational methods for the analysis and design of advanced reactor and fuel cycle systems. This program has been supporting the development of BISON, a high-fidelity and high-resolution fuel performance tool at the engineering scale. Incorporation of more physics-based models in BISON for the accident tolerant fuel applications motivated this study. This document details integration of new modeling capabilities in BISON, including: a tensile strength model for uranium dioxide (UO 2 ) fuel to incorporate the microstructural effects (e.g., grain size, fabrication pore size, and porosity), and atomistic-informed creep model for UO 2 fuel that is developed by Los Alamos National Laboratory. Sensitivity analyses are conducted on these models separately as well as a two-dimensional full rod application under normal operating conditions. Lastly, these new modeling capabilities in BISON are exercised in Halden IFA-677.1 and IFA-716.1 assessment cases.
Nuclear reactor systems that use fuel dissolved in a liquid have the potential for enhanced safety characteristics, improved fuel-cycle outcomes, and more efficient isotope-production configurations. In these reactor systems, the fueled liquid may simultaneously undergo irradiation, physical and chemical removal processes, and fueling. The modeling and simulation of this transmutation and decay with material additions and removals is an ongoing research area. An accurate simulation tool is critical to the reactor and fuel-cycle design, reactor deployment, and source-term characterization for these advanced reactor systems. The work described herein involved implementing, testing, and applying the capability to perform reactor physics simulations within the Oak Ridge National Laboratory-developed SCALE suite for nuclear systems analyses and design, leveraging much of its pedigree in quality-assurance and reactor-analysis capabilities. The functionalities to simulate irradiation with material feeds and removals had been added in ORIGEN, and the TRITON reactor physics sequence was extended to calculate the total removed material and track external nonirradiated mixtures to estimate separate processing or waste streams. Results from these capabilities align with analytical expectations obtained from ORIGEN for simplified test cases and with expectations for a molten salt reactor application. This implementation, available with the SCALE 6.3 release, provides for a more efficient and accurate material accountability methodology, allowing for the characterization, design, and analysis of the complete isotopic material inventory of advanced liquid-fueled systems for a variety of applications.
Reprocessing of used nuclear fuel (UNF) results emits several volatile radionuclides that must be removed from the bulk off gas prior to release in order to meet U.S. regulatory emission requirements. After other volatile radionuclides have been removed, krypton (Kr) remains, along with associated with xenon (Xe) in the gas stream. The half-life of Xe is short enough that by the time UNF is sufficiently cooled to be reprocessed Xe is no longer a radiological concern and it may be release to atmosphere or collected for other purposes. Kr, however, must be placed in long term storage. In order to ensure the smallest practical volume for long term storage, the Xe, which is nearly ten times the volume of Kr, must be separated from the Kr. Although cryogenic distillation has been used successfully for this purpose, high capital and operational cost, along with safety considerations, made development of gas adsorption processes for separation of Xe and Kr attractive. INL developed an engineered form sorbent consisting of silver mordenite in a polyacrylonitrile matrix (AgZ-PAN) capable of complete separation of Xe from Kr in a single pass, allowing Kr to be captured downstream with no detectable Xe present.
Advancement in additively manufactured strain gauges help address critical technology gaps to accurately monitor real-time materials behavior in reactor experiments. This is critical as it provides data to inform predictive models and simulations that enhance the development of reactors and fuel cycle systems. In this report, additively manufactured strain gauges are exposed to a neutron irradiation environment at the Ohio State University Research Reactor. This report goes over a 2-week campaign for neutron irradiating printed resistive strain gauges and capacitive strain gauges. These results complement the prior separate effects (i.e., mechanical strain, temperature, etc.) testing that were performed on these additive manufactured sensors and presented in prior milestone reports. These results also help progress our understanding of their usage in harsh environment applications. The outcome of developing advanced sensing and instrumentation capabilities plays an important role in increasing the safety, reliability, and energy efficiency of both next-generation and existing nuclear reactors.
Solvent extraction is commonly used to separate different f-metals found in spent nuclear fuel, but this process results in large volumes of highly contaminated liquid waste that must be remediated or stored at significant expense. The project funded under this award was aimed at addressing solvent-related issues encountered in conventional f-metal separations. Our strategy focused on using solvent-free mechanochemical reactions to prepare lanthanide and actinide borohydride complexes so that they could be separated based on differences in their volatility. Key deliverables described in this report include proof-of-principle results demonstrating that borohydrides called aminodiboranates can be used for volatile lanthanide/lanthanide and lanthanide/uranium separations, as we proposed. Moreover, exploration of a closely related class of borohydrides called phosphinodiboranates allowed us to identify underlying chemical factors that control the volatility of trivalent lanthanide and uranium borohydride complexes with identical structures. Details of published and pending research products are provided, and these include comprehensive synthesis and characterization efforts required to support fundamental studies related to the proposed separations. These technical efforts supported the training of nine graduate students and three undergraduate researchers, and they established air-sensitive transuranic capabilities at the University of Iowa to enhance radiochemical workforce development
The INL Analytical Research Laboratories and the CNL Analytical Laboratories share many of the same capabilities and expertise while also overlapping significantly in mission. Where there are similarities and differences in the types of samples and analytical procedures between the two facilities, each laboratory can learn much from the other, and establish a technical baseline that may be mutually beneficial. An exchange of knowledge and exposure to the international laboratories benefits both organizations, and it is the purpose of the proposed visits to the two facilities to foster understanding and learning between the respective scientists. Topics of common interest include but are not limited to multi-collector ICP-MS; high resolution gas MS; alpha, beta, and gamma spectrometry; and separations chemistry of nuclear materials. By sharing expertise, the INL and CNL Analytical Laboratories will improve their analyses providing more reliable results and capabilities that are competitive with other world-class facilities.
The future of nuclear power utilization in the United States may involve a transition from the once-through light water reactor fuel cycle to a so-called advanced fuel cycle. An advanced fuel cycle may offer improvements in natural resource utilization, reactor safety, and environmental impact. In addition, adoption of an advanced fuel cycle will result in changes in the amount, composition, and disposal of the nuclear wastes they produce. Characteristics intrinsic to the wastes themselves, such as mass and radioactivity at specific times, were used as waste management metrics in the Department of Energy 2014 Fuel Cycle Evaluation and Screening (FCES) study. Binning of these metrics informed fuel cycle according to relative potential benefit. However, waste properties alone cannot qualify management strategy. Therefore, comparing fuel cycles from the perspective of waste management can provide additional insights. To that end, an object-oriented Python package has been developed to perform fuel cycle waste management calculations. The package, named nwpy (short for Nuclear Waste analysis in Python), mimics the mass flow operations reported in the FCES study and interfaces with the ORIGEN-S code to assess metric data as reported in the FCES. In addition, this Python package determines the loading of waste streams into forms suitable for final disposal in a geological repository and uses such data for repository performance assessment. This work describes the Python package methodology, assumptions, and capabilities. As input data, the package requires information about the fuel cycle such as the mass of fuel discharged, the cooling time between reactor discharge and subsequent operations, and the separations process efficiencies and waste forms it produces. In addition, the isotopic composition of the reactor discharge stream, such as that available from the FCES database, is required. With that, it can perform prescribed mass flow and decay operations throughout the back end of the fuel cycle, the latter carried out by the ORIGEN-S code distributed with the SCALE6.2 software suite. The result is time-dependent data characterizing the waste on a per-package basis. Package loading for waste streams depends on the stream form (i.e. UNF vs. HLW, or glass HLW from aqueous reprocessing vs. ceramic HLW from electrochemical processing) and is based on literature review and engineering assumption. As an example of the application of the code, calculations for the areal footprint of direct-contact repositories for different fuel cycles is shown. Development is ongoing, and the package is expected to grow incorporating capabilities for waste management analyses such as waste transportation and radionuclide transport through the biosphere. (authors)
This document presents the test plan for the AGR-5/6/7 irradiation experiment, the combined fifth, sixth, and seventh irradiations of the United States Department of Energy Advanced Gas Reactor (AGR) Fuel Development and Qualification Program. The combined irradiation tests will consist of fuel qualification tests (AGR-5/6) and a margin test (AGR-7) for the industrially produced uranium oxycarbide (UCO) tristructural isotropic (TRISO) coated particle fuel developed by the AGR Program. The objective of the AGR-5/6/7 irradiation experiment is to establish the performance of UCO TRISO fuel fabricated using engineering-scale equipment in a production environment under and beyond normal operating conditions. Specifically, the goals of the AGR 5/6/7 irradiation experiment are: 1. Irradiate reference design fuel containing low-enriched UCO TRISO fuel particles to support fuel qualification. 2. Establish the operating margins for the fuel beyond normal operating conditions. 3. Provide irradiated fuel performance data and irradiated fuel samples for post-irradiation examination and safety testing. 4. Support the refinement of fuel performance and fission product transport models with online, post-irradiation examination and safety test data. In order to achieve the test objectives, the AGR-5/6/7 experiment will be irradiated in the northeast flux trap position of the Advanced Test Reactor at Idaho National Laboratory. The larger diameter of the northeast flux trap provides greater flexibility for test train design, significantly enhancing the capability for the combined irradiations. The test train contains five separate and independently controlled and monitored capsules. The middle capsule contains the AGR 7 margin test fuel. The two bottom and two top capsules contain the AGR 5/6 fuel. Each capsule contains a variable number of fuel compacts filled with UCO TRISO particles.
Vibroacoustic monitoring was investigated to aid in informing process operators with parameters regarding aqueous separation techniques. These techniques have a wide range of applications including nuclear fuel reprocessing. A small-scale solvent extraction system was set up with five magnetic drive contactors and two piston pumps to collect realistic operation. Vibration sensors were placed on three of the contactors and both pumps, and a microphone was placed near the system. Contactor rotational speed and pump flow rate were varied with known values to compare against measured vibroacoustic signatures. Spectral analysis allowed for the determination of contactor rotational speed and the ratio of organic to aqueous flow rate, an important parameter for ensuring optimal extraction. Vibration metrics such as kurtosis and crest factor provided additional details regarding individual rotational speeds and have potential in examination of faults for predictive maintenance. Overall, results indicate the capability of vibroacoustic monitoring to improve operator awareness and process outcomes.
The effect of electronic structure on chemical bonding and reactivity is one of the most important questions in the field of chemistry. Insight into chemical bond formation involving elements that contain f electrons (i.e., the lanthanides and actinides) is critical for solving specific technical challenges, such as development of advanced nuclear fuel cycles and efficient rare earth separations, as well as a broader understanding of bonding across the entire periodic table. The primary technique for studying the fundamentals of lanthanide and actinide bonding is crystallization of metal-ligand compounds followed by structural determination with X-rays and comparison to theory with computational chemistry. While this procedure has yielded significant insights for a wide variety of elements, it is challenging to apply to the heavier trans-uranic actinides such as berkelium and californium because of limited material availability, significant radioactivity, and poorly understood chemical reactivity of these elements. We hypothesize that by forming actinide-ligand clusters in a mass spectrometer and probing their reactivity in the gas-phase, many of the challenges associated with studying the heavier trans-uranic elements can be circumvented. This project will develop a capability to address a wide range of actinide bonding and reactivity phenomena, increasing Idaho National Laboratory’s capability to address fundamental questions at the forefront of heavy element chemical and molecular science.
Since 2017, Oak Ridge National Laboratory (ORNL) has been developing a passive fast-neutron emission tomography capability. The goal of this development is the ability to quantify the neutron source strength of individual fuel pins (rods) in spent nuclear fuel assemblies. Such a system could be used to measure the burnup of each fuel pin in a spent fuel assembly to take burnup credit when loading dry storage casks or to count individual fuel pins in spent fuel assemblies for safeguards purposes. At present, a laboratory prototype imager has been built and initial imaging measurements performed. The purpose of this prototype is to demonstrate imaging capability sufficient to resolve individual fuel pins in spent fuel assemblies, and in initial measurements, neutron sources separated by a spacing of 1.27 cm (similar to the spacing between fuel pins in commercial pressurized water reactor 17×17 nuclear fuel assemblies) have been resolved. This report documents the as-built imager, first measurements performed with it, and tomographic reconstructions performed using the measured data.