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Historic and modern nuclear graphite impurities: Pathways to improved waste strategies

Graphite has been used in large volumes as a structural material and neutron moderator since the earliest days of nuclear fission. However, no international consensus exists on the disposal of irradiated graphite, leaving much of the historic radioactive graphite inventory in interim vault or silo storage. With several new graphite-moderated reactors planned or under construction, the issue of graphite waste management is becoming increasingly urgent. This paper reviews and quantifies impurities in both historic and modern nuclear graphite, with emphasis on nitrogen—responsible for much of the 14 C inventory—and chlorine, which plays a critical role in repository performance and design. Modern graphites, benefitting from stringent quality-control measures developed for non-nuclear industries, meet or exceed the ASTM Ultra-High Purity nuclear standards, even without halide purification. Both chlorine and nitrogen concentrations have declined over time. For chlorine, identified as a key impurity influencing U.S. waste repository design, we propose a target of 0.1 appm in as-fabricated billets as a reasonable benchmark. Nitrogen sources are traced throughout the graphite production process, with surface and bulk concentrations characterized for all materials studied. Modern graphites commonly exhibit nitrogen levels below 5 appm, with values approaching 1 appm achievable. Using such reduced-nitrogen grades is critical to keeping graphite-induced radioactivity below the greater-than-Class-C waste threshold, thereby avoiding disposal cost penalties of nearly an order of magnitude.

Chlorine↗

Microbial potentiometric sensor technology for real-time detecting and monitoring of toxic metals in aquatic matrices

Considering that toxic metals can affect metabolic processes in microorganisms adversely, it can be hypothesized that these metals in water matrices would induce a decrease in metabolic activity of the biofilm microorganisms populating the surface of a sensing electrode, which could be registered as a change in the open-circuit potential (OCP) generated by the biofilm microorganisms. The goal of this study was to test this hypothesis and demonstrate the underlying principle that microbial potentiometric sensor (MPS) technology could be used for long-term and real-time monitoring and detection of rapid changes in metal concentrations in realistic aquatic environments. To address the goal, four objective were addressed: (1) a batch reactor with three graphite-based MPS electrodes was fabricated; (2) a set of single-ion solutions and one multiple ion solution were prepared reflecting realistic concentrations of metals found in electroplating wastewaters; (3) the responses of the MPS to the simultaneous presence of multiple toxic metal ions in a single solution were measured; and (4) the changes of the MPS signals to the presence of individual metal ion solutions were examined. While the hypothesis was validated, the study also revealed that the MPS was sufficiently sensitive to not only detect, but also quantify, toxic metal ion concentrations in aqueous solutions. The coefficients of determination, which were R 2 > 0.995, and responsiveness of <1 μmol/L for some toxic metal cations, strongly support the performance of MPS technology in the echelons of expensive analytical tools capable detecting and measuring trace elements.The magnitude of the MPS response was toxic metal specific. When the molar concertation normalizes the inhibition portion of the signal area, the assessed sensitivity order was: Se>Cd>Pb>Ag>Ni> Zn. The study provides valuable information for enforcement agents, environmental professionals, and wastewater treatment operators, so toxic metal pollution and its detrimental impacts can be prevented and mitigated.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molten Salt Reactor Signatures and Modeling Study

Molten salt reactor (MSR) technologies, either liquid fueled and cooled or only liquid cooled, pose specific, unique challenges for safeguards of the special nuclear material during the operation, fueling, and maintenance of the reactor. MSRs are one type of Generation IV technologies being invested in and considered for U.S. domestic fabrication primarily for electricity and process heat production. These designs have generated growing commercial interest for several reasons, including high (≈40%) thermal efficiency, ease of fueling, improved use of uranium fuel, potential utilization of thorium fuel, and proposed inherent safety features. U.S. companies have several planned designs that differ in fuel, cooling, and neutron energy spectrum. Driven by commercial interest and the intent of licensing MSRs, the U.S. Nuclear Regulatory Commission (NRC) has developed a vision and strategy to accommodate non-light water reactors (LWR), which include MSRs (U.S. Nuclear Regulatory Commission 2019). In addition, the Department of Energy (DOE) through the Office of Nuclear Energy (NE) Office of Advanced Reactor Technologies (ART), …sponsors research, development and deployment (RD&D) activities through its Next Generation Nuclear Plant (NGNP), Advanced Reactor Concepts (ARC), and Advanced Small Modular Reactor (aSMR) programs to promote safety, technical, economical, and environmental advancements of innovative Generation IV nuclear energy technologies. Reactor types considering the use of salts, liquid metals, or gases for coolant fall under both ARC and aSMR. Therefore, Research Design & Development is being pursued by DOE-NE through national laboratories, universities, and international and industrial collaborations. Additionally, the U.S. is a member of the Gen IV International Forum (GIF). The GIF is a cooperative, multinational organization to guide and carry out research and development needed for the GEN IV reactor systems (Forum 2018). GIF evaluated numerous reactor concepts and down-selected to the six most feasible advanced reactor technologies: gas-cooled fast reactor (GFR), lead-cooled fast reactor (LFR), MSR, supercritical watercooled reactor (SCWR), sodium-cooled fast reactor (SFR), and very high temperature reactor (VHTR). In support of the growing interest domestically and internationally, the Materials Protection, Accounting, and Control Technologies (MPACT) campaign, under the DOE-NE Fuel Cycle Technologies (FCT) program, engages in R&D activities by developing advanced instrumentation and analysis for safeguards and security of modern, advanced nuclear fuel cycle (non-LWR) facilities. Because of the historic experience in the operation of the Aircraft Reactor Experiment (ARE) and the Molten Salt Reactor Experiment (MSRE) (Robertson, MSRE Design and Operations Report Part I 1965), Oak Ridge National Laboratory (ORNL) is heavily engaged in the various R&D activities through the DOE complex related to MSRs including national technical leadership of the DOE-NE MSR campaign. This report discusses and presents the outcomes of the FY19 MPACT MSR Safeguards task. The challenges presented by MSRs for nuclear material accountancy and control (NMAC) and associated safeguards will be investigated. The objective of this research is to explore and compile the safeguards requirements and identify measurement signatures through an initial high-level MSR design and develop complementary advanced simulation and modeling capabilities. A high-level ORNL-developed MSR design called the Molten Salt Demonstration Reactor (MSDR) (Bettis, Alexander and Watts 1972) was used as the target reactor design for this research. The MSDR model incorporates technology from the MSRE and the Molten Salt Breeder Reactor (Robertson, Conceptual Design of a Single-Fluid Molten-Salt Breeder Reactor 1971). But the MSDR is a 750 MWth graphite moderated liquid fueled (low-enriched uranium) MSR compared to the MSRE’s of 7.5 MWth. The focus of this report is to discuss the evaluation of novel signatures, correlations, and indicators to understand the applicability of current safeguards instrumentation to MSRs using the modeling results from the MSDR.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Kinetics and transport of hydrogen in graphite at high temperature and the effects of oxidation, irradiation and isotopics

The kinetics of uptake and desorption impact the performance of graphite as a vector for tritium in high-temperature fission reactors and in the blanket of fusion reactors. Graphite components in these reactors are exposed to temperatures > 500 °C and H 2 partial pressures of few Pa and desorption temperatures are limited to < 1600 °C; limited data is available at these conditions. Here we review the mechanisms for uptake in, transport and desorption of hydrogen from graphite at high temperature, compiling data on uptake rates, diffusion coefficients and activation energies and providing a discussion of the impact of irradiation, pre-oxidation and isotope. At FHR conditions, trapping impacts uptake rates, leading to a reduction in apparent diffusivity by 35 to 80% compared to higher partial-pressure uptake. Timelines for desorption are not clearly defined; extrapolating from available data, at 1150 °C desorbing 80% of tritium uptaken at FHR conditions may take from 100 to 10,000 h.

36 MATERIALS SCIENCE↗

"Source Term Modeling for Advanced Gas Micro-Reactors"

Maintaining the safety of the public, environment, and operating personnel is the most important factor in designing, operating, maintaining, and decommissioning nuclear reactors. In recent years, there has been a growing interest in the development of micro-reactors employing TRi-structural ISOtropic (TRISO)-coated particle fuel. In gas reactors, TRISO fuel plays an important role in the safety case for high temperature reactors because of the fission product retention properties of the fuel. This ability enables the use of a functional containment strategy for the reactor where multiple barriers are used to prevent fission product release to the environment. Part of the safety analysis of these advanced reactors is the assessment of radionuclide releases under normal and accident conditions through the multiple credited safety barriers. Using conservative assumptions, a mechanistic analysis can be performed to quantify these releases that combines the probabilistic assessment of failure with analytic solutions to radionuclide transport equations. Source term modeling for TRISO fuel has been performed for previous reactor designs; however, these models are outdated, in many cases proprietary, and need updates to be applied to the current state of TRISO fuel technology and alternative gas reactor core configurations [1]. Currently, the only publicly available source term assessment for gas reactors is an expert-based Monte Carlo simulation based on the effectiveness of the fuel kernel, coating layers, and graphite block in a modular high temperature gas reactor [2]. Thus, there is a need to develop a simple, versatile, and mechanistic model of fission product release and transport in gas reactor cores that could be applied to a variety of reactors through user inputs and reactor-specific radionuclide inventories. The release is calculated by the diffusion of the key safety important fission products through the kernel, silicon carbide (SiC), graphite for both intact and defective TRISO particles based on fuel and graphite temperatures in the reactor under normal operation. These releases from the fuel enter the coolant where they can plate-out on cooler surfaces. A clean-up model is included for designs with a coolant purification system to remove fission gases. This initial distribution of fission products in the reactor serves as an initial condition for potential releases under postulated accident conditions. The model then can calculate the fission product release for any transient temperature profile and fission product releases can then be used to assess radiological dose to the workers and the public using conventional dose tools. Data on the diffusion of fission products is based on historic German TRISO experiments and the more current Department of Energy (DOE) Advanced Gas Reactor (AGR) TRISO fuel development program. The model is coded in python with inputs and outputs in excel spreadsheets, as well as python plotting utilities to aid in the interpretation of the results. References: [1] INL, NGNP Mechanistic Source Term White Paper, INL-10-17997, July 2010. [2] David A. Petti, Richard R. Hobbins, Peter Lowry, Hans Gougar, “Representative Source Terms and The Influence of Reactor Attributes on Functional Containment in Modular High Temperature Gas-cooled Reactors,” Nuclear Technology, Vol. 184, p. 181-197, Nov. 2013.

07 ISOTOPE AND RADIATION SOURCES↗

Identify and Assess Technical Challenges in Safeguards Measurements of Spent Advanced Reactor Fuels

Advanced reactor (AR) designs use various nuclear fuel types that can be significantly different than conventional light-water reactor (LWR) fuels, including differences in sizes, compositions, and chemical forms (e.g., oxide, carbide, metal). Nearly all the proposed AR fuels use high-assay low-enriched uranium (HALEU), which will have higher enrichments (5–20 wt% 235 U) than LWR fuels (currently limited to <5 wt% 235 U). In advance of the wide use of these new fuel types around the world, international safeguards organizations such as the International Atomic Energy Agency (IAEA]) are working with some of the AR vendors to formulate safeguards approaches for these AR fuel cycles. As part of the overall safeguards approach, it is important to identify the potential technical challenges in performing safeguards verification measurements of these AR fuels (both fresh and spent fuels) in advance of the widespread adoption of these new fuel types, because new safeguards technologies can take several years to develop, test, and approve for use. This report documents work performed in fiscal year 2024 based on modeling and simulation to assess the performance of the existing safeguards measurement technologies for irradiated or spent AR fuel elements or items. This work is a continuation of the work performed in fiscal year 2023 that focused on fresh AR fuels. Spent AR fuels have a distinct difference from their LWR counterparts: unlike the spent LWR fuels typically stored in a water-filled pool, some spent AR fuels—such as tristructural-isotropic (TRISO)-based fuels—will most likely be stored in air-filled hot cells. Because most safeguards measurements on spent fuel performed to date have been conducted under water, the air-filled hot cell environment could present unique challenges to safeguards measurements. Fork detector (FDET) and Cerenkov viewing device (CVD) systems have been the two primary instruments used by the IAEA for several decades to measure spent LWR fuel assemblies stored in pools for safeguards verification purposes. Because the lower refractive index of air causes Cerenkov light to be of lower intensity in air than in water, existing CVDs are likely unable to perform safeguards verification measurements for spent fuel stored in an air-filled hot cell, as is the case for the TRISO-based spent fuel elements (e.g., pebbles, graphite fuel blocks). Unlike FDET measurements, CVD measurements do not require fuel be moved, so they are a simpler and faster to take than FDET measurements. The inability to perform CVD measurements on the TRISO-based AR fuel types presents a major technical challenge in the effort to use existing technology to perform safeguards measurements on spent AR fuels. This study was mainly conducted through the modeling and simulation of an FDET or an FDET-like system on five spent AR fuel types, including one metallic fuel type and four TRISO-based fuel types in both pebble and graphite block forms in their respective storage configurations and environments. Because the various AR fuel types have significantly different dimensions, FDET systems must be adapted to accommodate them. Partial defect tests were also simulated in this study to assess the FDET’s ability to detect potential fuel diversions. The FDET measures the fuel’s total passive neutron and gamma emissions. The simulated FDET results from spent AR fuel items are compared against results from a typical spent pressurized water reactor (PWR) assembly. High-purity germanium (HPGe) gamma detector measurements were also simulated for the spent AR fuel types and the PWR assembly because the signature photopeaks have been used in LWR safeguards verifications, although HPGe is usually not used to detect diversions because of the fuel’s self-attenuation effects on those photopeaks. The results indicate that these detectors have significant challenges in performing safeguards measurements of the spent AR fuel items, including incompatibilities between AR fuel items and existing FDETs, lower neutron count rates, lower sensitivities to fuel diversions in certain AR fuel items, and significantly higher interference from a neighboring fuel item when the measurement is performed in air. These results suggest that an alternative technology or significant and timely technology development is needed to perform adequate safeguards measurements of some of these AR fuel items.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

2023 Critical Materials Strategy

The global effort to curb carbon emissions is accelerating demand for clean energy technologies and the materials they rely on. Demand for these materials will only continue to grow, especially as some nations aim to achieve net zero emissions by 2050. While some major materials like steel, copper, and aluminum are already powering the fossil fuel economy, others are more minor materials with potential supply risks. These risks could jeopardize the ability to reduce greenhouse gas emissions within the desirable timeframe to avoid significant climate change. In some cases, it may be necessary to take action to improve the resilience of material supply chains and mitigate supply risks. Understanding the importance of individual materials to clean energy and the supply risks associated with them is necessary to identify which materials may serve as potential roadblocks to a clean energy future. The U.S. Department of Energy (DOE) issued a series of 13 supply chain deep dive assessment reports on various energy technologies in 2022 in response to President Biden’s Executive Order on America’s Supply Chains (E.O. 14017). These reports emphasized that supply chain bottlenecks can occur at any stage of the value chain from mining and refining to component and even sub-system manufacturing. The bottlenecks are a combination of factors such as material availability, equipment availability, work force availability and quality, logistics, regulatory framework, and market conditions. These bottlenecks were worsened during the global Covid-19 pandemic. Its lingering impacts have hindered capacity expansion for material supply chains and prevented product lead-time recovery. One approach to reduce supply chain risks for the United States is to have a strong domestic manufacturing sector with a diverse set of producers. Boosting responsible domestic production would require leveraging the latest science not only in material extraction but also in developing substitutes, recycling, reuse, and remanufacturing. This report is an updated analysis of previous Critical Materials Strategy (CMS) reports published by the DOE in 2010, 2011, and 2019 based on national and global priorities, technology advancement, and technology adoption trends. Like the CMS reports, this analysis presents the results of a formal material criticality assessment to identify which materials are critical to the continued deployment of clean energy technologies globally. The analysis in this report leveraged the DOE supply chain deep dive assessments to develop the initial list of materials to evaluate. This DOE Critical Materials Assessment (CMA) is conducted independently of criticality assessments performed by other U.S. government agencies, such as that conducted by the U.S. Geological Survey (USGS). This analysis complements the USGS critical minerals determination in three aspects. First, the DOE assessment is performed from a global perspective, while the USGS analysis focusses on the importance of minerals to the U.S. economy. Second, this report focuses on the importance of materials to clean energy technologies, rather than to the economy in general. Lastly, this study is forward looking to 2035 based on clean energy deployment scenarios, whereas the USGS assessment is retrospective. Materials evaluated in this report that do not appear in the USGS Critical Minerals List include copper, uranium, electrical steel, and SiC. A draft version of this report received ~80 public comments related to supporting data and methodological improvement. Those comments have been incorporated as much as possible where appropriate. Highlights of findings from this 2023 CMA include: Rare earth materials (neodymium, praseodymium, dysprosium, and terbium) used in magnets in electric vehicle (EV) motors and wind turbine generators continue to be critical. While dysprosium (Dy) and terbium (Tb) are both heavy rare earth elements that serve the same function in magnets, the criticality of Tb is slightly lower than that for Dy in the short term due to the widespread use of Dy in high-grade magnets and Tb’s present role as a substitute. Similarly, praseodymium (Pr) is critical in the medium term but only near critical in the short term because it is more substitutable in magnets than neodymium (Nd); Materials used in batteries for EVs and stationary storage are now considered to be critical. While cobalt (Co) was found to be critical in this and previous reports, lithium (Li) becomes critical in the medium term due to its broader use in various battery chemistries and the rampant growth of the EV industry. Natural graphite is a new addition in this assessment and is also found to be critical; Platinum group metals used in hydrogen electrolyzers, such as platinum (Pr) and iridium (Ir), are critical due to an increased focus on hydrogen technologies to achieve net zero carbon emissions, while those used in catalytic converters, such as rhodium (Rh) and palladium (Pd), were screened out due to the decreased importance of catalytic converters in the medium term; Gallium (Ga) continues to be critical due to its use in light-emitting diodes (LEDs). In addition, the use of Ga has increased in magnet manufacturing and in semiconductor in forms such as gallium arsenide (GaAs) or gallium nitride (GaN); Major materials like Aluminum (Al), copper (Cu), nickel (Ni), and silicon (Si) move from noncritical in the short term to near critical in the medium term due to their importance in electrification; Electrical steel is near critical due to its use in transformers for the grid and electric motors in EVs.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Characterization of ultrafast-laser ablation of micro-structures in Li-ion battery anode and cathode materials: Morphology, rate, and efficiency

Characterization of the rate and quality of ultrafast-laser ablation of Li-ion battery (LIB) electrode materials is presented for a collection of common and next-generation electrodes. Laser ablated micro-structures on the surface of LIB electrodes have been shown to provide dramatic enhancement of high-rate capability and electrode wetting. However, industrial adoption is hampered by a lack of data enabling informed choice of laser parameters and predicting process throughput. Here this work bridges this gap by providing characterization of the ablation process at more laser parameters (laser fluence and number of pulses used) than are currently available in the literature. Further, we expand on previous graphite and lithium iron phosphate (LFP) ablation work by extending ablation characterization to new LIB materials, providing high data resolution and adopting new characterization metrics which are relevant for industrial application of this technology. Ablated pores are characterized by their ablated depth, volume, and how the depth and volume ablation rate changes as a function of pore depth. Finally, we provide a detailed characterization of the morphology of laser ablated micro-structures which informs how material and laser parameters affect the quality of laser-processed electrodes.

25 ENERGY STORAGE↗

Toward model-free temperature diagnostics of warm dense matter from multiple scattering angles

Warm dense matter plays an important role in astrophysical objects and technological applications, but the rigorous diagnostics of corresponding experiments is notoriously difficult. In this work, we present a model-free analysis of x-ray Thomson scattering (XRTS) measurements on isochorically heated graphite obtained at the Linac Coherent Light Source at multiple scattering angles. We demonstrate that the recent imaginary-time thermometry technique works for scattering data that have been measured in both forward and backward scattering geometry. This opens up the way toward a rigorous quantification of nonequilibrium effects in future experiments, where XRTS measurements are being obtained from multiple scattering angles from the same sample.

Equations of state↗

Protein engineering for critical metal recovery beyond REEs

Achieving decarbonization and electrification goals will require expanded production of critical minerals (CM), including Li, Co, Cu, rare earths, Ni, and graphite, whose supply chains are geopolitically vulnerable. Problematically, current extraction and separation processes pose severe environmental burdens that impede the development of a diversified domestic supply chain and undercut the environmental benefits of energy technologies [1, 2]. The development of efficient, economical, and environmentally sustainable processing technologies is thus important for meeting the CM demand of the emerging energy technology market. To this end, we have recently developed an all-aqueous protein-based process for rare earth element (REE) extraction and separation. To extend our protein-based approach to critical metals beyond REEs, the goal of this project was to develop a protein discovery and engineering pipeline to generate a panel of proteins that selectively bind target critical metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Synthesis of LiNiO 2 at Moderate Oxygen Pressure and Long-Term Cyclability in Lithium-Ion Full Cells

The widespread adoption of electric vehicles necessitates higher-energy-density and longer-life cathode materials for Li-ion batteries. LiNiO 2 offers a higher energy density at a lower cost than other high-Ni-content cathodes containing additional transition-metal ions. However, detrimental phase transformations and impedance growth, resulting from structural defects formed during synthesis, lead to poor cyclability and limit the practical viability of LiNiO 2 . Herein, we demonstrate a considerably improved cycle life for LiNiO 2 by synthesizing it under a pressurized oxygen environment. The capacity retention in pouch-type full cells with a graphite anode after 1000 cycles is increased from 59 to 76% by applying a mere 1.7 atm of oxygen pressure during the synthesis of LiNiO 2 . With iodometric titration and inductively coupled plasma optical emission spectroscopy analysis, we provide clear evidence that oxygen pressure during synthesis reduces the occurrence of lattice oxygen vacancies and increases the content of Ni 3+ in LiNiO 2 , improving its structural integrity and cyclability. Post-mortem analysis of the cycled cathodes provides insights into the sources of degradation occurring during long-term cycling. Here, this work demonstrates a practically viable, synthetic approach combined with doping and coating to achieve improved performance with high-Ni layered oxide materials. Furthermore, this work represents the first report of extended cycling of LiNiO 2 in pouch full cells with graphite anode and will, therefore, serves as an important benchmark for future research on LiNiO 2 .

25 ENERGY STORAGE↗

Graphite waste classification and disposal cost estimation for high temperature gas and salt reactors

As high-temperature reactor designs progress to demonstration, managing the radioactive wastes from these systems presents unique challenges. This work explores the irradiated graphite source term produced by three reactor designs: The Modular High Temperature Gas reactor (MHTGR), a pebble-bed High Temperature Gas Reactor (pb-HTGR), and a Fluoride-cooled High-temperature Reactor (FHR). We predicted a C-14 concentration of 4.3 Ci/m 3 for the MHTGR, 1.2 Ci/m 3 for the pebble bed HTGR, and 2.5 Ci/m 3 for the gFHR after 20 years of operation. The final C-14 concentration highly depended on the graphite nitrogen impurity, a major precursor for C-14. The C-14 concentration in all reactor types exceeded the 0.8 Ci/m3 threshold, resulting in a Class C waste classification. The costs associated with accepting the graphite after 20 years in a low-level waste disposal facility were projected to be 255 dollars per kWe for the MHTGR, 248 dollars per kWe for the pb-HTGR, and 56.8 dollars per kWe for the FHR.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Generation IV Benchmarking of TRISO Fuel Performance Models Under Accident Conditions Final Report

The Generation IV International Forum (GIF) is a co-operative international endeavor of fourteen members organized to carry out the research and development needed to establish the feasibility and performance capabilities of the next generation nuclear energy systems. GIF selected six reactor technologies, amongst which is the Very High Temperature Reactor (VHTR) that is primarily dedicated to the cogeneration of electricity and hydrogen. The technical basis for VHTR is the tristructural isotropic (TRISO)-coated particle fuel, the graphite as the core structure, helium coolant, as well as the dedicated core layout and lower power density to removal decay heat in a natural way. At the heart of safety features of the VHTR concept lie the TRISO fuel particles that are designed to keep their structural integrity and retain fission products at temperatures up to 1600°C. As part as the design and future operation of VHTRs, a key aspect is the accurate prediction of fuel performance under irradiation and accident conditions. Modeling and simulation allow prediction of TRISO fuel behavior when subject to neutron flux and in high temperature accident scenarios. The refinement of the fuel performance models and codes is performed by comparison to in-pile and out-of-pile experimental data that reproduce the expected irradiation conditions in high temperature gas-cooled reactors (HTGRs). Historically, the International Atomic Energy Agency (IAEA) developed a benchmark dedicated to the validation of predictive methods for fuel and fission product behavior through the Coordinated Research Program CRP-2 (IAEA, 1997). CRP-2 was later updated to cover fuel fabrication, quality assurance, irradiation performance, safety testing, and spent fuel. The scope of the resulting CRP-6 benchmarks focused on HTGR fuel performance and fission product release (IAEA, 2012). Taking advantage of additional TRISO fuel fabrication, irradiation, and safety testing campaigns, GIF launched a Generation IV Benchmarking of TRISO Fuel Performance Models under Accident Conditions in late 2015. This GIF benchmark is a three-year program steered by Idaho National Laboratory (INL, USA). The other participants include the Japan Atomic Energy Agency (JAEA, Japan) and the Korea Atomic Energy Research Institute (KAERI, Korea). The objectives of the benchmark are to: follow on the IAEA CRP benchmarks, (2) model fission product release under accident conditions, (3) compare results obtained by the fuel performance modeling codes of the benchmark participants, and (4) compare these code predictions to experimental data. Safety tests chosen for modeling include the first and second experiments of the Advanced Gas Reactor program (AGR-1 and AGR-2) and the High Flux Reactor (HFR) EU1bis experiment. This report presents the results obtained by the three research institutions using their respective fuel performance modeling codes. Comparisons of the corresponding fission product release predictions are made with experimental data from AGR-1, AGR-2, and HFR-EU1bis. The benchmark results show good agreements between all participants but also show a general trend of over-prediction of the experimental release data, which is mainly attributed to the use of over-estimated diffusion coefficients.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Advanced Reactor Supply Chain Assessment (GAIN Report)

Several net-zero scenario evaluations predict a rapid ramp up of nuclear energy in the coming decades. If this materializes, it will most likely strain the supply chains associated with the potential advanced reactor concepts awaiting deployment. To help assess the current and potential capacities of the various advanced reactor supply chains, the Gateway for Accelerated Innovation in Nuclear (GAIN) conducted a survey of companies able to produce components for advanced reactors in the near future (namely for sodium, gas-cooled, and molten salt reactors). Using an aggressive nuclear deployment scenario, the objective was to assess the ability of the various supply chains to meet the considerable demand projections for certain key components (vessels, heat exchangers, pumps, graphite, and sensors) and identify potential challenges. While individual companies were unable to meet the most optimistic nuclear deployment rate projections, it was found that on aggregate, a United States-based supply chain projected that expansion could be ramped up to meet a larger future demand of these components. However, meeting projected demand for several more complex items (namely gas or salt heat exchangers) was found to be more challenging. Deploying new reactors at scale necessitates the production of more and more supply chain components, requiring a ramp up in production. Supply chain companies were surveyed, and respondents appeared less able to meet short term demand (next year) versus longer-term demand projections (5 and 10 years). This reflects the need to obtain orders with adequate lead times (can range from 3 to 30 months). Future demand will need to be met by expanding existing capacity. These expansions will require suppliers to raise capital or secure other types of support (federal loans or grants) to invest in facilities, equipment, and workforce. Individual suppliers indicated financial investments could be in the range of $\$ $100 million to $\$ $1 billion for their own facilities (depending on the type of facility). The biggest risk, according to respondents, related to general uncertainties surrounding the future nuclear industry and whether the potential demand projections will materialize into real demand that is actionable from a business perspective. Businesses do not seem willing to take investments risks without clear orders. If businesses are not able to invest to expand the supply, it will either delay the deployment of advanced nuclear technology, or the supply chain will be met by suppliers outside of the United States. This report only focuses on the domestic supply chain’s ability to meet the various projections stipulated here for the specific assessed components (vessels, heat exchangers, pumps, graphite, and sensors). The report does not cover all reactor designs or all components that may ultimately be needed for any one reactor design. It also does not address whether any specific aspect of the supply chain will be cost competitive in the global market, nor how potential state-backed entities could affect the expansion of a United States-based supply chain. The largest challenges in ramping up capacity among respondents appear to be workforce related. This includes workforce availability, experience, training, and turnover. In addition to facility investment, suppliers will also need to invest heavily in long-term workforce training to meet production goals. This issue is not nuclear-specific, and the expansion of any supply chain will likely face similar challenges. While suppliers evaluated expected normal business demand from other markets outside of nuclear, it is possible that other market segments could expand more than predicted and compete for the same suppliers. One potential market that may compete for the same supplier resources is the United States military, as many of these suppliers support both the commercial nuclear sector as well as the Navy with reactors and components. In summary, suppliers in the United States believe that there is a way to increase production in order to begin meeting the demand which will exist for advanced reactors—as long as appropriate investments can be made in the supply chain in an appropriate timeframe. Based on the capacity projections and lead times, investment will be needed to meet the 5-year and 10-year production targets. Therefore, if significant nuclear deployment is to occur in the 2030s, investment and ramp up of the advanced nuclear supply chain will need to begin in the near future for the United States to successfully deploy these advanced reactors with domestic supply chains.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Summary of Vendor Irradiation Capsule Workshop Hosted at Oak Ridge National Laboratory, October 3-4, 2022

The Department of Energy office of Nuclear Energy, Advanced Reactor Technology office tasked Idaho National Laboratory (INL), and Oak Ridge National Laboratory (ORNL) with hosting a set of two workshops. The primary purpose of these workshops was to convince the commercial high temperature reactor community, specifically the graphite and composite experts, to collaborate with the building and operation of a graphite/ceramic composite irradiation capsule(s). The workshops were designed to first instruct the attendees on the technical and scheduling challenges in conducting such an experiment by providing information on different technical areas in scheduling, designing, building, operating, and disassembling such irradiation capsules. A secondary purpose was to determine the individual irradiation requirements (including the desired irradiated material properties) to understand what the remaining technical needs for gas-cooled and salt-cooled advanced nuclear reactors. The first workshop was held at ORNL October 3-4, 2022. This report summarizes the discussions held during this workshop. The second workshop was hosted at INL April 4-6, 2023 and will have a separate summary report.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Daikin Advanced Lithium Ion Battery Technology - High Voltage Electrolyte

An evaluation of high voltage electrolytes which contain fluorochemicals as either co-solvents or additives has been completed. The project objective was to identify a cell chemistry and electrolyte formulation which is capable of operating at 4.6 V. Stable cycle performance has been demonstrated in LiNi0.50Mn0.30Co0.20O2 (NMC532)/Artificial Graphite pouch cells to 4.6 V, with a discharge capacity retention greater than 80% after 300 cycles. A multitude of physical and chemical changes between 4.2 and 4.6V were investigated, with the goal of correlating identified degradation mechanisms with premature cell failure.

25 ENERGY STORAGE↗