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AGR-5/6/7 Final Release-to-Birth Ratio Data Analysis

AGR-5/6/7 is the last of a series of Advanced Gas Reactor (AGR) experiments conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) in support of development and qualification of tristructural isotropic (TRISO) low-enriched fuel for use in the high-temperature gas cooled reactor (HTGR). AGR configuration and irradiation conditions are based on prismatic HTGR technology that is distinguished primarily through the use of helium coolant, a low-power-density ceramic core capable of withstanding very high temperatures, and TRISO-coated particle fuel. The AGR tests provide valuable irradiation-performance data to support fuel process development, qualify fuel for normal operation and accident conditions, and support development and validation of fuel performance and fission-product (FP) transport models and codes. Each AGR test consists of multiple independently controlled and monitored capsules containing fuel compacts placed in a graphite cylinder shrouded by a steel shell. Release-to-birth ratios (R/B) for fission-gas isotopes released from each capsule are calculated from release rates, measured by germanium detectors in the Fission Product Monitoring System (FPMS) installed downstream from each capsule, and birth rates calculated using numerical models of FG generation. The R/Bs are a critical measure of the ability of the fuel kernel, the particle coating layers, and the compact matrix to retain fission-gas atoms, preventing their release into the sweep-gas flow, and the impact of initially defective particles and/or particle-coating failures that occur during irradiation. For fission-gas isotopes, particle failure is defined as failure of all coating layers, allowing gaseous fission atoms to escape from a particle. During the first five cycles (162B ? 165A), R/Bs were stable in the 10-8?10-6 range, and no in-pile particle failures were observed, based on the gross gamma counts. The maximum R/B value of around 2 ? 10-6 for Kr-85m resulted from the presence of as-fabricated exposed kernels (based on the high exposed kernel fraction), the dispersed uranium, and high fuel particle temperatures in Capsule 1. Comparison of capsule-measured R/Bs from these early cycles to predictions using the previously developed AGR R/B model demonstrated FG release from the AGR-5/6/7 TRISO fuel was comparable to that of previous experiments. In addition, the Kr-85m R/B per-exposed-kernel values are comparable to R/B values obtained in AGR-3/4 irradiation experiment and four irradiation experiments performed during 1980s: (1) HRB-17/18, (2) COMEDIE-BD1, (3) HFR B1, and (4) HRB-21. In contrast, all measured R/B values are lower than predictions by the commonly used Richards and German models, which are intentionally conservative. A large number of in-pile particle failures occurred in Capsule 1 by the end of Cycle 166A. During the final four cycles (166A ? 168A), apparent damage to the Capsule 1 gas line appeared to cause FG leakage from that capsule into the other four capsules, resulting in an increase in fission gas (FG) detected in the effluent for all capsules. Isolation of the Capsule 1 gas line during the last three cycles also prevented measurement of its FG release. Thus, R/Bs in all capsules after Cycle 166A are highly uncertain because of undefined amount of leakage from Capsule 1, especially for long-lived isotopes. A few hundred in-pile particle failures were estimated for Capsule 1 before the end of Cycle 166A, but the total number of failures is unknown due to the lack of FG release data in the later cycles. Based primarily on evidence from the gross gamma counts during Cycle 168A, approximately 15 particles failed in Capsule 3 and four particles failed in Capsule 2. In-pile failures in Capsule 3 were anticipated because this capsule was designed to operate beyond the HTGR normal operating temperature range. In contrast, no in-pile failures were identified in the top two capsules (4 and 5) based on the absence of the typical spikes in gross gamma counts and low failure estimates using the AGR model, developed in INL/EXT-14-32970, for R/B of the short-lived isotopes (Kr-89 and Xe-137) with minimal leakage from Capsule 1.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 1

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore fuel product. The long-term EnCore ® fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Westinghouse Accident Tolerant Fuel Phase 2B with Higher Enriched and Higher Burnup Add-On Project Final Technical Report Deliverable Volume 2

The Westinghouse Electric Company LLC (Westinghouse) accident tolerant fuel (ATF) program funded by Westinghouse and the US Department of Energy (DOE) utilized chromium (Cr) coated zirconium alloy cladding with doped UO 2 (ADOPT(TM)) and uranium silicide (U 3 Si 2 ) high density/high thermal conductivity fuel for its lead test rod (LTR) program with irradiation beginning in 2019. ADOPT is a Cr 2 O 3 +Al 2 O 3 doped UO 2 pellet with increased oxidation resistance and density, and increased resistance to fission gas release. Due to the issues with U 3 Si 2 fuel reaction in pressurized water reactor (PWR) environments, uranium nitride (U 15 N) has been substituted for U 3 Si 2 as a long-term fuel option. Cr coated cladding with ADOPT fuel is the near-term Westinghouse EnCore ® fuel product. The long-term EnCore fuel product is SiGA ® SiC/SiC composite cladding with high density/high thermal conductivity UN fuel. In 2020, the higher burnup and higher enriched and (HBHE) program was integrated into the ATF program. The objective of this expanded program is to extend ATF burnups to at least 75 MWd/kgU to economically facilitate 24-month cycles in PWRs. The ATF program now includes ADOPT fuel with enrichments >5% 235 U. Over the past several years, Westinghouse has tested the Cr coated zirconium (Zr) and silicon carbide (SiC) claddings in Westinghouse Churchill autoclaves and the Massachusetts Institute of Technology (MIT) reactor. Additionally, the Cr coated cladding has been tested in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL) and in LTR programs at the Doel 4 and Bryon 2 commercial reactors. High temperature tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried out to determine the time and temperature limits for the Cr coated zirconium claddings. These tests indicate that Cr coated Zr cladding can take temperatures up to about 1500°C for short periods of time without becoming totally oxidized. The main issue is the formation of the Cr-Zr eutectic at 1333°C resulting in the migration of this eutectic inward with the formation of ZrCr 2 which rapidly oxidizes to ZrO 2 on the outside of the tube. The Cr coated Zr cladding also delays the bursting of the tube, reduces the burst area, and reduces hydriding and embrittlement of the Zr which is a major benefit for reducing fuel fragmentation, redistribution, and dispersal (FFRD), the major licensing issue faced by HBHE. The manufacturing parameters for the SiC have been found to have a significant effect on the corrosion rate of the SiC in light water reactor (LWR) conditions and significant improvements have been made in the yield, quality, and oxidation resistance of the SiC cladding by identifying and tightening manufacturing process parameters. Current autoclave results for SiC composite claddings indicate that a corrosion rate of fewer than 2 micrometers per year can be achieved which meets corrosion requirements under normal operating conditions. High temperature steam oxidation tests at the state-of-the-art Westinghouse facilities in Churchill, PA and at Karlsruhe Institute of Technology (KIT) have been carried and determined that SiC cladding can withstand temperatures up to about 1800°C to 1900°C before excessive corrosion reactions begin, and that the SiC will not balloon and burst. ADOPT fuel pellets were incorporated into the Westinghouse ATF program because of their increased density and oxidation resistance. A topical report supporting the use of ADOPT pellets has been submitted to the NRC and will be approved shortly. ADOPT pellets have been a product in Europe for over 15 years. The additives work to make larger grain sizes which appear to reduce fission gas release during transients as well as increase the density of the pellet. Fuel rod and assembly design in preparation for the lead test rod (LTR) and lead test assembly (LTA) programs is underway as well as licensing efforts with the Nuclear Regulatory Commission (NRC). Finally, accident analyses coupled with economic evaluations for both operating savings as well as fuel savings have been initiated. Modular Accident Analysis Program 5 (MAAP5) calculations indicate that both Cr coated cladding and SiC composite cladding can increase the time to fuel rod loss of geometry for up to two hours longer than current Zr based cladding in a station blackout scenario. This additional time is due to the much higher oxidation resistance of the SiC and Cr coated cladding. These two hours can be used to implement additional response options instituted through the Diverse and Flexible Mitigation Capability (FLEX) program by reactor operators. Both ATF cladding options also reduce hydrogen production which dramatically reduces primary system and containment pressure and the risk of fission product release beyond containment in the unlikely event of an accident. The lower pressure in the system allows more time to feed cooling water to the core, resulting in the avoidance of fuel melting. The coping time is extended indefinitely if the modest water flow provided by FLEX continues. Experimental work on methods to rapidly fabricate SiC composite structures with high density and reduce the fabrication price of SiC fibers while maintaining a high level of performance is needed. Methods for mitigating or stopping the Cr-Zr eutectic are also needed to further improve the oxidation resistance of Cr coated Zr. Minimal (<1%) swelling of U 3 Si 2 and subsequent fission gas release has been demonstrated up to 20 MWd/kgU. Irradiation experiments with U 3 Si 2 fuel in ATR to determine these properties at 40 MWd/kgU were completed but post irradiation examinations were not done since U 3 Si 2 has been replaced by UN. UN has three issues that are being addressed. The first is increasing the oxidation resistance so that there is not excessive reaction up to ~1500°C. While UN increases the pellet density and additives to the UN postponed the temperature at which rapid oxidation occurred by ~100°C to 200°C, this is not enough, and pellet coating options are now being pursued. The second is developing a method to manufacture that does not require the multi-step process of UF 6 to UO 2 to UC to UN. Efforts are underway looking at UF 6 to UN 2 to UN and UF 6 to UF 4 to UN 2 to UN reactions. Finally, an economically acceptable process for potentially enriching the 15 N content of the nitrogen used to make UN to >95% 15 N was identified though not experimentally validated. In addition to the work supported by the DOE, research and testing activities are being carried on in a world-wide effort funded by many countries such as Sweden, United Kingdom, Belgium, Netherlands, Spain, Germany, Japan, and France. This work is being facilitated through the Westinghouse led Collaboration for Advanced Research on Accident Tolerant Fuel (CARAT) program. Annual meetings were organized in 2018 and 2019 by Westinghouse as a venue for presentation of this work and to provide for the cross-fertilization of ideas among the many outstanding researchers in the ATF area. No meetings were held in 2020 and 2021 due to the COVID-19 related restrictions on traveling and gatherings. Since SiC, coated cladding, and high-density fuel options are not currently used in the nuclear industry; support from the government and industry members is needed to further the significant effort of setting new standards. The same is true for the Nuclear Regulatory Commission (NRC) which must review and approve the commercial use of these new fuels since all current regulations are oriented toward Zr/UO 2 fuel. Several meetings have been held with the NRC to generate a fast-track approach to licensing ATF using a combination of atomic modeling, in-rod sensors, and in-reactor testing. This approach was memorialized in an “Accelerated Fuel Qualification White Paper” prepared by the Accelerated Fuel Qualification Working Group lead by General Atomics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effective Permeability of a Nuclear Fuel Assembly

This report aids in the development of models to perform characterization studies of aerosol dispersal and deposition within a spent fuel cask system. Due to the complex geometry in a spent-fuel canister, direct simulation of buoyancy-driven flow through the fuel assemblies to model aerosol deposition within the fuel canister is computationally expensive. Identification of an effective permeability as given in this work for a nuclear fuel assembly greatly simplifies the requirements for thermal hydraulic computations. The results of computations performed using OpenFOAM® to solve the Navier-Stokes Equations for laminar flow are used to determine an effective permeability by applying Darcy's Law. The computations are validated against an analytical solution for the special case of an infinite array of pins for which the numerical and analytical solutions have excellent agreement. The effective permeability of a 1717 PWR nuclear fuel assembly in a basket without spacer grids is numerically determined to be 1.85010 -6 m 2 for the range of fluid viscosities and pressure drops expected in a spent fuel storage canister. However, the flow is not uniform on the scale of multiple pins. Instead, significantly higher velocities are attained in the space between the assembly and the basket walls compared to the flow between the fuel pins within the assembly. Comparison with an analytical solution for fully developed flow through an infinite array of pins shows that the larger spacing near the basket walls results in about a 20% larger permeability compared to the analytical solution which does not include the enhanced flow in the space between the assembly and basket wall, or entrance and exit effects. A preliminary assessment of turbulence effects shows that with a k-epsilon model, significantly higher flow velocities are attained between the fuel pins within the assembly compared to the flow velocity in the space between the assembly and the basket walls. This is the opposite of what is determined for laminar flow.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Cold spray technology in nuclear energy applications: A review of recent advances

Cold spray technology is a promising solid-state, powder-based deposition methods for fabrication of coatings, near-net-shape manufacturing, and component repair. In recent years, this technology has been investigated for many applications in the nuclear energy sector. For example, it has been explored for the deposition of coatings of corrosion and oxidation materials on zirconium-alloys fuel claddings in light water reactors (LWR) for achieving more accident-tolerant fuel (ATF) cladding. Other examples of its use for nuclear energy applications include coatings for enhancements in wear resistance and heat transfer, near-net shape manufacturing of next-generation fuel claddings of oxide dispersion-strengthened (ODS) steels, and for mitigation and repair of potential chloride induced stress corrosion cracking in used fuel storage canister systems. This work reviews published literature on the application of cold spray process for nuclear energy applications, while pointing to gaps that have yet to be addressed.

36 MATERIALS SCIENCE↗

Carbonate-Catalyzed CO 2 Insertion into Hydrocarbon C-H Bonds (Final Technical Report)

The development of methods to utilize CO 2 as a feedstock for chemical and fuel synthesis is critical for creating renewable alternatives to fossil fuel-based products. This project investigated a class of catalyst materials known as "dispersed carbonates", which are composed of alkali carbonate salts (e.g. potassium carbonate) dispersed in porous support materials. These catalysts react with CO 2 and organic molecules to form chemicals known as carboxylates that have wide applications in the chemical industry. The project used a combination of spectroscopic and reactivity studies to provide fundamental insight into the structure and mechanism of dispersed carbonates in these reactions, leading to variants with greater reactivity. In addition, dispersed carbonates were investigated for CO 2 hydrogenation catalysis, which is critical for processes under development for making sustainable fuels. The dispersed carbonates proved to be highly active and selective catalysts for the reverse water gas shift reaction in which CO 2 is hydrogenated to CO. The dispersed carbonates provide a compelling alternative to conventional metal-based catalysts for reverse water gas shift that could enable new process designs with higher efficiency and lower complexity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dispersing Agents Impact Performance of Protonated Phosphonic Acid High-Temperature Polymer Electrolyte Membrane Fuel Cells

The microstructure of ionomers plays a significant role in the performance of high-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs). Here, we establish direct correlations between the properties of dispersing agents and the microstructure of a protonated phosphonic acid ionomer. Most importantly, the formation of the porous structure of a protonated phosphonic acid ionomer depends on the pK a of the liquid media. Namely, the acid–base interaction between the charged polymer and dispersing agents determines the porosity in the ionomer thin films. The HT-PEMFC performance increases with the level of porosity of the ionomer, as the pores enable fast reactant gas accessibility. Overall, this study concludes the importance of the pK a of ionomers’ dispersing media for the HT-PEMFC performance.

25 ENERGY STORAGE↗

A LOCA Analysis Tool: Coupling RELAP5-3D to BISON

Experimental evidence illustrates that at burnups slightly above the current regulatory limit of a rod-averaged burnup of 62 MWd/kgU, the ceramic UO 2 inside light-water reactor fuel rods becomes susceptible to a phenomenon known as fuel fragmentation, relocation, and dispersal (FFRD) during a loss of coolant accident (LOCA) transient. The severity of FFRD is strongly influenced by the zirconium-based (Zircaloy) cladding behavior during the LOCA transient. A Technology Commercialization Fund (TCF) project was awarded to an Electric Power Research Institute (EPRI)/Idaho National Laboratory team to create a LOCA analysis tool that couples BISON to the systems/thermal-hydraulics code RELAP5-3D [1] for analysis of LOCA scenarios. In addition, further refinements to existing BISON models were identified as necessary to more accurately represent more recent experimental evidence from the Studsvik Cladding Integrity Project (SCIP) and other experimental programs.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Atomically Dispersed CuN x Sites from Thermal Activation of Boron Imidazolate Cages for Electrocatalytic Methane Generation

Atomically dispersed metal sites (ADMSs) have been recognized as promising candidates for electrochemical conversion. Among a diverse range of molecular precursors for ADMS synthesis, framework materials are particularly interesting due to their high degree of tunability and control over the primary coordination sphere of the metal ions. In this work, we demonstrate that a copper boron imidazolate cage, BIF-29(Cu), is a convenient precursor for a competent catalyst with isolated Cu sites coordinated by N donors for carbon dioxide electroreduction (CO 2 RR). Although BIF-29(Cu) exhibited moderate methane selectivity over hydrogen evolution reaction (HER), the methane selectivity is significantly enhanced by 2 times (55% CH 4 at –1.25 V vs RHE) after mild thermal activation. Extensive characterization methods indicate the transformation of crystalline BIF-29(Cu) into an amorphous carbonaceous material comprising isolated CuN x sites. Moreover, in situ X-ray absorbance spectroscopy indicates stable CuN x sites that are reduced during CO 2 RR. This work encourages the discovery of single-site electrocatalytic systems through a rational selection of molecular precursor and calcination parameters for promoting product selectivity.

10 SYNTHETIC FUELS↗

Assessment of the CTF subchannel code for modeling a large-break loss-of-coolant accident reflood transient

With increased industry interest in extending reactor operating cycles, the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program has been investigating the behavior of high-burnup fuel during design basis accidents such as the large-break loss-of-coolant accident (LBLOCA) with consideration for risk of fuel fragmentation, relocation, and dispersal (FFRD). As part of that activity, the NEAMS subchannel thermal/ hydraulics (T/H) code, CTF, is being used for modeling of LBLOCA and to determine the impact of subchannel resolution on results. Although CTF includes a wide range of models for LBLOCA conditions, the code has not been used for this application while maintained at Oak Ridge National Laboratory (ORNL) until now. Therefore, here, in this work, a preliminary assessment of several of these models was performed using openly available reflood experimental data from the Flooding Experiments in Blocked Arrays (FEBA) tests. One coarse mesh and one fine mesh model were set up in CTF for high and low flooding rate tests performed in the unblocked FEBA facility. A coarse TRACE model was set up to be as consistent as possible with the coarse CTF model to allow for code-to-code benchmarking. The assessment shows a tendency of the codes to over-predict peak cladding temperature (PCT) near the top of the bundle and to quench early. Advanced spacer grid models were shown to improve upper bundle predictions in CTF. The resolved CTF model over-predicted PCT by a larger degree in the center channels in the low-flooding rate test, and it is believed that the radiative heat transfer model, which was not used in this study, may be needed to correct this over-prediction. Finally, this work demonstrates the importance of the droplet model in determining quench time and vapor temperature and PCT prediction, which necessitates a more in-depth validation of these models in the future.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

High Flux Isotope Reactor Low-Enriched Uranium Low Density Silicide Fuel Design Parameters

High Flux Isotope Reactor (HFIR) highly enriched uranium (HEU) to low-enriched uranium (LEU) conversion activities are ongoing as part of the Department of Energy (DOE) National Nuclear Security Administration (NNSA)’s nuclear nonproliferation mission. Design activities studying the conversion of HFIR from HEU to LEU fuel explored different fuel design features and shapes with a low density uranium-silicide dispersion (U 3 Si 2 -Al) fuel, which has a uranium density of 4.8 gU/cm 3 . The goal of these studies is to generate several HFIR LEU fuel designs of varying fuel fabrication complexity that meet the current HEU performance metrics and safety requirements. The documented designs will serve as references for fuel fabrication and qualification activities. Recent advancements in modeling and simulation tools enable quick prototyping of fuel designs. Shift, a Monte Carlo neutron transport and depletion tool optimized for high-performance computing (HPC) architectures, is used for efficient fuel cycle and performance metrics calculations. The HFIR Steady State Heat Transfer Code (HSSHTC) is used to vet the thermal safety margin. Also, a new automation tool that connects all fuel design analysis steps, named Python HFIR Analysis and Measurement Engine (PHAME), has been developed to expedite the design study in an efficient and reproducible manner. Leveraging these tools, several candidate fuel designs were selected for varying fabrication complexity. This report provides design feature details for four selected HFIR LEU low density U 3 Si 2 -Al fuel designs and their corresponding performance and safety metrics. Nominal, best-estimate design parameters and irradiation conditions, including fission rate densities, power densities, heat fluxes, and cumulative fission densities are provided for candidate fuel designs relevant to framing irradiation experiments to support fuel qualification efforts. Simulations show that the low density U 3 Si 2 -Al, with design features to enhance safety, can meet HEU core performance metrics and safety requirements if the reactor power is increased from 85 MW (HEU) to 95 MW (LEU) and if the active fuel length is increased from 50.80 cm (HEU) to 55.88 cm (LEU).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NEAMS Burnup Extension Accomplishments and Remaining Modeling Gaps

The economic viability of light-water reactors (LWRs) in the United States is declining in heavily subsidized markets, and as a result, the nuclear industry is looking for opportunities to enhance the economic competitiveness of nuclear power. This is not a foreign concept to the nuclear industry: in the mid-2000s, the nuclear industry set out to achieve zero fuel failures by 2010. The goal in this effort was to drive down the cost of reactor shut down by replacing a pin or bundle in response to fuel rod failure. 2010 brought about the initiative to deliver the nuclear promise to reduce operating cost by 30% to improve nuclear energy’s economic competitiveness before 2020. The emergence of accident-tolerant fuel also offers the nuclear industry an opportunity to build on these past successes and deliver affordable, clean energy. Accident-tolerant fuel has been shown to provide superior performance compared to traditional Zircaloy/UO2 fuel concepts, offering the unique ability to remove operational limitations that inhibit the economic viability of nuclear power. This has led the industry to begin building a technical case to extend the peak rod average burnup beyond 62 GWd/tU to extend pressurized water reactor cycle lengths to 24 months and to develop more efficient boiling water reactor core designs. The Nuclear Energy Advanced Modeling and Simulation (NEAMS) program mission is to develop advanced modeling and simulation tools and capabilities to accelerate the deployment of advanced nuclear energy technologies. The primary safety concern inhibiting the nuclear industry from extending burnup is related to high-burnup fuel fragmentation, relocation, and dispersal. Therefore, the NEAMS program developed a targeted 5-year plan to support the industry’s efforts to extend burnup. This milestone report summarizes the 5-year plan that was enacted in FY20, followed by a discussion of the ongoing activates required to fulfill the 5-year plan, as well as the approach to address the current modeling gaps. Additionally, an LWR stakeholder meeting was held to communicate work performed in the NEAMS program over the past three years, to assess the LWR community’s perspective on the impact of the program, and to identify remaining significant gaps in the NEAMS suite of capabilities. This engagement will be documented by the Electric Power Research Institute and used by NEAMS to redirect current LWR scope as needed and to develop the next phase for LWR research and development.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

High-Burnup BWR LOCA Burst Analysis Framework Development and Demonstration

Nuclear power currently contributes approximately 20% of total electricity generation in the United States and more than 10% globally. Given the increasing reliance on nuclear energy to achieve our nation’s goal of reaching net-zero carbon emissions by 2050, there is significant pressure on the existing nuclear industry to extend plant operational licenses and improve efficiency. This is crucial as the existing nuclear fleet serves as a vital bridge until new light water and advanced reactors can be developed and deployed, bolstering the supply of carbon-free energy to meet domestic demands. Operational costs primarily consist of plant operation and maintenance and fuel costs, influenced by materials and reactor core designs. These factors, coupled with heavily subsidized renewable energy markets, create a challenging economic environment for the existing light water reactor fleet, as well as for new build projects. To address these economic challenges, the nuclear industry has developed a strategic blueprint aimed at enhancing nuclear power’s economic sustainability. Past initiatives, such as efforts to eliminate fuel failures by 2010 and reduce operating costs by 30% before 2020, have laid the groundwork. Optimizing core design parameters, including burnup limits and enrichment levels, can lengthen cycles, reduce outages, reduce batch reload batch fractions and spent fuel storage requirements, and lower maintenance and operating expenses, thereby enhancing economic viability. In the United States, boiling water reactors (BWRs) comprise approximately one-third of the fleet, although much of the research and development focus has traditionally been on pressurized water reactors (PWRs). Advances in modeling and simulation, particularly through the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program, are crucial to the long-term viability of BWRs, just as they are for PWRs. A key research area of the high burnup/increased enriched fuel initiative is focused on addressing loss-of-coolant-accident (LOCA)-related issues. NEAMS has dedicated significant effort to enhancing tools to better support BWRs, with a current focus on showcasing the BWR framework for high-burnup LOCA analysis. This high-fidelity work will demonstrate a best estimate pin-by-pin high-burnup BWR LOCA analysis to assess full-core cladding rupture behavior. This modeling capability will help with better understanding and realistic evaluation of fuel fragmentation, relocation, and dispersal (FFRD) phenomena at BWRs, which then could be used to prevent FFRD at BWRs without penalizing operational parameters. In addition, the results of this work will help identify strategies to identify additional margins or to potentially limit cladding rupture through core design optimizations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Modeling spatial patterns of longleaf pine needle dispersal using long-term data

Abstract Background Predicting patterns of fire behavior and effects in frequent fire forests relies on an understanding of fine-scale spatial patterns of available fuels. Leaf litter is a significant canopy-derived fine fuel in fire-maintained forests. Litter dispersal is dependent on foliage production, stand structure, and wind direction, but the relative importance of these factors is unknown. Results Using a 10-year litterfall dataset collected within eighteen 4-ha longleaf pine ( Pinus palustris Mill.) plots varying in canopy spatial pattern, we compared four spatially explicit models of annual needle litter dispersal: a model based only on basal area, an overstory abundance index (OAI) model, both isotropic and anisotropic litter kernel models, and a null model that assumed no spatial relationship. The best model was the anisotropic model (R 2 = 0.656) that incorporated tree size, location, and prevailing wind direction, followed by the isotropic model (R 2 = 0.612), basal area model (R 2 = 0.488), OAI model (R 2 = 0.416), and the null model (R 2 = 0.08). Conclusions As with previous studies, the predictive capability of the litter models was robust when internally validated with a subset of the original dataset (R 2 = 0.196–0.549); however, the models were less robust when challenged with an independent dataset (R 2 = 0.122–0.319) from novel forest stands. Our model validation underscores the need for rigorous tests with independent, external datasets to confirm the validity of litter dispersal models. These models can be used in the application of prescribed fire to estimate fuel distribution and loading, as well as aid in the fine tuning of fire behavior models to better understand fire outcomes across a range of forest canopy structures.

54 ENVIRONMENTAL SCIENCES↗

Elucidating the effect of minor-actinide addition on fuel-cladding chemical interaction in an HT-9 clad U-Pu-Zr metallic fuel irradiated to 6.15 at.% burnup in EBR-II

Scanning and transmission electron microscopy (S/TEM) were used to characterize the local fuel-cladding chemical interaction (FCCI) in one cross-section taken from a HT-9 clad U-20.3Pu-10Zr-1.2Am-1.3Np (in wt.%) fuel irradiated to 6.15 at.% burnup with inner cladding temperatures ranging between 460–490 °C. Results showed that the total interaction thickness between fuel and cladding was <10 µm. Fe infiltrated the fuel to form U-Zr-Fe phases while fuel elements or lanthanides did not infiltrate into the cladding. Np was not involved in the formation of any phases in the examined locations; however, Am played a role by forming a ∼2 µm thick homogeneous Fe-Pu-Am planar front at the inner cladding wall. An oxidized Na layer existed in the fuel-cladding gap with Fe and lanthanide particles dispersed within, suggesting Na could facilitate the transport of fuel and cladding constituents. Secondary phases, including an FCC Zr-rich phase, lanthanide phases, and α’-Cr(Fe) were identified in the outer fuel and FCCI regions. Furthermore, this study suggests that, for the irradiation conditions specific to this cross-section, minor actinides have little impact on FCCI behavior beyond what would be observed in typical HT-9 clad U-Pu-Zr fuel pins systems.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Drop Analysis of the Advanced Test Reactor Fresh Fuel Shipping Container with Heavier Low-Enriched Uranium Fuel Contents

The Advanced Test Reactor Fresh Fuel Shipping Container (ATR FFSC) is a rectangular stainless steel container used for shipping radioactive material. The container is described in the ATR FFSC Safety Analysis Report (SAR). Per the ATR FFSC SAR, the ATR FFSC is designated a Type AF-96 packaging per the definition of 10 CFR §71.4, and was originally designed to transport high enriched uranium (HEU) reactor fuel elements for the Advanced Test Reactor (ATR), the Advanced Test Reactor Critical (ATRC) facility, the Massachusetts Institute of Technology Reactor (MITR), and the University of Missouri Research Reactor (MURR). The Department of Energy, National Nuclear Security Administration’s (NNSA), Office of Material Management and Minimization (M3) is working with the Idaho National Laboratory (INL) to develop and qualify new low enriched uranium (LEU) fuels and technologies for use in the ATR, ATRC, MITR, and MURR reactors. The LEU fuel elements will weigh significantly more than the current HEU designs and, combined with their associated Fuel Handling Enclosures for packaging, some configurations will exceed the 50 lbf used in the ATR FFSC qualifying drop tests. There are LEU versions of MITR, MURR, and ATR fuel elements. However, for this evaluation, drop analysis of the ATR FFSC with only the heavier ATR Low Enrichment (LOWE) fuel element is considered in this evaluation because the LOWE fuel element is the heaviest of the considered LEU fuel elements. The ATR HEU fuel element and the ATR LOWE fuel element are identical in every design aspect except for the fuel meat inside the 19 fuel plates. The LEU fuel meats are made using a U-10Mo high-density foil rather than uranium dispersed in aluminum in the HEU fuel elements. The high density of the uranium in the LEU fuel meat increases the LOWE fuel element weight to just under 44 lbf (versus the 22.1 lbf weight of the tested ATR HEU fuel element). ATR fuel elements are placed in a thin-gauge aluminum weldment called a "Fuel Handling Enclosure" during packaging. The Fuel Handling Enclosure is used to cover and protect the element during loading and unloading operations. The ATR Fuel Handling Enclosure weighs about 15 lbf per the drawings in the ATR FFSC SAR and the weight is accounted for in this evaluation. Transporting the heavier LEU fuel elements require evaluation of two issues. The first is the effect of the increased mass of the LEU fuel elements on the survivability of the ATR FFSC package following the requisite drop qualifications. The second is the effect of the increased mass of the fuel plates on the fuel element during the same drops. The ATR FFSC containing an ATR HEU fuel element in an ATR Fuel Handling Enclosure was physically dropped multiple times to qualify the container as a Type AF-96 package. The ATR FFSC SAR describes the drop tests performed with an actual ATR HEU fuel element weighing 22.1 lbf contained in a 14.3 lbf Fuel Handling Enclosure for a total payload of 36.4 lbf. Those drop tests showed that the ATR FFSC maintained containment of the ATR HEU fuel element and the fuel element was not significantly damaged. (Containment herein is not defined as a leak tight but is retention of the radioactive contents.) The purpose of the evaluation is to analytically show that, for a similar set of tests, the ATR FFSC maintains containment of the heavier ATR LOWE fuel element and to assess the damage to the fuel element during the drops. The approach was to create finite element analysis (FEA) models that produce the same results as the physical drops. Those models were then used as the benchmarks for the follow-on analyses using the heavier contents. FEA models of the drops of ATR FFSC using up to a 115 lbf fuel element were run and evaluated. Likewise, drops of a LOWE fuel element weighing 44 lbf in the ATR FFSC were run and evaluated. It is important to note that this report was done at the quality level necessary to be included in a nuclear facility safety basis. However, it is not the intent of this report to conclude the suitability of the ATR FFSC for transporting the heavier payloads. This report only describes the results of the FEA as related to the required drop scenarios. Incorporation of the FEA into the safety basis will be evaluated by the ATR FFSC design authority. The physical drop tests of the HEU fuel element and FEA drop analysis for the LOWE fuel element showed noteworthy damage to the fuel plates. An aluminum protective block was conceived to mitigate the damage. The concept requires the blocks to be placed in the fuel element between the end boxes and fuel plates. Additional FEA drop analyses were performed using the protective block. The addition of the blocks is primarily intended to mitigate the damage to the LOWE fuel element fuel plates. However, FEA drop analyses of the ATR HEU fuel element with the blocks were also performed and included for information.

42 ENGINEERING↗

High-Platinum-Content Catalysts on Atomically Dispersed and Nitrogen Coordinated Single Manganese Site Carbons for Heavy-Duty Fuel Cells

Fuel cells for heavy-duty vehicles (HDVs) have attracted considerable attention because of their unique scalability, better fuel economy, the less demand for hydrogen refilling infrastructure. However, the potential application requires more stringent fuel cell durability up to 25,000 h. Membrane electrode assemblies (MEAs) made from platinum group metal (PGM) catalyst with relatively high loading 0.3 mgPt cm –2 play a crucial role in ensuring high-power and long-term durability. Integrating fine PGM nanoparticles and robust carbon support with strengthened interactions is critical for improving MEA performance and durability. Herein, a unique atomically dispersed and nitrogen coordinated single Mn site-rich carbon (M–N–C) support was developed for high content (40 wt%) platinum catalysts for the oxygen reduction reaction (ORR) cathode with reduced thickness. Compared with two controls studied in this work (e.g., a porous graphitic carbon-supported Pt and a commercial TKK Pt/C catalysts), the Pt (40 wt%)/Mn–N–C catalyst exhibited much enhanced catalytic activity and stability for the ORR in both aqueous acidic electrolyte and polymer electrolyte-based MEA. Here, we carefully elucidated the—role of the Mn–N–C support in promoting Pt catalyst concerning its high surface area, partially graphitic structure, and nitrogen dopants, providing better Pt nanoparticle dispersion, and strengthened interactions between Pt and carbon. Consequently, the MEA from the Pt (40 wt%)/Mn–N–C catalyst generated a 1.61 A cm –2 at 0.7 V based on HDV conditions (0.2 mgPt cm –2 and 250 kPa air). More importantly, the MEA is highly durable and can retain 1.31 A cm –2 at 0.7 V after 30,000 voltage cycles (~19% loss), surpassing the commercial Pt/C catalyst (loss of ~56%). Therefore, the Mn–N–C carbon-supported Pt catalyst holds a great promise to meet the challenging DOE target (1.07 A cm –2 at 0.7 V after 150,000 cycles) for HDVs.

25 ENERGY STORAGE↗

A Plan to Qualify New Fuel for the High Flux Isotope Reactor for Material Minimization

The High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL) is one of five high power research reactors the Office of Material Management and Minimization (M3) Program, Office of Conversion is working to convert from using highly enriched uranium (HEU) fuel to using low-enriched uranium (LEU) fuel. This effort stems from the primary objective within the U.S. Department of Energy (DOE) National Nuclear Security Administration (NNSA) to achieve permanent threat reduction by minimizing, and when possible, eliminating weapon-usable nuclear material around the world. Under M3’s Office of Conversion, the U.S. High Performance Research Reactor (USHPRR) Project is pursuing fuel qualification and licensing of the high-performance reactors to operate with LEU fuels. All high-performance reactors except HFIR will be converted to LEU monolithic uranium-molybdenum alloy fuel. HFIR will be evaluated for conversion to LEU using a uranium silicide fuel, namely, U3Si2-Al dispersion fuel.The mission of the USHPRR Project is to develop the technology needed to reduce, and eventually eliminate, worldwide use of HEU in civilian applications. The goal is to develop the technical means needed to use low enriched uranium (LEU) instead of HEU fuel in research and test reactors without significant penalties in performance, economics, or safety of the reactors. The USHPRR Project has four major elements, called Pillars: Fuel Qualification (FQ) managed at Idaho National Laboratory (INL), Fuel Fabrication (FF) managed at Pacific Northwest National Laboratory (PNNL), Reactor Conversion (RC) managed at Argonne National Laboratory (Argonne), and Cross-Cutting (CC) managed at Savannah River National Laboratory (SRNL). FQ is responsible for the qualification of the fuel type. RC is responsible for supporting reactor conversion analysis and overseeing licensing submittals leading to conversions of domestic reactors to LEU fuel. For the FQ effort, FQ (INL) worked in collaboration with RC (Argonne) and ORNL to develop the plan for the uranium silicide fuel qualification for HFIR.The resulting HFIR Fuel Qualification Plan provides the general approach for the USHPRR team to move the selected uranium silicide fuel design for HFIR conversion through qualification. Authorization and use in HFIR will be approved through the DOE’s Office of Science. Uranium silicide fuel was previously qualified in NUREG-1313 at an approximate maximum heat flux of 1.4 MW/m2 and a maximum fuel section temperature of about 130°C. In addition to the different regulator process utilized by DOE, these upper limits will be exceeded in HFIR; therefore, further testing will be necessary to ensure the fuel can meet HFIR qualification requirements. The HFIR fuel loading may exceed 4.8 gU/cm3 which was determined in the NUREG-1313 safety evaluation to be acceptable for use in non-power NRC-regulated reactors provided there exist no other safety considerations. In addition, the uranium silicide fuel will need to be qualified in a HFIR-specific design. This plan includes the currently available information from the USHPRR Project Functions and Requirements document and expands these requirements to ensure that planned tests have traceable results providing evidence that the requirements have been met. Data collection methods are discussed as well as the process to show that the requirements have been met. This document is designed to provide a pathway for researchers to obtain data necessary and at the appropriate quality level for HFIR fuel qualification.

Shokes, Tamara↗