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Review of the Technical Basis for Properties and Fuel Performance Data Used in HEU to LEU Conversion Analysis for U-10Mo Monolithic Alloy Fuel

This report provides the technical basis for properties and fuel performance data used in conversion analysis for U.S. High Performance Research Reactors (USHPRR) that will convert from highly enriched uranium (HEU) to low-enriched uranium (LEU) using a new U-10Mo monolithic alloy fuel that is being qualified. The conditions that the fuel experiences changes between an HEU and LEU fuel element design due to many causes, including the density of the fuel, the presence of U-238 resonant absorber, changes to the plate and coolant channel dimensions, and changes in fuel management due to reactivity or optimization. These types of changes have been documented in operational and safety analyses conducted for conversions over decades for over 70 reactors. These conversions have all, or almost all, required recalculation of safety-related values as well as establishing operational characteristics of the core, including power distribution, reactor core power level, and cycle length between required fuel management. An overall objective of conversion is to change the reactor core design as little as possible while maintaining the reactors’ scientific, isotope production, medical, and engineering missions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Impact of MURR LEU Conversion on Beryllium Reflector Lifetime

The U.S. National Nuclear Security Administration (NNSA) Office of Material Management and Minimization (M 3 ) has developed and is pursuing an integrated approach to address the persistent threat posed by unintentional proliferation of nuclear materials. The NNSA M 3 approach reduces the risk of highly enriched uranium (HEU) and plutonium falling into the hands of non-state actors by minimizing the use of and, when possible, eliminating weapons-usable nuclear material around the world. In this geopolitical context, most research and test reactors, both domestic and international, have completed or started a program of conversion from the use of HEU to low-enriched uranium (LEU) as fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of increasing the initial nitric acid concentration from a maximum of 7.5 to 8.5 M during the dissolution of aluminum spent nuclear fuel

H-Canyon is blending solutions from the dissolution of High Flux Isotope Reactor (HFIR) and Material Test Reactor (MTR) fuels with Target Residue Material (TRM) to prepare feed solution for the 1st Cycle of solvent extraction. The initial acid concentration for HFIR fuel dissolution is limited to 7.5 M by the flowsheet; however, an increase in the initial concentration is desirable to more easily achieve the target acidity for solvent extraction using the current blending strategy. To provide flexibility in batching the highly enriched uranium (HEU) solutions, the Savannah River National Laboratory (SRNL) was requested to evaluate the potential for increasing the maximum HNO3 concentration for HFIR fuel dissolution from 7.5 to 8.5 M. In response to this request, a literature review was performed to evaluate the impact of a higher starting HNO3 concentration on the dissolution of aluminum spent nuclear fuels (ASNF) including both HFIR and MTR fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of Nuclear Materials on Both Sides of Regulatory Control: from IAEA Safeguards to Global Counter-Nuclear Smuggling

Global nuclear security is dependent upon the sustained and verifiable control of radiological and nuclear (R/N) materials within nuclear facilities, under the administrative purview of national governments. It is the responsibility of each country to account for their R/N materials holdings and to ensure that they do not escape regulatory control and fall into the wrong hands. The Office of Nuclear Smuggling Detection and Deterrence (NSDD) is tasked with providing support to foreign partners in developing the tools and expertise to detect, disrupt, and investigate R/N materials encountered out of regulatory control, in such circumstances as at border crossings and other checkpoints, or in the course of routine policework. Thankfully, such incidents are infrequent, and NSDD continues to work bilaterally with partner countries to strengthen their capabilities to combat nuclear smuggling and trafficking incidents in their countries. For the vast majority of R/N materials that remain under regulatory control, however, it is critical that their safe storage and use be independently verified. Even a single loss incident of R/N materials, particularly of special nuclear materials (highly-enriched uranium and plutonium) has the potential to cause a catastrophe. How can the international community be assured that R/N materials currently under national regulatory control remain there?

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Sulfur Pellets Responses to a Bare and Steel Reflected Pulse of the Oak Ridge National Laboratory Health Physics Research Reactor

The experiments analyzed in this report were conducted at the Health Physics Research Reactor (HPRR), also known as the $\textit{Fast Burst Reactor}$. The reactor was designed and built at Oak Ridge National Laboratory (ORNL) in 1961. The HPRR was an unmoderated, unshielded fast reactor that used highly enriched uranium and molybdenum alloy as fuel. The reactor was initially sent to the Nevada Test Site in 1962, where it was used to evaluate radiation doses received as a result of the Hiroshima and Nagasaki bombings during World War II. A few years later, the reactor was sent back to ORNL to be part of the Dosimetry Application Research (DOSAR) facility shown in Figure 1, which included a reactor building shown on the left (west) of the picture and a control and laboratory building in the upper right corner (northeast). The critical assembly was used for numerous technical studies, including systems calibration, dosimetry, radiobiology of plants and animals, testing of radiation alarms, as well as teaching and training in radiation dosimetry and nuclear engineering. Between 1963 and 1987, the HPRR was operated for thousands of hours, achieving criticality close to 10,000 times and motivating many publications. The HPRR was decommissioned in 1987. The goal of this effort was to use historical data from operation of the HPRR to create a criticality accident alarm system (CAAS) benchmark to be included in the $\textit{International Handbook of Evaluated Criticality Safety Benchmark Experiments}$ (ICSBEP Handbook). A thorough inspection was performed of all available documentation and information available. The most promising experiments that were selected for evaluation were those described in the 1987 ORNL report entitled $\textit{Health Physics Research Reactor Reference Dosimetry}$, ORNL-6240. The report includes reference dosimetry results of the shielded and unshielded configurations of the HPRR after burst operations. Because of changes to the reactor positioning and storage systems that were made in 1985, the previous dosimetry reports became obsolete, and the newly designed experiments were needed to create the HPRR’s adjusted dosimetry data. The various results reported in ORNL-6240 include reference doses and dose equivalents from different conventions at different distances and elevations as determined using the detected neutron fluence and conversion factors. The HPRR neutron fluence was obtained through different methods, including sulfur pellet analysis and threshold detector unit data. Information about the HPRR spectrum was also obtained through Bonner sphere measurements. This benchmark is focused on a part of the measured sulfur fluences reported in Appendix H of ORNL-6240. Standard commercial sulfur pellets were placed at different distances from the HPRR centerline during burst operation and were activated due to the 32 S(n,p) 32 P reaction. The resulting 32 P activity was then measured and the information about the corresponding sulfur fluence and/or neutron dose could be extracted. Many of those measurements have 7 been performed with the HPRR in its bare configuration or with different shields (combinations of Lucite, concrete, steel). All the necessary, precise information about material and/or dimensions of the different shields was not found, so it was decided to focus only on the unshielded and steel-shielded configurations to minimize the benchmark uncertainty. A total of 31 cases (24 unshielded and 7 shielded cases at different positions) of sulfur fluence were selected before evaluation to develop the benchmark.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Minimum Resolution Requirements for Gamma Identification Algorithms

Each year there are millions of dollars spent on the research and production of high-resolution detectors. This research indicates that the pursuit of higher resolution detectors is not always necessary. The terminal resolution of a NaI detector, or highest detector resolution, at which identification algorithms fail to identify highly enriched uranium (HEU) was evaluated using GADRAS, Genie, and GammaVision. GADRAS employs a template matching algorithm, while Genie and GammaVision utilize a mathematical approach for peak search and identification. The NaI spectra utilized for evaluation were generated using the GADRAS Inject tab and source modeling functions. Each spectrum included terrestrial and cosmic background from Dallas, TX. The resolutions for each spectrum were increased from a default 8.92% to a point where each algorithm would fail to identify 235 U from a HEU source. Six different source configurations were used in this research: bare HEU, 50% shielded HEU, 90% shielded HEU, bare HEU with an interference source of 99 mTc, bare HEU with 99 mTc both shielded 50%, and bare HEU with 99 mTc both shielded 90%. T

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiological Handling and Containment Considerations in Support of an American Medical Isotope Producer

This work will discuss evaluation and design of new and modified facility level radiological containment, transfer, and handling systems in support of the United States’ American Medical Isotope Production Act. In the United States alone, Molybdenum-99 (Mo-99) is used as a precursor to locally generate its decay product, technetium-99m (Tc-99m), for use in approximately 40,000 medical procedures every day to detect cancer and heart disease. Currently, however, Mo-99 is primarily produced overseas and typically requires highly enriched uranium (HEU) which is classified as weapon -usable. This poses a serious security risk to the United States and, in 2012, Congress passed the American Medical Isotope ACT which aimed to cease all Mo-99 production that requires HEU and support American based companies who have found safer production methods. Through this effort, a system was designed and developed to access irradiated material in processing hot cells for ease of material introduction and removal in the confined area. The proposed solution uses a double-door design that allows for easy access to material while also providing shielding through a mechanically manipulated carousel. A system was also designed to transport irradiated materials from target reactors to a target receipt box using a rail guide system, pneumatic motor, and lead screw drive.

07 ISOTOPE AND RADIATION SOURCES↗

Evaluation of Niowave's Proposed Solvent Washing Approach

Niowave, Inc., is a domestic supplier of medical and industrial isotopes from uranium (U) and radium (Ra). The company has recently entered into a cooperative agreement with the U.S. Department of Energy’s National Nuclear Security Administration (NNSA) and plans to deploy a superconducting electron accelerator (LINAC) to fission U for molybdenum-99 ( 99 Mo) production without the need for a nuclear reactor or highly enriched uranium (HEU). NNSA provided funding to the Savannah River National Laboratory (SRNL) to support Niowave in this effort. SRNL evaluated the application of the solvent washing process for Niowave.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluation of China Experimental Fast Reactor Startup Tests (Final Report)

This report documents the results and observations on the Coordinated Research Project (CRP) of the International Atomic Energy Agency (IAEA) on “Neutronics Benchmark of CEFR Start-Up Tests.” The China Experimental Fast Reactor (CEFR) is a 65MWt sodium-cooled fast reactor with highly enriched uranium oxide fuels. The reactor achieved the first criticality in 2010, and series of start-up tests were conducted to measure various reactor physics parameters. In 2018, IAEA has launched the CRP for validation and qualification of member states' computation capabilities in the field of fast reactor simulation utilizing the measured data in the CEFR start-up test. Twenty-nine international organizations from eighteen member countries, including Argonne National Laboratory, have participated in the CRP.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Involute Working Group – Validation of CFD Turbulence Models for Steady-State Safety Analysis of Corner Geometry

Worldwide, three research reactors have fuel plates curved as a circle-involute (a spiral generated around a circle): Oak Ridge National Laboratory High Flux Isotope Reactor located in Tennessee, U.S.A. [1], Institut Laue-Langevin High Flux Reactor located in Grenoble, France [2], and Technical University of Munich Research Neutron Source Heinz Maier-Leibnitz located in Garching, Germany [3]. All three reactors are currently using highly enriched uranium ( 235 U/U ≥ 20 wt%) as fuel, and all three are actively engaged in activities to convert to low-enriched uranium ( 235 U/U < 20 wt%) fuel.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Safety Analysis Report For Packaging, Y-12 National Security Complex, Model ES-3100 Package with Bulk HEU Contents

This safety analysis report for packaging (SARP) presents the results of the safety analysis prepared in support of the Consolidated Nuclear Security, LLC (CNS) request for licensing of the Model ES-3100 package with bulk highly enriched uranium (HEU) contents and issuance of a Type B(U) Fissile Material Certificate of Compliance. This SARP, published in the format specified in the U.S. Nuclear Regulatory Commission (NRC) Regulatory Guide 7.9 and using information provided in UCID-21218 and NRC Regulatory Guide 7.10, demonstrates that the Y-12 National Security Complex (Y-12) ES-3100 package with bulk HEU contents meets the established NRC regulations for packaging, preparation for shipment, and transportation of radioactive materials given in Title 10, Part 71, of the Code of Federal Regulations (CFR) [10 CFR 71] as well as U.S. Department of Transportation (DOT) regulations for packaging and shipment of hazardous materials given in Title 49 CFR.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nucleation, Growth, and Aggregation of Todorokite Nanoparticles from Both Geochemical and Materials Science Perspectives (Final Technical Report)

A vast amount of manganese (Mn) nodules exists in ocean sediments, covering about 30% of the ocean floor. Tunneled and layered Mn(IV) oxides, hereafter called TMOs and LMOs, are the primary mineral phases hosting Mn. Owing to their unique structure and properties, these Mn oxides are highly enriched in transition metals, platinum group metals, and rare earth elements, up to several percentages in weight. Thus, many metals are stored in these nodules and the nodules have thus been increasingly considered for their potential as a source of strategic metals for national security applications and the energy industry. The nodules also play an important role in trace metal biogeochemical cycling in the ocean because they control the partition and distribution of trace metals in oceanic sediments. Layered and tunneled structures differ in their mineralogical and chemical properties. For example, TMOs contain fewer metals compared to LMOs in ocean nodules. Therefore, the relative proportion of the two types of minerals in ocean nodules determines the metal sequestration capacities of the nodules, hence the amount of metals stored in the nodules and metal cycling in oceans. The overall objective of this study is to investigate the mechanisms of layered to tunneled structural transform driven by redox reactions. Specifically, we focus on the redox reactions between Mn(IV) and Mn(II) because they often coexist during Mn redox cycling.

58 GEOSCIENCES↗

IER 557: Godiva Pulse Repeatability and Characterization (CED-3A Report)

Godiva IV is a fast burst critical assembly constructed of approximately 65 kg of highly enriched uranium (HEU) fuel alloyed with 1.5% molybdenum for strength. Godiva IV is proposed as the radiation source for IER 498: Design a Shielding Benchmark with a Metal Critical Source. IER 498 proposes a two-burst method to determine the performance of shielding samples, comparing the transmission of the source radiation to detectors with and without a shielding sample present. This eliminates the need for an absolute calibration and allows many uncertainties to cancel. However, the source term variability must be low compared to other sources of experimental uncertainty to ensure the overall uncertainty meets acceptable levels to provide useful measurements. The primary goal of this experiment is to quantify the source term variability, or reproducibility, of Godiva bursts, focusing on the 70 °C bursts planned for IER 498 measurements. Discussions during IER 498 noted that a number of bursts (on the order of six to ten) as identical as possible would be performed and that a 5-7% standard deviation in source intensity would be acceptable.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Impact of Changes in ENDF/B-VII.1 and ENDF/B-VIII.0 235U Nuclear Data Indicated by NDSE Studies on LLNL Pulsed Sphere Simulations

A recent journal article by J.A. Gomez et al. measured gamma-ray die-off curves of three subcritical static highly-enriched uranium (HEU) assemblies driven by an external neutron source with a new detector system. This new detector system was developed for being used in dynamically driven subcritical assemblies as part of the Neutron Diagnosed Subcritical Experiments (NDSE) program. Simulations of these die-off curves with various nuclear data and comparison to experimental data indicated that a decrease of the ENDF/B-VII.1 235 U(n,inl) cross section by a factor 0.8 and 0.85 for ENDF/B-VIII.0 would lead to better predictions of experimental data. Here, we test the proposed changes with another type of measurement response, namely neutron-leakage spectra emitted in LLNL pulsed sphere measurements. These spheres were pulsed by 14-MeV neutrons produced via the D+T reaction in their center. The proposed changes in nuclear data have a distinctly smaller impact on predicting pulsed-sphere neutron-leakage spectra than for the die-off curves; they lead to a worsened prediction of the inelastic valley of LLNL pulsed-sphere neutron spectra indicating that the proposed change could constitute a compensating error. Changes in the inelastic angular distributions along with the cross section might be worthwhile to study

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurements for Flattop-HEU Benchmark Reevaluation

In June 2022, high-fidelity measurements of the Flattop critical assembly were taken at the National Criticality Experiments Research Center (NCERC) at the Nevada National Security Site by a team from Los Alamos National Laboratory, Figure 1. Flattop-HEU is composed of a sphere of highly enriched uranium (HEU) surrounded by a thick spherical natural uranium (NU) reflector as shown in Figure 2 and Figure 3. These measurements were taken as part of the reevaluation of the Flattop-HEU benchmark evaluation for the International Criticality Safety Benchmark Evaluation Program (ICSBEP) Handbook. This reevaluation is being completed to update the benchmark to modern standards with significantly improved fidelity and uncertainty analysis. [1] The measurements address the largest identified uncertainties determined during a preliminary reevaluation in 2015. [2]

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Subcriticality Measurements for a Changing Concentration Uranyl Nitrate Solution Tank by Californium Source-Driven Noise Analysis

Subcritical californium source-driven noise analysis (CSDNA) measurements were performed at the Oak Ridge Critical Experiments Facility in 1983 using a stainless-steel tank with an inside diameter of 76.2 cm and a height of 91.4 cm but only filled with a uranyl (93.16 wt.% 235 U) nitrate solution to a height of 76.2 cm for all measurements. The free acid content of the uranyl nitrate solution was less than 0.01 N to minimize hazards in handling. The total available highly enriched uranium for these measurements was 5,296 g. The concentration of the solution was varied from the highest density of 14.71 grams of uranium per liter (g U/L) initially in 16 steps, lowering the concentration to 0.3492 g U/L, and finally using a tank filled with only water. The tank had a Plexiglas lid to minimize evaporation. The Cf source was contained in a re-entrant Lexan tube which could be in the solution parallel to the axis of the cylindrical tank. The detectors were 3 He proportional counters in the solution in shrink-fit tubing to isolate the counters from the fissile solution and adjacent to the outside of the tank. In some cases, the detectors were scintillators adjacent to the outside of the tank. In other cases, the source was external to the tank. Some data presented in this report are from notes and are not in the logbook. The prompt neutron decay constant was obtained from fitting the date from the CSDNA measurements. The purpose of this report is to document the experimental information for the measurements performed so that later, researchers could perform the required uncertainty and calculational analyses and documentation to use these data for an International Nuclear Criticality Safety Benchmark Program (ICSBEP) or a Nuclear Energy Agency benchmark. The prompt neutron decay measurements could be the basis of as International Reactor Physic Benchmark Program. The data from these measurements are available from the Records Management Services Department of Oak Ridge National Laboratory, and the logbook is also available from the ICSBEP at Idaho National Laboratory. Preparation of the present report is part of a larger cooperative effort between Idaho National Laboratory (INL) and Oak Ridge National Laboratory (ORNL) to document more than 15 undocumented critical and subcritical experiments enumerated in ORNL/TM-2019/18 and performed by ORNL at ORCEF and other USDOE critical experiments facilities using more than 500 operational days of critical facility time.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Impact of Irradiation and Decay Time on Chemical Speciation in Uranyl Sulfate Solution

A pH-1, 200-g U/L, highly enriched uranyl sulfate solution was neutron-irradiated using an accelerator-driven neutron source (the Universal Neutron Irradiator, UNI) to fission U-235 under conditions similar to those used by SHINE to produce Mo-99 in a subcritical assembly. We completed a series of five uranyl sulfate irradiations to assess the impact of irradiation and decay time on uranium precipitation and iodine speciation in solution. The duration of each irradiation was increased in order, with the shortest irradiation taking 2.9 hours and the longest, 64.5 hours. A total of 9.5E16 U-235 nuclei were fissioned in all irradiations, and a maximum fission power density of 0.26 W/mL was reached in the final irradiation. We observed no evidence of uranyl peroxide or other precipitates, demonstrating that the addition of Fe 2+ to a final Fe concentration of 200 ppm in the target solution was successful at preventing precipitation under representative irradiation conditions. Nonvolatile I - was found to be the dominant (>70%) iodine species in solution, both immediately after irradiation and after days to weeks of decay time.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Thermal-Epithermal eXperiments – Hafnium Experiment Performed at the DOE’s National Criticality Experiments Research Center (NCERC)

The Thermal-Epithermal eXperiments (TEX) – Hafnium (TEX-Hf) experiments were completed in October 2022 at the DOE National Criticality Experiments Research Center (NCERC) at the Nevada National Security Site (NNSS). This measurement campaign provides seven unique configurations that can be used to validate the neutron absorption and scattering cross sections of hafnium in a highly enriched uranium (HEU) system. Hafnium is a strong neutron absorber important for marine propulsion systems. Mike Zerkle of the Naval Nuclear Laboratory (NNL) states, “The experiments were requested by Naval Reactors to provide a suite of unclassified, clean, and well-characterized benchmarks to drive improvements to hafnium nuclear data.” The experiments were a collaboration between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and NNL, funded by the Nuclear Criticality Safety Program (NCSP). The Hf was procured directly by NNL and provided for the experiment.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗