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At least 181 records · Page 10

Depletion benchmark for a high-assay low-enriched uranium fuel experiment in the advanced test reactor

Reactor physics depletion benchmarks for high-assay low-enriched uranium (HALEU) fuel are limited in number. In particular, there is limited data for HALEU benchmarks for U-10Mo (uranium-10% molybdenum) plate fuel that is being developed for use in the United States’ high performance research reactors including the Advanced Test Reactor (ATR), Advanced Test Reactor Critical Facility (ATR-C), High Flux Isotope Reactor (HFIR), Massachusetts Institute of Technology Reactor (MITR), University of Missouri Research Reactor (MURR), National Bureau of Standards Reactor (NBSR). These six reactors currently operate with highly enriched uranium dispersed fuel in an aluminum matrix. In support of conversion to a HALEU fuel, qualification of U-10Mo formed into a monolithic foil is being performed. Fuel qualification involves irradiating fuel specimens in the ATR. The irradiation tests provide an opportunity to benchmark depletion capabilities of reactor physics codes in support of the ATR operation, as well as develop benchmarks that can be used by other institutions to benchmark other reactor physics codes. This paper documents the development of a benchmark model of the irradiation of the ATR Full-size plate In center flux trap Position 7 (AFIP-7) experiment using the depletion codes MC21 and Advanced Dimensional Depletion for Engineering of Reactors (ADDER).

Nielsen, Joseph W. [Idaho National Laboratory (INL↗

Crystallographic characterization of (C 5 H 4 SiMe 3 ) 3 U(BH 4 )

New syntheses have been developed for the synthesis of (borohydrido-κ 3 H)tris­[η 5 -(tri­methyl­sil­yl)cyclo­penta­dien­yl]uranium(IV), [U(BH 4 )(C 8 H 13 Si) 3 ] or Cp' 3 U(BH 4 ) (Cp' = C 5 H 4 SiMe 3 ) and its structure has been determined by single-crystal X-ray crystallography. This compound crystallized in the space group P1¯ and the structure features three η 5 -coordinated Cp' rings and a κ 3 -coordinated (BH 4 ) – ligand.

36 MATERIALS SCIENCE↗

A High-Assay Low-Enriched Uranium Fuel Transportation Concept

The uranium 235U enrichment commonly used in fuel production for U.S. light water nuclear reactors typically does not exceed 5 wt%. In contrast, many of the currently investigated advanced reactor concepts demand fuel with higher enrichments. This includes high-assay low-enriched uranium (HALEU), characterized by a 235U enrichment of 5 to 20 wt%. The necessity of HALEU transportation in the fuel production cycle leads to new challenges caused by various technical and regulatory hurdles. Current U.S. Nuclear Regulatory Commission–approved transportation package designs for UF6 with enrichments above 5 wt% provide relatively small payloads [=116 kg (250 lb)]. Furthermore, in accordance with 10 CFR 71.55, package design activities for fissile material enriched above 5 wt% need to consider water infiltration in the containment as part of the criticality safety evaluations. This study presents a transportation package concept for HALEU advanced nuclear reactor fuel with a significantly higher payload of up to 376 kg (830 lb) of fissile material per package and up to 1881 kg (4149 lb) of HALEU per legal weight truck. The anticipated chemical form of the transported material is UO2 downblended from available highly enriched uranium. The concept utilizes a combination of existing transportation packaging, 18 inner canisters, and a novel basket design that includes a borated aluminum flux trap. Criticality and shielding evaluations; fundamental structural, confinement, and thermal assessments; and studies on package operations are presented. The results of this study build significant confidence in the technical feasibility of a high-capacity HALEU transportation package concept while demonstrating the concept’s potential to meet U.S. regulatory requirements.

Eidelpes, Elmar↗

Reactions of U + with H 2 , D 2 , and HD Studied by Guided Ion Beam Tandem Mass Spectrometry and Theory

The kinetic energy-dependent reactions of the atomic actinide uranium cation (U + ) with H 2 , D 2 , and HD were examined by guided ion beam tandem mass spectrometry. An average 0 K bond dissociation energy of D 0 (U + – H) = 2.48 ± 0.06 eV is obtained by analysis of the endothermic product ion cross sections. Quantum chemistry calculations were performed for comparison with experimental thermochemistry, including high-level CASSCF–CASPT2–RASSI calculations of the spin–orbit corrections. CCSD(T) and the CASSCF levels show excellent agreement with experiment, whereas B3LYP and PBE0 slightly overestimate and the M06 approach badly underestimates the bond energy for UH + . Theory was also used to investigate the electronic structures of the reaction intermediates and potential energy surfaces. The experimental product branching ratio for the reaction of U + with HD indicates that these reactions occur primarily via a direct reaction mechanism, despite the presence of a deep-well for UH 2 + formation according to theory. The reactivity and hydride bond energy for U + are compared with those for transition metal, lanthanide, and actinide cations, and periodic trends are discussed. Furthermore, these comparisons suggest that the 5f electrons on uranium are largely core and uninvolved in the reactive chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A preliminary investigation into the feasibility of laser ablation U–Pb isotope ratio measurement via all‐faraday cup detection with 10 11 ‐ and 10 13 ‐Ω amplifiers on the Neoma multicollector‐inductively coupled plasma‐mass spectrometer

Rationale Signal detection for uranium–lead (U–Pb) dating of zircon is typically performed via ion counters. Here, we develop a preliminary understanding of the strengths and limitations of faraday‐cup‐based detection. Methods A suite of zircon reference materials and the NIST‐610 glass were sampled using laser ablation followed by U–Pb isotope ratio measurement on a Neoma multicollector‐inductively coupled plasma‐mass spectrometer. Results We were able to produce geologically accurate 207 Pb/ 206 Pb, 206 Pb/ 238 U, and 207 Pb/ 235 U ratios for the NIST‐610 glass and the zircon standards, with ages ranging from ~2.5 Ga to ~337 Ma (TanBrown A, Oracle, 91550, Mud Tank, Temora, and Plešovice). Two of the younger zircon standards examined (94‐35, ~55.6 Ma, and Fish Canyon, 28.6 Ma) yielded accurate 206 Pb/ 238 U but not 207 Pb/ 235 U or 207 Pb/ 206 Pb ratios, whereas the youngest zircon standard (Penglai, ~4.4 Ma) failed for all three ratios of interest. The accuracy and precision of the all‐faraday method are directly tied to signal intensity, with reliable data capable of being produced even when both isotopes in a ratio have signals below ~0.001 V (equivalent to ~62 500 cps on an ion counter). Conclusion The all‐faraday cup multicollection method provides sufficient sensitivity to obtain geologically meaningful U–Pb data, with possible advantages being that laser pit depth‐dependent changes in the observed interelemental fractionation behavior may be easier to correct using a static collector configuration compared to when the ion beam is swept across a single detector while also removing the need for an interdetector‐type calibration. Further work is needed to refine the all‐faraday cup method (e.g., application of background subtraction and common Pb corrections, outlier removal, and interelement as well as down‐hole fractionation corrections), but our initial results demonstrate that the faraday detector method has sufficient sensitivity to warrant further study.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Separation of protactinium from uranium-niobium alloys for 231 Pa– 235 U radiochronometry in nuclear forensic investigations

The isolation and purification of protactinium from uranium materials is essential for 231 Pa– 235 U radiochronometry, but separating Pa from uranium-niobium alloys, a common material in the nuclear fuel cycle, is challenging due to the chemical similarity of Pa and Nb. Here, in this work, we present three resin chromatography separation techniques for isolating Pa from U and Nb which were independently developed by three different laboratories through ad hoc adaptations of standard operating procedures. Our results underscore the need for and value of purification methods suitable for a diversity of uranium-based materials to ensure the operational readiness of nuclear forensics laboratories.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microstructure, Thermal, and Mechanical Properties Relationships in U and UZr Alloys (Final Report)

Uranium-zirconium (U-Zr) alloys are candidate fuel systems for transmutation based reactors that can be used to burn long-lived minor actinides and fission products in fast spectrum reactors. Metallic fuels have also been gaining more recent attention for applications as accident tolerant fuels, as well as for use in small modular reactors. This research focused on a “science-based” approach to capture the connections between U and U-Zr alloys’ three-dimensional (3-D) microstructure, thermal properties, and mechanical properties through closely coordinated experiments and modeling efforts from the unirradiated to the irradiated fuels. Advanced characterization and modeling techniques were used to understand irradiation-induced microstructural evolution and its direct impact on the thermal and mechanical properties of U and U-Zr fuel. Closely coordinated experiments and modeling were performed to provide crucial data that does not currently exist. Overall, this research spanned multiple length and time scales within the models and experiments. The scope of the research encompassed the understanding of the irradiation effects in U and various U-Zr alloys with particular attention paid to three task areas: (1) microstructural evolution, (2) in-situ/ex-situ thermal and mechanical properties, and (3) multiscale modeling connections to microstructure, thermal, and mechanical properties. This research resulted in (1) the 3-D characterization of neutron irradiated U-Zr fuel in multiple phase regions to better understand fission gas swelling and constituent redistribution, (2) development of a microstructural model linking thermal and mechanical properties via in situ Raman and nanoindentation, (3) and mesoscale phase field modeling was coupled with the AEH method in the MOOSE framework was used to calculate the effective thermal conductivities of U-Zr fuels consisting of α-U and δ-UZr 2 heterogeneous microstructures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Radiological Characterization of Uranium Decay Products in LEU U-10Mo Before and After Heat Treatment

Fuel for the U.S. high-performance research reactor fleet is undergoing significant development as the United States moves away from using highly enriched uranium dispersion fuels. The proposed fuel is a high-density, low-enriched uranium (LEU, 19.75 wt% U 235) alloyed with ten weight percent molybdenum fuel (known as LEU U 10Mo). The LEU U 10Mo fuel samples studied in this report were made by down-blending highly enriched uranium with a master alloy, which is cast from molybdenum rods and depleted uranium, via vacuum induction melting and then casting.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Anthropogenic uranium signatures in turtles, tortoises, and sea turtles from nuclear sites

Chelonians (turtles, tortoises, and sea turtles) grow scute keratin in sequential layers over time. Once formed, scute keratin acts as an inert reservoir of environmental information. For chelonians inhabiting areas with legacy or modern nuclear activities, their scute has the potential to act as a time-stamped record of radionuclide contamination in the environment. Here, we measure bulk (i.e., homogenized scute) and sequential samples of chelonian scute from the Republic of the Marshall Islands and throughout the United States of America, including at the Barry M. Goldwater Air Force Range, southwestern Utah, the Savannah River Site, and the Oak Ridge Reservation. We identify legacy uranium ( 235 U and 236 U) contamination in bulk and sequential chelonian scute that matches known nuclear histories at these locations during the 20th century. Our results confirm that chelonians bioaccumulate uranium radionuclides and do so sequentially over time. This technique provides both a time series approach for reconstructing nuclear histories from significant past and present contexts throughout the world and the ability to use chelonians for long-term environmental monitoring programs (e.g., sea turtles at Enewetok and Bikini Atolls in the Republic of the Marshall Islands and in Japan near the Fukushima Daiichi reactors).

63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗

Transmission electron microscopy investigation of phase transformation and fuel constituent redistribution in neutron irradiated U-10wt.%Zr fuel

Uranium-10wt.%zirconium (U-10wt.%Zr) is a primary candidate for fast reactor nuclear fuels. However, there is a lack of data characterizing neutron irradiated crystallographic phases and chemistry. In the current study, the microstructural evolution of a U-10wt.%Zr fuel neutron irradiated to a burnup of 5.7 at.% was investigated by scanning transmission electron microscopy, energy dispersive spectroscopy, and selected area electron diffraction to determine the major phases, alterations in microstructure, and variations in local chemical composition at different localities of a fuel cross-section. The current study revealed that the irradiated U-10wt.%Zr fuel was comprised of various major phases, including a-U, ß-U, and d-UZr2, as well as amorphous and crystalline solid fission product (FP) precipitates within different regions of the fuel cross-section. Regions A and A/B in the center of the fuel were comprised of U-rich, U-intermediate, and U-lean localities with a-U and d-UZr 2 composing the major phases. Regions B and C in the intermediate and peripheral fuel localities, respectively, were comprised of a-U grains, U-rich (ß-U) grains with Zr-rich precipitates, U-intermediate grains (d-UZr2), and solid FP precipitates. The major phases identified were associated with the nanoscopic chemical concentrations, the phase diagram, and the as-characterized specimen temperature, with the exception of the non-equilibrium ß-U phase identified in region B. The U-lean localities in regions A, A/B, B, and C were Zr-enriched pathways along subgrain/grain boundaries. This phenomenon suggests that Zr is susceptible to radiation-induced segregation in U-Zr fuels and indicates a new mechanism for constituent redistribution.

36 MATERIALS SCIENCE↗

University of Missouri Research Reactor (MURR) LEU Fuel Fluid-Structure Interaction Analysis

The University of Missouri Research Reactor (MURR ® ) is one of five U.S. high performance research reactors (USHPRR), plus one critical facility, that are actively collaborating with the National Nuclear Security Administration (NNSA) Material Management and Minimization (M 3 ) Reactor Conversion Program to convert from highly enriched uranium (HEU, ≥ 20 wt.% U-235) to low-enriched uranium (LEU, < 20 wt.% U-235) fuel. A new type of LEU fuel with very high density, based on an alloy of uranium and 10 weight percent molybdenum (U-10Mo), is expected to allow the conversion to LEU of USHPRR that have been found unable to be converted with previously qualified uranium silicide-aluminum (U 3 Si 2 -Al) dispersion fuel. MURR has been working with the USHPRR Reactor Conversion (RC) Pillar at Argonne National Laboratory to perform fuel element design and fuel cycle performance analyses, steady-state thermal hydraulics safety analyses, and accident safety analyses in preparation for the conversion of MURR and to support a preliminary Safety Analysis Report (SAR) for conversion to LEU fuel. In this work, Fluid-structure interaction (FSI) analysis at the fuel element level, as compared to the fuel plate level of the previous work. is performed which models all components of the MURR LEU fuel element, including fuel plates and the supporting structures e.g., side plates, end fittings, and combs. Therefore, the effect of supporting structures on the coolant flow distribution, the fuel plate deflection, and the resulting coolant channel gap reduction can be evaluated. In addition to the nominal element geometry and flow rate, the tolerances in the geometry dimensions of coolant channel and plate thickness, the effect of a comb on plate deflection, and the uncertainty of the flow rate per element are considered in this work. The effect of comb on plate displacement is quantified through two bounding cases: the case assuming a perfect bond between the comb and plates and the case neglecting the comb effect. Note that in this analysis, the FSI has been decoupled from the other structural effects caused by irradiation (e.g., swelling and irradiation creep). Assessment of combined effects is planned for a later stage of this project.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Magnetism and finite-temperature effects in UZr 2 : A density functional theory analysis

The structure and the thermophysical properties of d-UZr 2 are investigated using 0 K density functional theory and ab initio molecular dynamics (AIMD). Modeling the true paramagnetic state of this intermetallic compound has been challenging using first-principles calculations. For the first time, we find that the generalized gradient approximation method without applying an on-site Coulomb interaction term (Hubbard U) can result in a ground state that is antiferromagnetic (AFM). We believe that this weak AFM ground state is the closest to the real paramagnetic state. We found that structure optimization at finite temperatures using AIMD is necessary to achieve this ground state instead of the non-magnetic and ferromagnetic states previously reported in the literature. Our findings indicate that applying the Hubbard U on uranium f-orbitals in this metallic system is unnecessary and not recommended, as it leads to a large overestimation of the volume and introduces an unphysical strong spin polarization. Finally, our approach results in atomic volume, thermal expansion, and heat capacities that have strong agreement with experiments.

36 MATERIALS SCIENCE↗

Impact of UV-light and pH on the Fate of Tc, I, and U in Wetlands at Savannah River Site - 20230

The Savannah River Site (SRS) is one of the major nuclear facilities owned by the U.S Department of Energy. During the Cold War, these facilities produced large amounts of radioactive and hazardous waste. On site, three unlined seepage basins in the F-Area received approximately 1.8 billion gallons of low-level waste containing nitric acid, radionuclides, and dissolved metals due to plutonium and tritium production operations. The acidic nature of the waste created a source of relatively mobile radionuclides below the basins. Radionuclides previously disposed of within the F-Area, including uranium isotopes (U), technetium-99 (Tc-99), and iodine-129 (I-129), are moving with groundwater towards Four Mile Branch Wetland, where they are subsequently upwelling and interacting with natural organic matter (NOM). Many environmental factors including redox conditions, porewater composition, pH, light, and temperature affect the degradation of organic matter as well as interactions with Tc-99, U, and I-129. In particular, the high concentrations of nitrate from the acidic waste may increase the formation of reactive oxygen species (ROS) that impact both degradation of NOM and behavior of contaminants. In the presence of sunlight, I-129, Tc-99, and U speciation and complexation behavior may be affected by ROS and NOM degradation products in addition to the factors generally considered in subsurface systems in the absence of light. This research aims to determine whether the interactions between radionuclides, NOM, and nitrate affect the fate of I-129, Tc-99, and U and which processes are controlling their behavior. Experiments were conducted at variable pH in the presence of NaNO{sub 3} in order to determine the impact of light and pH on NOM degradation and to evaluate the impact on the fate of contaminants of concern. Soil samples high in NOM collected from two sites in the Southeastern United States (Savannah River Site and the Everglades) were studied. Batch experiments were conducted with NOM and the following aqueous contaminants, U, I-129, Tc-99 with exposure to ultraviolet (UV) light in an environmental chamber. This study was conducted in a sterile environment in order to exclude the potential for microbial degradation of organic matter. Results indicated photodegradation of NOM and significant interaction of radionuclides with NOM. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Preliminary Thermo-Mechanical Analysis of Irradiated MURR LEU Fuel Element

The University of Missouri Research Reactor (MURR) is a multi-disciplinary research and education facility providing a broad range of analytical, materials science, and irradiation services to the research community and the commercial sector. MURR is one of five U.S. high performance research reactors (USHPRR), plus one critical facility, that is actively collaborating with the National Nuclear Security Administration (NNSA) Material Management and Minimization (M3) Office of Reactor Conversion and Uranium Supply to convert from the use of highly enriched uranium (HEU, ≥ 20 wt% U-235) to low-enriched uranium (LEU, < 20 wt% U-235) fuel. A new type of very high-density LEU fuel based on an alloy of uranium and 10-weight percent molybdenum (U-10Mo) is expected to allow the conversion of some USHPRR, including MURR, to LEU fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Analysis of FRAM Measurements to Establish Methodology Uncertainty

Qualification measurements were performed at Oak Ridge National Laboratory (ORNL) on a variety of measurement standards. These measurements will be used to qualify the Fixed-Energy, Response Function Analysis with Multiple Efficiency (FRAM) code with a high purity germanium (HPGe) detector for use at ORNL. Measured items include uranium isotopic standards, U 3 O 8 line sources, and a uranium tetrafluoride source. The 235 U enrichment was estimated using the FRAM isotopic analysis software for each source and compared with the declared isotopic values.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Formation and Consolidation of UN Nanostructures in U-Mo Fuel via Mechanical Alloying and Spark Plasma Sintering

Uranium-molybdenum (U-Mo) alloys show promise as a nuclear fuel system due to their high thermal conductivity and high fuel loading capability. However, U-Mo systems suffer from irradiation induced swelling ultimately affecting the cladding via mechanical and chemical interaction. To address these shortcomings, this thesis investigated the formation of uranium mononitride (UN) nanoparticles within a U-10Mo matrix. To promote the formation of UN, U-10Mo powders were mechanically alloyed under a high purity nitrogen cover gas (99.9995%) atmosphere. Variations were made in stainless steel milling media size, duration of milling, and number of times the milling jar was re-aerated with nitrogen gas. UN nanoparticulates were successfully formed within the U-Mo matrix and was characterized utilizing light element analysis, X-ray diffractometry, scanning and transmission-electron microscopy, electron energy loss spectroscopy, and atom probe tomography. Presence of the UN nanoparticles was found as early as 1-hour into the mechanical alloying process, and significant iron contamination found after 10-hours of milling. The U-Mo/UN powders were compacted using spark plasma sintering techniques in order to stabilize the nanostructure. U-Mo/UN compacts containing small amounts of neodymium and helium were analyzed to observe the defect migration tendencies of fission products within the fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Thermal properties of U-Mo alloys irradiated under high fission power density

A variety of physical and thermal property measurements made on irradiated U-Mo alloy monolithic fuel samples with a Zr diffusion barrier and clad in Al alloy 6061 are reported. These properties form the basis for additional investigations in thermal behavior of U-Mo fuel under high performance research reactor irradiation conditions. Measurements were performed on samples harvested from fuel plates irradiated under high fission power density and surface heat flux and complement previous measurements on samples subjected to moderate fission power density and surface heat flux. Specific heat capacity of irradiated monolithic U-Mo increases with increasing temperature and fission density, but carries large uncertainties associated with thickness measurements used to determine the mass fraction of the layer constituents for extraction of the U-Mo specific heat capacity, specifically the very thin and nonuniform Zr diffusion barrier. Density of irradiated monolithic U-Mo decreases with increasing fission density resulting from fission gas swelling and porosity formation. Thermal diffusivity of irradiated monolithic U-Mo increased with increasing temperature and decreased with increasing fission density. Thermal conductivity of irradiated monolithic U-Mo increased with increasing temperature, and in general, appeared to decrease and become less sensitive to temperature with increasing fission density. Thermal conductivity measurements compared to a semi-empirical model agreed within ±30%. It is suspected that the main driver in deviation between model calculations and measurements is the fission gas swelling determination, which does not account for fission power density or irradiation temperature.

uranium (U), molybdenum, nuclear fuel, thermal con↗

Thermo-Mechanical Analysis of Irradiated MURR LEU Fuel Plates

The University of Missouri Research Reactor (MURR®) is a multi-disciplinary research and education facility providing a broad range of analytical, materials science, and irradiation services to the research community and the commercial sector. MURR is one of five U.S. high performance research reactors (USHPRR), plus one critical facility, actively collaborating with the National Nuclear Security Administration (NNSA) Material Management and Minimization (M 3 ) Reactor Conversion Program to convert from the use of highly enriched uranium (HEU, ≥ 20 wt% U 235) to low-enriched uranium (LEU, < 20 wt% U-235) fuel. All USHPRR, including MURR, completed designs with a new type of very high-density LEU fuel based on an alloy of uranium and 10-weight percent molybdenum (U-10Mo) for conversion to LEU fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗