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At least 127 records · Page 7

Aluminum-doped U 3 Si 2 composite fuels with enhanced oxidation resistance

Al-doped U 3 Si 2 composite fuels with controlled microstructure were fabricated by spark plasma sintering that display greatly-improved oxidation resistance as compared with monolithic and Al-doped silicides prepared by standard powder metallurgy or arc melting. The effects of Al additives on the thermal-mechanical properties and oxidation resisance of the micron- and nano-sized U 3 Si 2 composites were investigated. Additionally, a minimal addition of 1.8 at% Al is effective to increase the onset oxidation temperature of as-fabricated U 3 Si 2 pellets to 580 °C, which can be further increased to 610 °C by thermal annealing. The Al-doped U 3 Si 2 composite fuels also display simultaneously higher hardness and fracture toughness than un-doped U3Si2. These results highlight an effective strategy by integrating minimal Al additives, microstructure control and post-thermal annealing to design advanced silicide fuels with excellent oxidation resistance, desired thermal-mechanical properties and maintained high fissile element density.

36 MATERIALS SCIENCE↗

U 3 Si 2 and UO 2 composites densified by spark plasma sintering for accident-tolerant fuels

This work reports the synthesis and characterization of the U 3 Si 2 and UO 2 composites sintered by spark plasma sintering (SPS) with controlled microstructures for accident-tolerant fuel application. The U 3 Si 2 and UO 2 composites with different silicide and oxide ratios were synthesized by SPS at temperatures from 1000 to 1300 °C for 5 minutes. The microstructure and phase composition of the SPS densified composite fuels were characterized with scanning electron microscopy, X-ray diffraction (XRD), and energy dispersed spectroscopy (EDS). A systematic study of the thermal and mechanical properties was conducted using microhardness testing and laser flash apparatus, along with oxidation resistance measurements using thermogravimetric analysis (TGA). The results show that the synthesis of composite fuels can be achieved with a 90% theoretical density (TD) at 1000 °C and over 95% TD when sintered at 1300 °C. XRD and EDS results confirmed that the dominant phases in the composites are U 3 Si 2 and UO 2 . Improved physical density generally leads to improved hardness, fracture toughness, thermal diffusivity, and onset temperature during the oxidation process. U 3 Si 2 was found to play a dominant role in determining the mechanical and oxidation properties of the composite fuels, whereas UO 2 had a more important impact on controlling the thermal diffusivity of the composites. The composite with 50 wt% UO 2 sintered at 1300 °C displayed the onset oxidation temperature of 500 °C by dynamic oxidation testing using TGA at a ramp degree of 10 °C/min. The composite also achieved a high fracture toughness of ~3.5 MPa m ½ . Finally, these results highlight the potential of composite fuel forms densified by SPS with simultaneously enhanced fissile element density, fracture toughness, thermal transport properties, and oxidation resistance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fabrication and thermophysical properties of UO 2 -UB 2 and UO 2 -UB 4 composites sintered via spark plasma sintering

Uranium dioxide (UO 2 ) composites with uranium diboride (UB 2 ) and uranium tetraboride (UB 4 ) have been proposed as advanced fuel candidates due to their high thermal conductivity, high melting point, high fissile density and their ability to incorporate a built-in burnable poison by tailoring the targeted 10 B/ 11 B ratio. As such, it is important to assess the fabrication, and thermal and micromechanical properties of such composites. In this work, UO 2 -UB 2 and UO 2 -UB 4 samples with boride phase fractions of 5, 15 and 30 wt% were fabricated to high densities (above 95 % theoretical density) via spark plasma sintering (SPS). This enabled sintering at relatively low temperatures and short timescales. SPS also aided in maintaining the target phase fractions of the samples as reactions between the constituent phases were suppressed due to the short timescales and reducing environment during sintering. Here, thermal diffusivity measurements from 299 to 1273 K were conducted through laser flash analysis (LFA). The diffusivity increased as a function of boride weight fraction, and UB 2 additions increased the thermal diffusivity of the composites more than UB 4 additions. Assessment of the LFA results indicated in-situ reactions between the UO 2 and boride phases that suppress the thermal diffusivity occur above 800 K for all samples. Oxidation of the boride phase was proposed as the underlying reaction. This was supported by thermodynamic assessments from the literature, as well as microstructural, crystallographic, and nanoindentation characterization performed on these samples.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electron microscopy characterization of the fuel-cladding interaction in medium burnup annular fast reactor MOX

In this work, we present electron microscopy data focused on the fuel-cladding interaction layer in annular fast reactor MOX with HT-9 cladding at medium burnup. In agreement with previous literature data, the volatile fission products Cs, Te and I have migrated radially into the extreme fuel periphery and partially interacted with the cladding. The accumulation of Cs has occurred in the outermost rim of the fuel pellet, where grain recrystallization has also been observed. Significant amounts of Pd have been found in the interaction zone, particularly in the sample taken from the upper half of the fissile column where the cladding temperatures are higher. At this axial location, Cr has been enriched at the cladding inner surface and diffused into the fuel. Furthermore, chromium remains mainly in metallic form, but locally formed oxides. The fission products Cs, Te and I are found, with variable composition, in form of nanocrystalline regions dispersed in the metallic Cr-rich layer. The morphology and chemical characteristics of the layer suggest a non-oxidative corrosion mechanism as principal cladding degradation phenomenon occurring in this sample, with local onset of Cr oxidation within the nanocrystalline precipitates.

36 MATERIALS SCIENCE↗

Irradiation-enhanced diffusion and diffusion-limited creep in U 3 Si 2

U 3 Si 2 is an advanced fuel candidate due to its relatively high fissile density and attractive thermal properties. Compared to standard UO 2 fuel, there are significant data gaps for the thermophysical and thermomechanical properties of U 3 Si 2 . Point defect concentrations and mobilities under irradiation govern a number of important fuel performance properties, such as creep and fission gas release. In this work, we utilized density functional theory (DFT) data to inform a cluster dynamics framework to predict point defect concentrations in U 3 Si 2 under irradiation. Molecular dynamics (MD) simulations were used to examine the contribution of atomic mixing during ballistic cascades to diffusion, as well as the diffusivity of U and Si at grain boundaries. These atomic scale models for diffusivity were then used to inform a creep model based on bulk (Nabarro-Herring) and grain boundary (Coble) diffusional creep, and climb-limited dislocation creep. The model compares well against available experimental data and has been implemented in the BISON fuel performance code. Finally, a demonstration case using simple power profiles has been carried out, showing that negligible creep occurs due to the low temperatures experienced by U 3 Si 2 in-reactor, a consequence of its high thermal conductivity.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

First-principles investigation of the thermophysical properties of NaCl, PuCl 3 , and NaCl-PuCl 3 Molten salts

Molten salts have a variety of applications that span the nuclear and solar industries, and which involve thermal storage and heat transfer. There is a present knowledge gap in the thermophysical properties of molten salts, which limits the readiness level of molten salt applications. This is especially pertinent for molten salt reactors where the fissile material is dissolved within the molten salt. Ab initio molecular dynamics is a common method employed to investigate the structural and thermophysical properties at elevated temperatures. NaCl-PuCl 3 is a candidate fuel salt in molten salt reactors. The scope of this study is to investigate the seven unique compositions and a range of temperatures of NaCl-PuCl 3 and calculate the density, heat capacity, compressibility, enthalpy of mixing, and coefficient of thermal expansion. Within this work, the van der Waals (vdW) interactions are primarily handled with the vdW-DF2 functional but spot-checked with both the dDsC and DFT-D3 methods. The calculated densities are in good agreement with the NaCl and the eutectic compositions, and no experimental values exist for PuCl 3 at these temperatures. The densities are fit to a first-order Redlich-Kister expansion as a function of both composition and temperature. The heat capacity in the literature is scattered but the calculated values agree well with one of the experimental results. Here, the heat capacity increases as a linear function with respect to concentration at a rate of about 7.5 J/mol-K per 10 mol% PuCl 3 .

36 MATERIALS SCIENCE↗

Assessment of uranium nitride interatomic potentials

Uranium mononitride (UN) is a promising nuclear fuel due to its high fissile density, high thermal conductivity, and suitability for reprocessing. In this study, two uranium nitride interatomic potentials are assessed: Tseplyaev and Starikov's angular-dependent potential and Kocevski et al.'s embedded atom model potential. Predictions of the thermophysical and elastic properties of UN, UN 2 , and α- and β-U 2 N 3 computed using both potentials are assessed and compared to available experimental data. Notably, the Tseplyaev potential performs better with the energetic aspects of UN, e.g., specific heat capacity and point defect formation energies, whereas the Kocevski potential performs better with the structural aspects of UN, e.g., thermal expansion as well as with the elastic properties. The reasons why the Kocevski potential underestimates the UN specific heat are explained by examining the UN phonon properties modeled using both potentials. The Kocevski potential shows better identification of the mechanical stability ranges of UN, UN 2 , and α- and β-U 2 N 3 , reasonably predicting the melting point of UN and predicting stable structures for UN 2 and α- and β-U 2 N 3 . On the other hand, the Tseplyaev potential predicts a premature phase change of both UN and UN 2 and cannot stabilize α- nor β-U 2 N 3 . However, the Kocevski potential cannot predict a stable α-U phase and is thus not suitable for the calculation of formation energies for non-stoichiometric point defects.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Molecular-dynamics study of diffusional creep in uranium mononitride

Uranium mononitride (UN) is a promising advanced nuclear fuel due to its high thermal conductivity and high fissile density. Yet, many aspects of its mechanical behavior and microstructural features are currently unknown. In this paper, molecular dynamics (MD) simulations are used to study UN's diffusional creep. Nanometer-sized polycrystals are used to simulate diffusional creep and to calculate an effective GB width. It is found that Nabarro-Herring creep is not dominant in the temperature range of 1700–2000 K and that the dominant diffusional creep mechanism is Coble creep with an activation energy of 2.28 ± 0.09 eV. A method is proposed to calculate the diffusional GB width and its temperature dependence in polycrystals. The effective GB width of UN is calculated as 2.69 ± 0.08 nm. This value fits very well with the prefactor of the phenomenological Coble creep formula. It is demonstrated that the most comprehensive thermal creep model for UN can be represented as the combination of our Coble creep model and the dislocation creep model proposed by Hayes et al.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

3D pore structure reconstruction of fluff region in top of EBR-II irradiated fuel by X-ray micro-computed tomography

Metallic fuels comprised of U-Zr binary and U-Pu-Zr ternary alloys are a promising fuel candidate for sodium-cooled fast reactors and possess many advantages over ceramic fuels such as higher uranium density and improved thermal conductivity. Fluff is a highly porous structure forming at the top of metallic fuel slugs during irradiation and was extensively observed in past sodium-cooled fast reactor (SFR) experiments such as Idaho National Laboratory’s Experimental Breeder Reactor II (EBR-II). Previous investigations have shown that fluff is rich in fissile atoms and hence could have neutronics implications, but its formation mechanisms are not understood. In this work, two cube-shaped lift outs were taken from the fluff and bulk fuel regions of a high burnup U-19Pu-10Zr composition EBR-II fuel slug and characterized by micro computed tomography (Micro-CT) and energy dispersive x-ray spectroscopy (EDS). This was used to characterize differences in microscale porosity and composition between fluff and bulk fuel, and to support or oppose postulated fluff formation mechanisms. Surface EDS showed minimal differences between the elemental compositions of the fluff and fuel cubes. However, three-dimensional (3D) pore analysis from the tomography scans showed significant differences between the fluff and fuel cube pore size distributions at the microscale level. The high porosity and irregular pore distribution seen in macroscale fluff was also present within the micro-scale fluff cube, having a much higher porosity than the fuel cube which was concentrated in a few large pore networks. In conclusion, these results indicate support for a creep driven mechanism of fluff formation.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effect of iodides on thermal behavior and phase partitioning in LiCl-KCl

Liquid-fueled molten salt reactors (MSRs) are designed to operate with fissile materials and, ultimately, fission products dissolved in the primary molten salt coolant. Understanding the speciation and transport of iodine—a high-yield fission product—is essential because this element’s accidental release poses significant environmental concerns due to its capacity to be readily absorbed by the human thyroid gland. Here, we report the impact of iodide species (LiI and KI) on phase transitions, phase distribution, and phase stability in LiCl–KCl-eutectic salt mixtures. The study employed a combination of computational and experimental techniques, including thermodynamic FactSage calculations, differential scanning calorimetry, and high-temperature X-ray diffraction. The results indicate that the presence of iodide (10–25 wt%) significantly alters the melting behavior of the LiCl–KCleutectic system. Adding 10 wt% LiI has a more-pronounced effect than 10 wt% KI, as LiI converts to KI, leading to formation of LiCl, thereby, altering the LiCl-KCl ratio which significantly affects the melting temperature of the mixture. Furthermore, the evolution of crystalline structure, solid-fraction composition, and the dynamics of mixed-halide solid–liquid partitioning as a function of temperature indicate the potential for selective iodide separation from chloride-salt mixtures via solid–liquid separation techniques. Overall, the presented findings provide valuable insights that are beneficial for the design and operation of MSRs, as well as for the safe handling and effective processing of used nuclear fuel using advanced pyrochemical techniques.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Development of a Reference Database for Beta-Delayed Neutron Emission

Beta-delayed neutron emission is important for nuclear structure and astrophysics as well as for reactor applications. Significant advances in nuclear experimental techniques in the past two decades have led to a wealth of new measurements that remain to be incorporated in the databases. In this work, we report on a coordinated effort to compile and evaluate all the available β-delayed neutron emission data. The different measurement techniques have been assessed and the data have been compared with semi-microscopic and microscopic-macroscopic models. The new microscopic database has been tested against aggregate total delayed neutron yields, time-dependent group parameters in 6-and 8-group re-presentation, and aggregate delayed neutron spectra. New recommendations of macroscopic delayed-neutron data for fissile materials of interest to applications are also presented. The new Reference Database for Beta-Delayed Neutron Emission Data is available online.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Absolute Branching Ratios of Prominent $γ$ Rays Following $α$ Decay of 233 U

The absolute $γ$-ray branching ratios (emission probabilities) for 19 prominent peaks in the $α$ decay of 233 U are reported with energies ranging from 97 to 366 keV. The branching ratios were obtained from $α-γ$ coincidence measurements, normalized to the $α$ singles. The high-purity 233 U material (> 99.98%) was separated from its decay products before preparation of a 4.74-mg/cm 2 uranyl nitrate foil with a 6-mm diameter. Furthermore, this is the first report on the absolute normalization of the branching ratios since 1984 and it is the only measure by $α-γ$ coincidences, where the $α-γ/α$ ratio removes several potential systematic biases. Overall, the results are consistent with the adopted literature, and they validate the quantities most relevant to the non-destructive assay of fissile 233 U material, which is relevant to the thorium fuel cycle and associated safeguards.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Sensitivity of the active neutron coincidence collar response during simulated and experimental fresh fuel assay

Verification of the fissile (and fertile) content in fresh nuclear fuel assemblies is conducted by the IAEA to enforce the Nuclear Non-Proliferation Treaty using the UNCL (Uranium Neutron Collar — Light Water Reactor Fuel). The UNCL uses an uncorrelated AmLi neutron source to interrogate the fuel, producing a signal of coincident fission neutrons (Doubles rate) used to assay 235 U content of the fuel. The cost of producing calibration assemblies and limited availability of diverse commercial assemblies at any one time historically restricted the ability to explore the full parameter space experimentally. Monte Carlo simulations can overcome this, but introduce additional sources of uncertainty. In this work, the sensitivity of simulations and measurements to various parameters is assessed for a reference 1616 PWR assembly of uniform 3.2% enrichment. Uncertainty contributions in this evaluation include: simulated AmLi neutron source spectrum, AmLi neutron emission rate, AmLi anisotropicity, high density polyethylene (HDPE) density, the precise position of the fuel assembly within the detector, and experimentally the statistical uncertainty. The overall total systematic uncertainty estimate for the simulation of the absolute/relative Doubles rates responses are estimated to be approximately 2.0%/1.5%, and for experimental measurements systematic uncertainty reduces to 1.1%. This analysis supports further work using the relative Doubles rates in place of measurements for updating and extending the UNCL analysis methodology as systematic uncertainty is reasonably small.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A new generation of uranium coincidence fast neutron collars for assay of LWR fresh fuel assemblies

The active uranium neutron coincidence collar provides a means of non-destructively assaying the fissile linear density of Light Water Reactor fresh fuel assemblies containing low enriched uranium. These neutron collars can operate in two modes: a thermal and a fast mode. In fast mode, a neutron collar has an added cadmium (Cd) liner in the sample cavity of the detector to reduce the impact of the burnable poison (thermal neutron absorber) on the detector signal (doubles). The main advantage for operating in fast mode is a detected signal that is less dependent of the burnable neutron poison content and thus less dependent on facility operator declarations. The drawback is that operating in fast mode requires a longer measurement time (~hour vs tens of minutes for thermal mode) to achieve the statistically needed precision in the measurements. The trend in the modern reactor fuel assemblies is moving to higher burnup by using higher initial enrichment and, consequently, a higher number of burnable poison rods to compensate the initial neutron reactivity. The increase of the burnable poison loading has motivated the development of a new generation of high efficiency fast neutron collars to allow practical measurements in-field by nuclear inspectors. This paper describes the development and performance evaluation of a new generation of neutron collars, for both boiling water reactor (BWR) and pressurized water reactor (PWR) fuels, jointly developed between the US Department of Energy, through Los Alamos National Laboratory, and the Euratom Safeguards Directorate of the European Commission. In this work, we present here calibrations with reference fuel assemblies at Los Alamos National Laboratory as well as the results of in-field measurement campaigns in fuel fabrication plants with modern commercial fuel assemblies. The experimental results show that a typical PWR verification can be made in a total time of 30 min with an uncertainty in the measured mass of 2% at one standard deviation (1σ). A BWR verification can be made in 47 min with an uncertainty in the measured mass of 1.9% at 1σ, or a total time of 20 min with 1σ uncertainty in the measured mass of 2.5%.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Performance evaluation of neutron noise analysis in detecting special nuclear materials

Reliable and rapid inspection techniques play a vital role in preventing illicit trafficking of special nuclear materials. Active interrogation systems using neutrons produced by portable, high-flux deuterium-deuterium or deuterium-tritium neutron generators are being actively developed as a secondary scanning tool for this purpose. In this study, a neutron noise analysis-based approach for detecting unshielded and shielded special nuclear materials by using a pulsed deuterium-tritium neutron generator was evaluated. Here, this approach analyzes the fluctuation of neutron counts. Its performance was quantified with regard to time-to-detection to achieve a minimum probability of detection of 99% and a probability of false alarm of less than 1% considering various amounts of special nuclear materials and different shielding configurations. It was demonstrated that this approach could detect 17 uranium slugs in 5 s given a neutron generator yield of 8.1 × 10 7 n/s. These slugs could be detected within a reasonable time frame (200 s) when they were shielded by 10.16 cm of high-density polyethylene. The results obtained using the neutron noise analysis approach were compared with those obtained using the commonly used differential die-away analysis technique, a sensitive technique for detecting the presence of fissile materials by utilizing the prompt fission neutrons produced when the source neutrons from a neutron generator are completely diminished. For example, the time to detect 2 unshielded uranium slugs was 2.1 s when using the differential die-away analysis technique; it increased to 93 s for the neutron noise analysis approach. Although the noise analysis-based approach exhibits an overall performance which is not as good as that of differential die-away, neutron noise provides an alternative method for effective detection of special nuclear materials.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

EVALUATION OF HOT CHANNEL FACTOR FOR SODIUM-COOLED FAST REACTORS WITH MULTI-PHYSICS TOOLKIT

The evaluation of hot channel factor (HCF) is of great significance to the quantification of safety margins for reactor designs. In this paper, HCFs for a sodium-cooled fast reactor (SFR) are evaluated with the Simulation-based High-efficiency Advanced Reactor Prototyping (SHARP) toolkit, which is developed under the Nuclear Energy Advanced Modeling and Simulation (NEAMS) Campaign of DOE for multi-physics reactor performance and safety simulations. The high-fidelity neutronics and thermal hydraulics solvers PROTEUS and Nek5000 in the SHARP toolkit are coupled to perform the multi-physics simulations for HCF evaluation. The HCFs induced by cladding manufacturing tolerance, fissile content mal-distribution, wire orientation and uncertainties on the cladding, coolant, and fuel properties are evaluated for a reference core SFR design (AFR-100). The HCFs calculated with the SHARP toolkit are compared to legacy HCFs for similar reactor types. The comparison demonstrates the reduction or elimination of modeling uncertainties in the calculation of HCFs using high fidelity advanced modeling and simulation tools without the need of expensive experiments. Moreover, the reduction of the uncertainties on HCFs evaluation allows an increase in nominal parameters and safety margin, which in turn improves the economic competitiveness of the SFR.

Hot channel factor (HCF)↗

Transformational Challenge Reactor preconceptual core design studies

In the nuclear industry, a manufacturing-informed design approach has the potential to yield the most benefit from advanced manufacturing. By leveraging advanced materials, data science, and rapid testing and deployment, manufacturing-informed design can drive down costs and development times, ultimately improving future commercial viability. This approach is being demonstrated in the US Department of Energy Office of Nuclear Energy (DOE-NE) Transformational Challenge Reactor (TCR) program. Preconceptual design activities for TCR have been focused on analyzing and maturing four reactor core design concepts: two fast-spectrum and two thermal-spectrum systems. Furthermore, the designs were iteratively modified and analyzed, and subcomponents were manufactured in parallel over weeks instead of months or years. To meet key program initiatives (e.g., timeline and material use), several constraints—including fissile material availability, component availability, materials compatibility, and additive manufacturing capabilities—were factored into the design effort, yielding small cores less than one cubic meter in volume with near-term viability. Additionally, the TCR program has made significant progress on development of advanced moderator materials such as yttrium hydride, advancing the feasibility of gas-cooled thermal spectrum systems using less than 250 kg of high-assay low enriched uranium (HALEU) and occupying less than 1 m3. Each of the two resulting thermal designs uses a different fuel form: traditional UO2 ceramic fuel and tristructural isotropic (advanced TRISO) fuel particles embedded inside a SiC matrix. Core neutronics and thermal performance for these systems were assessed and summarized. Evaluation of the performance metrics for these two moderated designs has yielded the downselected TCR design: a TRISO-fueled and yttrium hydride moderated gas-cooled reactor.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Exploring diversion-pathway analysis of a generic molten-salt fast reactor using multiphysics informed signatures

Molten salt reactors are being explored by multiple commercial ventures due to their inherent safety features, flexibility in fuel sources, and high fuel utilization and thermal efficiency. The continual flow of fuel salt, large fissile quantities present, and ability to add or divert material due to the liquid nature introduces new challenges for international safeguards. To understand how international safeguards should be applied, it is important to capture the inherent multi-physics nature of a molten salt reactor. This work examines a generic molten salt fast reactor to understand how potential diversion scenarios would affect the concentration of radionuclides in the primary and auxiliary systems. Three types of diversion were examined: a slow drip of fuel salt, gaseous plutonium extraction, and uranium metal plating. The analysis determined that several key isotopes become statistically significant once diversion begins, indicating that detection of such diversion cases would be possible through measuring specific signatures such as gamma spectra.

22 - GENERAL STUDIES OF NUCLEAR REACTORS↗