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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Understanding the Hydronium Cation in the Solid State: A Study in Synthetic Hydronium Uranyl Phosphate and Arsenate Mineral Systems and Their Irradiation Stability

Here, we present neutron diffraction, electronic structure calculations, and optical vibrational spectroscopic characterization of hydronium uranyl phosphate (HUP), the synthetic analog of chernikovite ((H 3 O)(UO 2 )(PO 4 )·3H 2 O) to gain insight into structural features of the hydronium cation in the solid state. HUP crystallizes in P2 1 /c instead of previously reported P4/ncc 1 at room temperature and Pccn below 302 K. Lower symmetry was required due to hydronium and interstitial water positions within the structure. Crystallographic positions of hydronium cations determined from powder neutron diffraction data are bolstered by Raman and attenuated total reflectance infrared spectroscopic measurements and are further informed by density functional theory with phonon eigenvector analysis for spectral assignments. Finally, HUP and its arsenate analog (trogerite, (H 3 O)(UO 2 )(AsO 4 )·3H 2 O), (HUAs) were studied using He 2+ irradiation as an analog for α radiolysis to investigate the irradiation stability of these phases and the stability of hydronium cations in the solid state. Dose studies were employed wherein each sample was irradiated to 5, 10, 15, 25, and 50 MGy. Structural insight regarding irradiated materials is gained using optical vibrational spectroscopy and powder X-ray diffraction. Surprising irradiation stability of HUAs was found up to 50 MGy of dose, which may have important implications for understanding and modeling the geologic stability of legacy U.

actinides↗

Irradiation stability and thermomechanical properties of 3D-printed SiC

Neutron irradiation tests were carried out on 3D-printed SiC derived from binderjet additive manufacturing and chemical vapor infiltration. Irradiation was carried to 2.3 dpa over a temperature range of 400–850 °C. Anisotropy that had been observed in the thermal conductivity of 3D-printed SiC prior to irradiation vanished after irradiation as the irradiation defect thermal resistivity accumulated in the material. No degradation in strength was observed in the material before or after irradiation, at various temperatures, or in different orientations. Electron microscopy of the microstructure after neutron irradiation showed distinct defect morphologies in the heterogenous material, but no evidence for irradiation-induced cracking or degradation in the microstructure was observed.

36 MATERIALS SCIENCE↗

EPR Investigation of Temporal and Thermal Stability of Irradiated Sweeteners

Abstract Electron paramagnetic resonance was used to study the dosimetric properties of commercial sweeteners (sucrose, saccharin, and stevia). The results concluded that sugar has dosimetric properties of interest, which makes it suitable for dose reconstruction, emergency response, and nuclear forensics applications. The radiation dose response was investigated by irradiating samples up to 10 Gy and found to be linear. The post-irradiation stability of samples was observed to be useful for the intended applications. The results showed that the post-irradiation intensities vary from one sample to another, with the general trend demonstrating a small increase in intensities shortly after irradiation followed by an approximately constant leveling out. Finally, the effect of isochronal annealing was studied by heating samples to various temperatures. The results showed an overall stable behavior of the signal below melting temperature.

Environmental Sciences & Ecology↗

Microstructural stability of irradiated yttrium hydride under thermal cycles

Hydrides that retain their hydrogen in service are critical for advanced microreactor and space nuclear systems. Hydrogen retention is affected by evolving microstructure under temperature and irradiation extremes. This study investigated microstructural features in neutron-irradiated yttrium hydride and the stability of these features under thermal cycles. Differential scanning calorimetry was used to determine hydrogen desorption and temperatures at which significant phase changes are occurring, and transmission electron microscopy was used for microstructural analysis after each thermal cycle. Cyclic heating led to crystallization and epitaxial growth of surface oxidation and dehydriding of the matrix. Other features such as the bulk matrix crystal structure, irradiation-induced cavities, and matrix precipitation remained constant after thermal cycling. Results allow us to design better hydride alloys through microstructure tailoring and potential irradiation conditioning treatments.

36 MATERIALS SCIENCE↗

Nonequilibrium defect-phase nanostructures stabilized by irradiation in undersaturated Ni-Si nanocrystalline alloy

Nanocrystalline thin films of the undersaturated alloy Ni-8.5 at% Si were subjected to 2 MeV Ti irradiation at temperatures ranging from 450˚C to 550˚C. Correlative microscopy combining transmission electron microscopy (TEM), scanning-TEM and atom probe tomography (APT revealed that large dose irradiation at 450˚C of samples with initial grain sizes below 100 nm stabilized a novel nanostructure which surprisingly contained three co-existing phases, the γ face-centered-cubic (FCC) matrix, γ' L12 ordered precipitates on intragranular dislocation loops and Ni 31 Si 12 precipitates at triple junctions (TJs). In contrast, irradiation at 550˚C and irradiation of larger grain-size samples at 450˚C only produced a γ-γ' two-phase coexistence. Analysis of the three-phase nanostructure and phase field simulations indicates that radiation-induced segregation is most pronounced at TJs, thus triggering the formation of Ni 31 Si 12 precipitates. These incoherent precipitates, in turn, are expected to stabilize the grain size under irradiation. The results are generalized using the concept of driven defect-phases. It is suggested that the stabilization of driven defect-phases may impart radiation resilience by providing localized relaxation modes to the microstructure evolution during and after temporary perturbations in irradiation conditions.

36 MATERIALS SCIENCE↗

Microstructure-dependent rate theory model of defect segregation and phase stability in irradiated polycrystalline LiAlO 2

We report gamma lithium aluminate (LiAlO 2 ) is a breeder material for tritium and is one of key components in a tritium-producing burnable absorber rod (TPBAR). Dissolution and precipitation of second phases such as LiAl 5 O 8 and voids are observed in irradiated LiAlO 2 . Such microstructure changes cause the degradation of thermomechanical properties of LiAlO 2 and affect tritium retention and release kinetics, and hence, the TPBAR performance. In this work, a microstructure-dependent model of radiation-induced segregation (RIS) has been developed for investigating the accumulation of species and phase stability in polycrystalline LiAlO 2 structures under irradiation. Three sublattices (i.e. [Li, Al, V] I [O, V o ] II [Li i , Al i , O i , V i ] III ), and concentrations of six diffusive species (i.e. Li; vacancy of Li or Al at [Li, Al, V] I sublattice, O vacancy at [O, V o ] II sublattice, and Li, Al and O interstitials at [Li i , Al i , O i , V i ] III interstitial sublattices; are used to describe spatial and temporal distributions of defects and chemistry. Microstructure-dependent thermodynamic and kinetic properties including the generation, reaction, and chemical potentials of defects and defect mobility are taken into account in the model. The parametric studies demonstrated the capability of the developed RIS model to assess the effect of thermodynamic and kinetic properties of defects on the segregation and depletion of species in polycrystalline structures and to explain the phase stability observed in irradiated LiAlO 2 samples. The developed RIS model will be extended to study the precipitation of LiAl 5 O 8 and voids and tritium retention by integrating the phase-field method.

36 MATERIALS SCIENCE↗

Microstructural evolution and hardness changes in ion irradiated nickel-based Haynes 282 superalloy

This study investigated the crucial aspects of thermal and irradiation stability in precipitation hardened Haynes 282 Ni-based superalloy. The Haynes 282 Ni-based alloy was irradiated by 8 MeV Ni 3+ ions to assess its resistance to phase instabilities and mechanical property alterations. The mid-range doses (at a depth of ∼1 µm) were 1 and 10 displacements per atom (dpa) at temperatures of 600°C and 750°C. Nanoindentation tests provided insights into bulk equivalent hardness of the irradiated and pristine regions, while scanning transmission electron microscopy (STEM) and energy dispersive X-ray spectroscopy (EDS) were used to examine the microstructural evolution of irradiation-induced defects and γ′ -Ni 3 (Al, Ti) precipitates and defect structure under irradiation. These precipitates, with an average diameter of 29 nm and a number density of 5 x 10 21 /m 3 , acted as robust dispersion strengthening agents with high radiation point defect sink strength. Remarkably, irradiation did not significantly alter the size or number density of the γ′ precipitates, indicating exceptional thermal stability and radiation resistance of these precipitates at the examined conditions. Radiation-induced dislocation loops were observed at 600°C, albeit without a substantial impact on mechanical properties due to the dominance of γ′ precipitates on the overall alloy strength. The superior stability of γ′ precipitates observed in this study contrasts with several previous research findings on Ni-based alloys that reported poor precipitate stability. Plausible reasons for this difference are discussed. Moreover, this work explicitly outlines a physically grounded approach to ensure accurate microstructure-hardness correlations and clarifies the hardening model by addressing common misapplications of superposition in prior studies.

36 MATERIALS SCIENCE↗

Post-irradiation Examination Status for the BSU-269 Project

High-density uranium inter-metallic uranium silicide (U 3 Si 2 ) was initially considered as a potential advanced nuclear fuel for light water reactor (LWR) systems due to several advantages it demonstrated in thermophysical properties, chemical, and irradiation stability. In addition to understanding the basic thermophysical and mechanical properties of U 3 Si 2 under LWR irradiation conditions, it is important to assess its performance with advanced claddings such as FeCrAl, SiC, or conventional Zr-based claddings. Several aspects of the fuel cycle and fuel performance are being evaluated for U 3 Si 2 coupled with different types of claddings. To thoroughly characterize the U 3 Si 2 -cladding system, their chemical compatibilities and the potential for fuel-cladding chemical interaction (FCCI) must be addressed. Interdiffusion studies have been performed between U 3 Si 2 /Zry-4 and U 3 Si 2 /FeCrAl using diffusion couples. For the U 3 Si 2 /Zry-4 system, ZrSi 2 was the primary interdiffusion product observed at 800°C in addition to other secondary phases from the Zr alloying elements such as Fe and Cr. Low melting point U 6 Fe was also observed at 1000°C. For the U 3 Si 2 /FeCrAl system, at temperatures above 500°C, chemical diffusion Fe-U and Fe-U-Si was observed, increasing with rising temperatures. Although information from these non-irradiated tests is a fundamental first assessment, follow-up with focused irradiation tests is necessary. Irradiation can significantly alter the structure and evolution of the FCCI layers compared to the non-irradiated conditions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Radiation-resistant metal-organic framework enables efficient separation of krypton fission gas from spent nuclear fuel

Capture and storage of volatile radionuclides that result from processing of used nuclear fuel is a major challenge. Solid adsorbents, in particular ultra-microporous metal-organic frameworks, could be effective in capturing these volatile radionuclides, including 85 Kr. However, metal-organic frameworks are found to have higher affinity for xenon than for krypton, and have comparable affinity for Kr and N 2 . Also, the adsorbent needs to have high radiation stability. To address these challenges, here we evaluate a series of ultra-microporous metal-organic frameworks, SIFSIX-3-M (M = Zn, Cu, Ni, Co, or Fe) for their capability in 85 Kr separation and storage using a two-bed breakthrough method. These materials were found to have higher Kr/N 2 selectivity than current benchmark materials, which leads to a notable decrease in the nuclear waste volume. The materials were systematically studied for gamma and beta irradiation stability, and SIFSIX-3-Cu is found to be the most radiation resistant.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Boride-based Ceramic Super-high Temperature Thermocouples in Harsh Environments (Final Scientific/Technical Report)

An electromotive force (emf) can be generated along a temperature gradient between the cold end and hot end of a thermoelectric material, termed the Seebeck effect. Based on the Seebeck effect, metallic alloys have been extensively employed to detect temperatures for centuries, named thermocouples. However, commercially available thermocouple alloys suffer from limitations, such as oxidation, chemical degradation, and poor long-term stability under high-temperature harsh environments. This DOE-funded project aimed to develop high-temperature, chemically tolerant thermocouples suitable for operation in extreme environments relevant to semiconducting thermoelectric materials. The research focused on boride-based semiconducting thermoelectric compounds as candidates for next-generation thermocouples with enhanced oxidation resistance, chemical stability, and thermal robustness under conditions representative of charcoal-fired electricity facilities. During the funded years, boride materials were synthesized using an arc-plasma technique under ambient air and argon atmospheres, enabling scalable and cost-effective production compared with conventional boride fabrication methods. The synthesized borides were processed into nanostructured powders, followed by consolidation into dense bulk materials using a spark plasma sintering (SPS) bottom-up approach. Comprehensive characterization was performed, including microstructural analysis, electrical transport measurements, and optical and thermal property evaluation. Both p-type and n-type boride electric legs were fabricated and integrated into boride-based thermocouples. The thermal and irradiation stabilities of the boride nanomaterials and bulk thermoelectric materials were systematically evaluated to assess suitability for long-term operation in harsh environments. Additionally, 12 students were broadly hands-on trained spanning the full research workflow, including word processing and technical editing (e.g., LATEX for manuscript and poster preparation), data collection and analysis (using Python and related libraries and hardware interfaces), sample preparation (including arc-plasma synthesis and spark plasma sintering), and advanced characterization techniques (such as X-ray diffraction, UV–vis spectroscopy, electron microscopy, differential thermal analysis (DTA), and Seebeck coefficient measurements, etc). Overall, this project demonstrated the feasibility of boride-based thermoelectric materials as durable high-temperature thermocouples, providing a promising pathway toward robust temperature sensing technologies aligned with DOE energy infrastructure and extreme-environment monitoring needs.

20 FOSSIL-FUELED POWER PLANTS↗

Multiscale Modeling of the Mechanical Response of Silicon Carbide Composite Within the Accelerated Fuel Qualification Framework

The accelerated fuel qualification (AFQ) framework has been used for the initial development of multiscale modeling of silicon carbide (SiC) fiber reinforced composite (SiC-SiC). The AFQ framework provides a methodology to leverage physics-informed multiscale modeling along with a reduced set of empirical test data to reduce the time and cost of licensing and qualification of new nuclear fuel systems while maintaining the overall nuclear power plant safety case. SiC-SiC is being proposed for in-core applications, most notably fuel cladding, for current and next-generation nuclear reactors because of its high temperature stability, irradiation tolerance, and ability to withstand many accident conditions. As these composites exhibit multiscale architectures and complex microstructure-based fracture mechanics, it is an appealing use case for the AFQ methodology. While the end goal of this work is a single multiscale model that can be used for predictive in-core performance, current focus is on the individual various length scale models. Four individual models have been initially developed from microscale to engineering system level to capture key physics-based effects across different length scales. These models include a microscale homogenized tow model, a mesoscale fast Fourier transform–based weave model that integrates the homogenized tow model, a mesoscale finite element–based weave model, and a system-level BISON fuel performance model. Results of these models have undergone an initial comparison with separate-effects test data showing a good match to experimental results. By using the AFQ framework during model development, several near-term benefits have been secured including a reduction in development time for the SiC-SiC cladding, more targeted irradiation testing, and a better understanding of uncertainty.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Irradiation Effects on Stability of δ-UZr2 phase in U-50 wt% Zr Alloy

U-50wt%Zr is a candidate metallic nuclear fuel with potential application in light water reactors due to its excellent thermal properties and high radiation tolerance. The Zr-rich UZr fuels possess greater swelling resistance and fission gas release characteristics compared with U-rich UZr fuels. In this current study, the δ-phase U-50wt%Zr is proton irradiated at room temperature to 1 displacement per atom (dpa) to provide insights on phase stability under irradiation conditions. High resolution characterization of Transmission Electron Microscopy (TEM) and Atom Probe Tomography (APT) characterization techniques are used to elucidate microstructural changes due to irradiation. TEM and APT results show highly oriented bcc β-Zr-rich platelet precipitates nucleating adjacent to α-U phases inside the UZr 2 matrix. Formation of this platelet morphology is characteristic of Widmänstatten structure which can be attributed to a variety of factors such as differences in thermal expansion coefficient between the phases, grain size, alloy composition, and cooling rate. The phases present are distinctly different than those observed through in situ annealing, but irradiation accelerates diffusion and phase separation kinetics. These microstructural changes in U-50wt%Zr are different from those achieved by pure thermodynamic or high temperature heavy ion irradiation experiments. Finally, our work, together with previous ones, highlight the necessity to study the U-Zr phase diagram under non-equilibrium thermodynamics conditions to support this material's deployment as a viable nuclear fuel form.

36 MATERIALS SCIENCE↗

Thermal Stability and Ion Irradiation Response of Refined Grained V – 4Cr – 4Ti

Since the 1960’s, there has been interest in V-4Cr-4Ti and similar alloys as candidates for low activation structural materials for advanced nuclear reactors. V-4Cr-4Ti was produced using arc melting and subsequently subjected to large strain extrusion machining to produce a multimodal microstructure largely composed of nanocrystalline and ultrafine grain sizes. In-situ thermal stability of the multimodal V-4Cr-4Ti to 800 °C shows the formation of vanadium carbides with negligible grain growth. In-situ dual-beam 16 KeV He+ and 1 MeV Kr2+ ion irradiation performed at 700 °C to a final dose of ~5 displacements per atom show the formation of small He cavities well distributed throughout the system, with preferential clustering at grain boundaries. This work provides insight into how the increased fraction of grain boundaries affect the simultaneous dual beam ion irradiation response of multimodal V – 4 wt.% Cr – 4 wt.% Ti at elevated temperatures. Analysis of the cavities reveal an areal density of 0.024±0.007 cavities/nm2 and swelling of 0.236% after the dual-beam ion irradiation. Nanoindentation shows a ~50% increase in hardening after the ion irradiation at 700 °C.

TEM↗

Effects of ZrN coating and heat treatment on U-Mo dispersion fuel systems under irradiation

The stability of U-Mo fuel particles embedded in an Al matrix under irradiation can be enhanced through ZrN coatings and/or heat treatment. Here, the present study investigates the irradiation behavior of fuel plates containing U-Mo fuel particles fabricated under various heat-treatment conditions and ZrN coating thicknesses. Different fission densities were also applied to each fuel plate to evaluate the effects of these variables. Results indicate that higher fission densities lead to more grain recrystallization and high burnup structure (HBS) development in the fuel particles. Heat treatment was found to mitigate the accumulation of fission gas bubbles in fuel particles at low fission densities by coarsening their grains. Fuel particles with ZrN coatings of a 1.2 μm thickness or above exhibited reduced formation of U-Mo/Al interaction layers, suggesting the existence of a critical ZrN coating thickness that minimizes the development of these layers. Fission gas bubbles were predominantly observed at grain boundaries of U-Mo fuel particles irradiated at low fission densities. Subgrain boundaries, which appeared to originate from the original grain boundaries containing fission gas bubbles or HBSs, were also observed, indicating the early stage of HBS propagation in the fuel particles.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗