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At least 343 records · Page 19

Physical aging in graphite/epoxy composites

Sub-Tg annealing has been found to affect the properties of graphite/epoxy composites. The network epoxy studied was based on the chemistry of tetraglycidyl 4,4'-diamino-diphenyl methane (TGDDM) crosslinked by 4,4'-diamino-diphenyl sulfone (DDS). Differential scanning calorimetry, thermal mechanical analysis, and solid-state cross-polarized magic-angle-spinning nuclear magnetic resonance spectroscopy have been utilized in order to characterize this process of recovery towards thermodynamic equilibrium. The volume and enthalpy recovery as well as the 'thermoreversibility' aspects of the physical aging are discussed. This nonequilibrium and time-dependent behavior of network epoxies are considered in view of the increasingly wide applications of TGDDM-DDS epoxies as matrix materials of structural composites in the aerospace industry.

Kong, E. S. W.↗

Self-diffusion of liquid deuterium hydride and liquid tritium

Here, we present a quasi-elastic neutron scattering study of liquid deuterium hydride carried out using the Disk Chopper Spectrometer at the National Institute of Standards and Technology. Under saturated vapor pressure, the self-diffusion constant of deuterium hydride obeys an Arrhenius law D = D 0 exp(-E A /k B T), where the prefactor D 0 is given by D 0 = 9.5 ± 1.2 Å 2 /ps and the activation energy is given by E A = 58 ± 2 K. We apply the quantum law of corresponding states to the known diffusion constants of the hydrogen isotopologues. From this application, we estimate that D 0 ≈ 9.1 Å 2 /ps and E A ≈ 75 K in liquid tritium. Young’s theory of quantum-mechanical effects in van der Waals fluids is shown to apply to the diffusion constants of the liquid hydrogens. Our results underscore the importance of nuclear quantum effects in shaping the properties and behavior of the hydrogen isotopologues.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Examination of actinide chemistry at solid-water interfaces to support advanced actinide separations (Final Report)

In this work we have examined the thermodynamics of actinide interactions with solid interfaces in the presence and absence of multi-functional complexing ligands. The term “interactions” is a global term to capture many potential reactions including aqueous complexation, sorption/surface complexation, surface-mediated redox reactions, electrostatic attraction and repulsion, surface passivation, surface precipitation, and counter-ion competition. Each of these potential reactions may control actinide interactions with a solid surface. This work is helping to develop a more fundamental understanding of actinide bonding at solid:water interfaces and examine unique surface mediated oxidation/reduction reactions which are not expected based on the reduction potentials of aqueous species. We place a large emphasis on understanding both sorption and desorption processes as a means of understanding the sorption mechanisms. This work is directly aligned with the DOE BES Heavy Element Chemistry programs interests in understanding “the chemical and physical properties of these elements to determine solution, interfacial and solid-state bonding and reactivity”.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Radiation Transport Properties of Potential In Situ-Developed Regolith-Epoxy Materials for Martian Habitats

Mission crews in space outside the Earth s magnetic field will be exposed to high energy heavy charged particles in the galactic cosmic radiation (GCR). These highly ionizing particles will be a source of radiation risk to crews on extended missions to the Moon and Mars, and the biological effects of and countermeasures to the GCR have to be investigated as part of the planning of exploration-class missions. While it is impractical to shield spacecraft and planetary habitats against the entire GCR spectrum, biological and physical studies indicate that relatively modest amounts of shielding are effective at reducing the radiation dose. However, nuclear fragmentation in the shielding materials produces highly penetrating secondary particles, which complicates the problem: in some cases, some shielding is worse than none at all. Therefore the radiation transport properties of potential shielding materials need to be carefully investigated. One intriguing option for a Mars mission is the use of material from the Martian surface, in combination with chemicals carried from Earth and/or fabricated from elements found in the Martian atmosphere, to construct crew habitats. We have measured the transmission properties of epoxy-Martian regolith composites with respect to heavy charged particles characteristic of the GCR ions which bombard the Martian surface. The composites were prepared at NASA Langley Research Center using simulated Martian regolith, in the process also evaluating fabrication methods which could lead to technologies for in situ fabrication on Mars. Initial evaluation of the radiation shielding properties is made using radiation transport models developed at NASA-LaRC, and the results of these calculations are used to select the composites with the most favorable radiation transmission properties. These candidates are then evaluated at particle accelerators which produce beams of heavy charged particles representative in energy and charge of the radiation at the surface of Mars. The ultimate objective is to develop the models into a design tool for use by mission planners, flight surgeons and radiation health specialists.

Miller, Jack↗

Survey of Modeling and Simulation Techniques for Advanced Manufacturing Technologies Volume II – Predicting Material Performance from Material Microstructure

This report describes the current state of modeling and simulation techniques for predicting the properties of materials fabricated with advanced manufacturing techniques, given the initial microstructure of the material. The report includes a literature survey and a gap analysis outlining and prioritizing key issues in applying these modeling and simulation techniques to nuclear reactor structural materials. The discussion covers both physics-based and data-driven modeling techniques and includes a broad range of manufacturing techniques and materials that may have future nuclear applications. This report is the second in a two-part series, with the first report covering modeling and simulation methods for predicting the initial, as-manufactured structure of advanced manufacturing materials, given a description of the process. Both reports focus on a set of manufacturing technologies likely to be applied to reactor structural components. Taken together, the two reports provide a complete summary of the current state of processing-structure-properties models for advanced manufacturing as well as a survey of applications to reactor structural materials

42 ENGINEERING↗

Corrosion-Resistant Coatings for Mitigation and Repair of Spent Nuclear Fuel Dry Storage Canisters

This report summarizes the results of a literature survey on coatings and surface treatments that are used to provide corrosion protection for exposed metal surfaces. The coatings are discussed in the context of being used on stainless steel spent nuclear fuel (SNF) dry storage canisters for potential prevention or repair of corrosion and stress corrosion cracking. The report summarizes the properties of different coating classes, including the mechanisms of protection, their physical properties, and modes of degradation (thermal, chemical, radiological). Also discussed are the current standard technologies for application of the coatings, including necessary surface pretreatments (degreasing, rust removal, grinding) and their effects on coating adhesion and performance. The coatings are also classified according their possible use for in situ repair; ex situ repair, requiring removal from the overpack; and ex situ prevention, or application prior to fuel loading to provide corrosion protection over the lifetime of the canister.

36 MATERIALS SCIENCE↗

The Neutron Star Zoo

Neutron stars are a very diverse population, both in their observational and their physical properties. They prefer to radiate most of their energy at X-ray and gamma-ray wavelengths. But whether their emission is powered by rotation, accretion, heat, magnetic fields or nuclear reactions, they are all different species of the same animal whose magnetic field evolution and interior composition remain a mystery. This article will broadly review the properties of inhabitants of the neutron star zoo, with emphasis on their high-energy emission. XXX Neutron stars are found in a wide variety of sources, displaying an amazing array of behavior. They can be isolated or in binary systems, accreting, heating, cooling, spinning down, spinning up, pulsing, flaring and bursting. The one property that seems to determine their behavior most strongly is their magnetic field strength, structure and evolution. The hot polar caps, bursts and flares of magnetars are likely due to the rapid decay and twisting of their superstrong magnetic fields, whose very existence requires some kind of early dynamo activity. The intermediate-strength magnetic fields of RPPs determines their spin-down behavior and radiation properties. However, the overlap of the magnetar and RPP populations is not understood at present. Why don't high-field RPPs burst or flare? Why don't lower-field magnetars sometimes behave more like RPPs? INS may be old magnetars whose high fields have decayed, but they do not account for the existence of younger RPPs with magnetar-strength fields. Not only the strength of the magnetic field but also its configuration may be important in making a NS a magnetar or a RPP. Magnetic field decay is a critical link between other NS populations as well. "Decay" of the magnetic field is necessary for normal RPPs to evolve into MSPs through accretion and spin up in LMXBs. Some kind of accretion-driven field reduction is the most likely mechanism, but it is controversial since it is not clear how effective it is or on what timescale a buried field might re-emerge. One piece of evidence in favor of accretion-driven field reduction is the fact that NSs in LMXBs, which are older systems (> 108 yr), have mostly low fields and NSs in HMXBs, which are younger systems (107 − 108 yr), have higher fields. This may be an indication that accretion-driven field reduction or decay has not had enough time to operate in HMXBs but has in LMXBs. However, there does not seem to be any evidence of decaying fields in either the LMXB or HMXB populations; e.g. smaller magnetic fields in older systems. On the other hand, CCOs are very young so if they acquired their low fields through mass fallback accretion, the field submergence would have had to operate on much faster timescales than it apparently does in LMXBs. But as we continue to find new species in the NS zoo, one of these may someday be the "Rosetta Stone" that will give us the clues for solving these puzzles.

Zoo↗

In situ irradiation of spent nuclear fuels

To improve the economics of commercial nuclear reactors, nuclear vendors and utilities are seeking approval for increased burnup usage of the existing nuclear fleet. This is especially critical for meeting the clean energy initiative by the United States Government, Department of Energy (DOE). However, one of the key challenges the nuclear industry faces in this regard is that the regions exposed to high burnup and low temperatures exhibit a fine-grained microstructure with large bubbles known as high-burnup structure (HBS) [1]. The formation of HBS has been correlated to the diminished performance of the reactor, as well as fuel fragmentation and pulverization during transient and accidental conditions [2]. Therefore, it is paramount to understand the mechanisms for HBS formation along with its impact on the properties and performance of nuclear fuels. While existing programs, such as Nuclear Energy Advanced Modeling and Simulation (NEAMS) and Advanced Fuel Campaign (AFC) are focusing on evaluating the performance impact of HBS, the physical mechanisms contributing to HBS formation are still not fully understood. In addition, having predictive capabilities and sound understanding of the microstructural evolution of nuclear fuel is essential for accelerated development, qualification, and deployment of new nuclear materials and novel reactor designs for advanced nuclear reactors. There is a lack of consensus among researchers regarding the mechanisms leading to such restructuring observed in HBS. Grain subdivision due to polygonization versus recrystallization, continuous versus discrete recrystallization occurring in tandem or conjunction, etc., have been proposed and debated. In general, it is hypothesized that defect accumulation and dislocation interaction within the grains cause the realignment of dislocations into grain boundaries, leading to the new subgrain formation, which over time transforms into new grains. However, due to the lack of transient data, the importance of fission rate, irradiation, thermal, and stress history of the fuel on the restructuring could not be assessed. In situ microstructural evolution under various irradiation conditions is desired to bridge this gap. Alternatively, phase-field-based models have been developed to capture HBS formation via discrete recrystallization utilizing the classical nucleation approach [3–5]. However, in these models, the grain nucleation criteria are often defined based on empirical relations for burnup and fission gas density leading to dislocation density change. A mechanistic approach to capture the dislocation interaction with the microstructural features leading to grain subdivision is lacking.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission Evaluation Tools and Analytics (FETA)

This living document presents the Python package FETA. FETA computes observables resulting from the fission process. This document provides the definition of these observables as well as the physics models that are implemented to compute them. Some of these models are used to determine the initial conditions of fission fragments, e.g., the excitation energy E* and spin distribution p(J, π) at scission for prompt decay, while others are related to the nuclear structure and decay properties of the fragments, e.g. the ground-state properties, level density and low-lying excitation spectrum, γ-strength functions and electromagnetic transitions, and neutron transmission coefficients. The end goal for FETA is to enable users to substitute every one of these models by their own files providing these quantities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Spectroscopic Signatures of MQ-Resins in Silicone Elastomers

Polysiloxane elastomers have a large application space due to their versatile cross-linking chemistry and highly tunable physical and mechanical properties. One approach for improving the mechanical integrity of commercial polysiloxane “silicone” elastomers while maintaining their optical transparency is the addition of small, silicone-resin molecules to the network. However, both the poly(dimethylsiloxane) (PDMS) network and the silicone-resin particles have an amorphous structure and complex chemistry, which makes the characterization of their structural properties and segmental network dynamics difficult. Here, we report the synthesis and characterization of a series of model silicone networks modified with a specific class of silicone-resin known as MQ-resin using Raman and advanced nuclear magnetic resonance (NMR) spectroscopy methods. Raman spectroscopy was successfully used to quantify the contribution of the MQ-resin to the network, to determine the type of MQ-resin present in the network, and to investigate the completeness of the network cross-linking reaction. Furthermore, solid-state and 1H double-quantum (DQ) NMR spectroscopies were used not only as a detection method for the MQ-resins but also to quantify changes in the segmental dynamics of the network as a function of MQ-resin concentration. The combination of Raman and NMR spectroscopies describes a series of samples where the MQ-resin particles and PDMS chains maintain their independent segmental dynamics up to high concentrations of MQ-resins (40–50% MQ), where the physical properties of the resin dominate the physical properties of the overall network. The results from our spectroscopic analyses are consistent with the results from macroscopic characterization techniques such as solvent uptake and mechanical testing. The spectroscopic insights into the structure–property relationships of PDMS-MQ composites presented in this study are a valuable tool not only for the synthesis and reverse engineering of future generations of commercial silicone elastomers but also for understanding the mechanisms of aging and degradation over the material lifetime.

36 MATERIALS SCIENCE↗

Impact of f-element complexation on the radiolytic robustness of separations ligands

Impact of f-element complexation on the radiolytic robustness of separations ligands Gregory P. Horne, Makayla R. Baxter, Corey D. Pilgrim, Travis S. Grimes, Center for Radiation Chemistry Research, Idaho National Laboratory, P.O. Box 1625, Idaho Falls, ID, 83415, USA Cristian Celis Barros, Department of Chemistry and Biochemistry, Florida State University, Tallahassee, FL 32306, USA. E-mail: ccelisbarros@fsu.edu Andrew R. Cook, Department of Chemistry, Brookhaven National Laboratory, Upton, New York, 11973, USA Stephen P. Mezyk, Department of Chemistry and Biochemistry, California State University Long Beach, 1250 Bellflower Boulevard, Long Beach, California, 90840-9507, USA The effects of ionizing radiation are ubiquitous throughout all aspects of a nuclear fuel cycle. However, the complexity and intensity of these effects are greatest during the management of used nuclear fuel, owing to the presence of a wide spectrum of radionuclides from neutron capture and fission processes. With regards to used nuclear fuel (UNF) reprocessing, radiation-induced processes typically promote the destruction of active compounds (e.g., complexants and additives) with the concomitant formation of potentially detrimental degradation products and corresponding changes in physical and chemical properties, which ultimately impact the effectiveness and longevity of a given reprocessing system. Concerning UNF complexants, radiation chemistry studies have historically focused on their radiation robustness in the absence of the metal ions they were designed to selectively complex. This knowledge gap is worrisome as previous studies on aqueous phase complexants have demonstrated significant changes in radiolytic behavior upon metal ion complexation.1-4 More recently, the rate of reaction of the n-dodecane radical cation—believed to be the major organic phase radiation-induced transient species responsible for complexant radiolysis in n-dodecane based solvent systems—with hexa-n-octylnitrilo-triacetamide (HONTA) was shown to increase by an order-of-magnitude upon complexation of europium or americium.5 These findings have significant implications on the projected longevity of complexants in UNF reprocessing solvent systems. Consequently, a thorough understanding of metal ion complexation effects on the radiolytic integrity of UNF complexants is essential to evaluate their potential for process application. Presented here are two recent studies from the Idaho National Laboratory Center for Radiation Chemistry Research group that demonstrate the various impacts of f-element complexation (uranium, americium, and lanthanides) on the radiolytic integrity (gamma and electron pulse) of tributyl phosphate (TBP), N,N-di-(2-ethylhexyl)butyramide (DEHBA), N,N-di-2-ethylhexylisobutryamide (DEHiBA), and 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP]) under UNF reprocessing conditions. References 1) Bhattacharyya and Kundu, Int. J. Radiat. Phys. Chem., 1971, 3, 1. 2) Kundu and Matuura, Int. J. Radiat. Phys. Chem., 1975, 7, 565. 3) Ilan and Czapski, Biochimica et Biophysica Acta, 1977, 498, 386. 4) Buettner, Doherty, and Patterson, Fed. Euro. Biochem. Soc., 1983, 158 (1), 143. 5) Toigawa, Peterman, Meeker, Grimes, Zalupski, Mezyk, Cook, Yamashita, Kumagai, Matsumura, Horne, PCCP, 2021, 23, 1343.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Benchmarking MELCOR's NAC Package to ABCOVE Test AB7

This report presents analyses of the AB7 ABCOVE sodium spray fire experiment with the MELCOR code. This code simulates the progression of accident events for analysis and auditing purposes of nuclear facilities during accident conditions. Historically, the ABCOVE experiments have contributed to the validation of aerosol physics and related phenomena. Given advancements in sodium-cooled reactor designs, characterization of the sodium spray combustion may further the review and validation of newly incorporated sodium properties and physics packages, namely, the sodium equations of state (EOS) and the sodium combustion (NAC) package within MELCOR. Previously, the AB5 and AB6 experiments were analyzed with and without the NAC package. This work builds on the previous analyses with a demonstration of the current code capabilities of MELCOR with a more mild Na spray and pool fire scenario.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Unravelling the radiation-induced redox chemistry of plutonium ions in aqueous solution

Plutonium plays a critical role in nuclear fuel cycle technologies, but our understanding of its fundamental radiation-induced redox chemistry is limited. Changes in oxidation states affect the speciation and transport of plutonium ions in solution. For example, solvent extraction techniques used to separate and recover plutonium from used nuclear fuel rely on the selective formation, maintenance, and complexation of specific plutonium oxidation states. However, radiolytically generated radicals, ions, and molecules can drive the oxidation state distribution of plutonium ions far from equilibrium, ultimately changing the physical and chemical properties of the bulk system. These radiation-induced processes are inevitable due to the ionizing radiation fields generated by the radioactive decay of plutonium and its daughter nuclides. Therefore, mechanistically understanding how plutonium's various oxidation states respond to ionizing radiation is essential for predicting its behavior in solution. Here, we present significant advances in our understanding of radiation-induced plutonium redox chemistry by using time-resolved (electron pulse) and dose accumulation (alpha and gamma) irradiation techniques, along with quantitative multiscale modeling methods.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Properties of Medium Nuclei from First Principles

During this project we have extended the Auxiliary Field Diffusion Monte Carlo (AFDMC) to calculate several properties of light/medium nuclei. In particular, we have included and tested several models of three-body forces and the associated approximations required, and the comparison with other exact calculations for simpler problems demonstrated the accuracy of the AFDMC method. In this project we have also developed new subroutines to solve for the ground-state of open shell nuclei. This case requires very complex wave function with respect to the case of closed-shell nuclei. We have used the AFDMC code to calculate many properties of nuclei up to the Oxygen, including energies, radii, spatial and momentum distributions and others.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Multiscale Modeling of Silicon Carbide Cladding for Nuclear Applications: Thermal Performance Modeling

The complex multiscale and anisotropic nature of silicon carbide (SiC) ceramic matrix composite (CMC) makes it difficult to accurately model its performance in nuclear applications. The existing models for nuclear grade composite SiC do not account for the microstructural features and how these features can affect the thermal and structural behavior of the cladding and its anisotropic properties. In addition to the microstructural features, the properties of individual constituents of the composites and fiber tow architecture determine the bulk properties. Models for determining the relationship between the individual constituents’ properties and the bulk properties of SiC composites for nuclear applications are absent, although empirical relationships exist in the literature. Here, a hierarchical multiscale modeling approach was presented to address this challenge. This modular approach addressed this difficulty by dividing the various aspects of the composite material into separate models at different length scales, with the evaluated property from the lower-length-scale model serving as an input to the higher-length-scale model. The multiscale model considered the properties of various individual constituents of the composite material (fiber, matrix, and interphase), the porosity in the matrix, the fiber volume fraction, the composite architecture, the tow thickness, etc. By considering inhomogeneous and anisotropic contributions intrinsically, our bottom-up multiscale modeling strategy is naturally physics-informed, bridging constitutive law from micromechanics to meso-mechanics and structural mechanics. The effects that these various physical attributes and thermo-physical properties have on the composite’s bulk thermal properties were easily evaluated and demonstrated through the various analyses presented herein. Since silicon carbide fiber-reinforced SiC CMCs are also promising thermal–structural materials with a broad range of high-end technology applications beyond nuclear applications, we envision that the multiscale modeling method we present here may prove helpful in future efforts to develop and construct reinforced CMCs and other advanced composite nuclear materials, such as MAX phase materials, that can service under harsh environments of ultrahigh temperatures, oxidation, corrosion, and/or irradiation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Selection and Characterization of Surrogate Material for Developing Zr Barrier Coatings for Uranium Nitride Particles

In support of UC 1-x N x fuel kernels (~ 800 micrometer diameter) development work ongoing at Oak Ridge national laboratory (ORNL), where the fuel kernels will be embedded inside a possible zirconium based matrix, Argonne National Laboratory (ANL) is contributing to help develop a robust metal diffusion barrier coating. Zirconium nitride (ZrN) and Zirconium oxide (ZrO2) were selected as possible diffusion barrier candidates, and the atomic layer deposition (ALD) has been chosen as a candidate technology to deposit the film. Development of such a barrier coating with the ALD process entails significant number of trials to study relevant parameters. Therefore, to prevent needless wastage, instead of coating directly over fuel kernels, a surrogate candidate with similar dimensions and physical properties were been selected and coated to develop the diffusion barrier coating.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of Aluminum Metal Powders for Plutonium-238 Program

As part of radioisotope thermoelectric generator (RTG) production for power sources in deep space exploration, Oak Ridge National Laboratory (ORNL) produces plutonium-238 ( 238 Pu). To produce 238 Pu, neptunium-237 ( 237 Np) targets are fabricated at ORNL and subsequently irradiated at the High Flux Isotope Reactor (HFIR) at ORNL and the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). Specifically, current flowsheets utilize neptunium dioxide ( 237 NpO 2 ) targets. Aluminum (Al) powder is blended with 237 NpO 2 target material to improve thermal conductivity during irradiation. The current composition of 237 NpO 2 /Al pellets (i.e., cermets, or ceramic–metallics) is 20% 237 NpO 2 , 70% Al, and 10% void space. Al powders utilized by the 238 Pu program are high-fired under vacuum before blending into targets. The primary objective of this work is to measure the physical, chemical, and thermal properties of Al before and after the high-firing process. Properties of interest include the morphology, surface texture, particle size, crystal phase(s), and thermal conductivity of the material. These properties are measured with existing materials characterization equipment at ORNL, including powder x-ray diffraction (pXRD), scanning electron microscopy (SEM) with energy-dispersive spectroscopy (EDS), laser flash analysis (LFA), and thermogravimetric analysis (TGA). A secondary objective of this work is to compare the Al powders before and after the high-firing procedure to determine the effects of high-firing on chemical, physical, and thermal properties and to determine the efficacy of the high-firing process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗