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At least 253 records · Page 14

Design and validation of a fission-product source for radioactive beams

A neutron-generator-based source of fission products (nuCARIBU) is being developed to replace the existing source at Argonne National Laboratory. Neutrons generated by reaction are thermalized in a compact polyethylene [(moderator and impinge on a thin 235 U foil to produce fission products. Experiments have been conducted to verify the nuCARIBU concept and simulation results using a 4 MeV, 0.16 µ⁢A proton beam from the ATLAS accelerator irradiating a LiF neutron production target and two different simplified versions of the nuCARIBU (C 2 ⁢H 4 ) n moderator with thicknesses of 3.81 cm and 1.91 cm separating it from the enriched 235 U fission foil. Here, the emitted γ-ray peaks of 1383.93 keV ( 92 Sr), 358.0 keV ( 104 Tc), 565.992 keV ( 134 Te), and 258.411 keV ( 138 Xe) obtained from fission products are used to determine the neutron-induced fission rates in the fission foil. The measured fission rates are in good agreement with those simulated using the PHITS Monte Carlo code with user-defined neutron production cross sections based on well-known cross section data. These experimental results, consistent with the simulations, show that the current 252 Cf source (CARIBU) can be replaced by the neutron induced fission source (nuCARIBU).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Effects of Applied Interfacial Pressure on Li-Metal Cycling Performance and Morphology in 4 M LiFSI in DME

Lithium-metal anodes can theoretically enable 10x higher gravimetric capacity than conventional graphite anodes. However, Li-metal anode cycling has proven difficult due to porous and dendritic morphologies, extensive parasitic solid electrolyte interphase reactions, and formation of dead Li. We systematically investigate the effects of applied interfacial pressure on Li-metal anode cycling performance and morphology in the recently developed and highly efficient 4 M lithium bis(fluorosulfonyl)imide in 1,2-dimethoxyethane electrolyte. We present cycling, morphology, and impedance data at a current density of 0.5 mA/cm 2 and a capacity of 2 mAh/cm 2 at applied interfacial pressures of 0, 0.01, 0.1, 1, and 10 MPa. Cryo-focused ion beam milling and cryo-scanning electron microscopy imaging in cross section reveal that increasing the applied pressure during Li deposition from 0 to 10 MPa leads to greater than a fivefold reduction in thickness (and therefore volume) of the deposited Li. This suggests that pressure during cycling can have a profound impact on the practical volumetric energy density for Li-metal anodes. A “goldilocks zone” of cell performance is observed at intermediate pressures of 0.1–1 MPa. Increasing pressure from 0 to 1 MPa generally improves cell-to-cell reproducibility, cycling stability, and Coulombic efficiency. However, the highest pressure (10 MPa) results in high cell overpotential and evidence of soft short circuits, which likely result from transport limitations associated with increased pressure causing local pore closure in the separator. All cells exhibit at least some signs of cycling instability after 50 cycles when cycled to 2 mAh/cm 2 with thin 50 μm Li counter electrodes, though instability decreases with increasing pressure. In contrast, cells cycled to only 1 mAh/cm 2 perform well for 50 cycles, indicating that capacity plays an important role in cycling stability.

25 ENERGY STORAGE↗

Ferroelectric Al1 − xBxN thin films integrated on Si

Ferroelectric Al0.93B0.07N thin films are prepared (100) Si substrates. The necessary c-axis out-of-plane orientation to observe macroscopic ferroelectric switching was achieved by implementing an initial Ar/N2 plasma treatment, followed by a thin layer of AlN to initiate the desired texture and a 150 nm W layer. The plasma treatment facilitates crystallinity enhancement of the AlN template layer, allowing for subsequent growth of highly oriented W and Al0.93B0.07N layers. The W layer exhibits random in-plane orientation and exclusive (110) out-of-plane orientation with a rocking curve width of 1.4°. When grown on these W surfaces, 175 nm thick Al0.93B0.07N films exhibit random in-plane orientation and exclusive (001) texture with rocking curve full-width-half-max values of 1.6° and RMS roughness values less than 1 nm. Polarization hysteresis measurements show robust hysteresis with coercive field values of 5.4 MV/cm and remanent polarization values of 136 μC/cm2. XPS depth profile analysis suggests that the plasma treatment converts the existing native oxide to a nitrogen rich oxynitride with approximate composition Si3O0.5N3.67. Cross-sectional TEM reveals that the oxynitride interlayer is amorphous and ∼3.4 nm thick, more than double the native oxide thickness measured by multiwavelength ellipsometry, implying that (oxy)nitride growth continues after conversion of the native oxide. This new family of ferroelectric wurtzites is interesting from an integration perspective given their chemical compatibility with mainstream semiconductors. Developing synthesis routes that promote needed texture while preserving compatible processing windows is an important step toward practical integration.

Physics↗

Plug-and-play polymer microfluidic chips for hydrated, room temperature, fixed-target serial crystallography

The practice of serial X-ray crystallography (SX) depends on efficient, continuous delivery of hydrated protein crystals while minimizing background scattering. Of the two major types of sample delivery devices, fixed-target devices offer several advantages over widely adopted jet injectors, including: lower sample consumption, clog-free delivery, and the ability to control on-chip crystal density to improve hit rates. In this study we present our development of versatile, inexpensive, and robust polymer microfluidic chips for routine and reliable room temperature serial measurements at both synchrotrons and X-ray free electron lasers (XFELs). Our design includes highly X-ray-transparent enclosing thin film layers tuned to minimize scatter background, adaptable sample flow layers tuned to match crystal size, and a large sample area compatible with both raster scanning and rotation based serial data collection. The optically transparent chips can be used both for in situ protein crystallization (to eliminate crystal handling) or crystal slurry loading, with prepared samples stable for weeks in a humidified environment and for several hours in ambient conditions. Serial oscillation crystallography, using a multi-crystal rotational data collection approach, at a microfocus synchrotron beamline (SSRL, beamline 12-1) was used to benchmark the performance of the chips. Furthermore, high-resolution structures (1.3–2.7 Å) were collected from five different proteins – hen egg white lysozyme, thaumatin, bovine liver catalase, concanavalin-A (type VI), and SARS-CoV-2 nonstructural protein NSP5. Overall, our modular fabrication approach enables precise control over the cross-section of materials in the X-ray beam path and facilitates chip adaption to different sample and beamline requirements for user-friendly, straightforward diffraction measurements at room temperature.

59 BASIC BIOLOGICAL SCIENCES↗

Characterization of the Fusion Zone in Laser Beam Welds on SS304L

Designing a welded joint requires consideration of the welding process, component/assembly structure and weld geometry, material composition, properties, and desired joint performance. The designer must also specify a set of acceptance criteria used to evaluate the welds. This study was conducted to support the design team responsible for specifying the spot weld profile by investigating the relationship between weld process parameters and the weld geometry and properties to further inform design optimization. The subjects of this study are two thin stainless steel 304L (SS304L) components joined by Laser Beam Welding (LBW). The components are the Housing, which contains flexible circuitry, and the Cover that protects the circuitry during handling, installation, and under service loads. Figure 1 illustrates coupon versions of the Cover and Housing used to simulate the interface between these components for weld testing. These coupon representations of assembly components were designed to match the material and relevant geometry related to the welded joint while other features not relevant to the welded joint are excluded.The objective of this study was to characterize the sensitivity of the weld geometry and mechanical properties to the input weld parameters to inform further Finite Element Analysis (FEA) efforts in balancing joint strength against assembly deformation caused by the welding process. Characterization was accomplished by varying laser welding parameters around the current design values and measuring weld geometry on the cross-sections. Nanoindentation with a spherical and flat-ended tip was used on polished section cuts of the weld to obtain direct estimates of the stress-strain response of the Fusion Zone (FZ) for comparison to the Base Metal (BM).

42 ENGINEERING↗

Shear Behavior of Artificial Clay Seams within Bedded Salt Structures

Bedded salt contains thin layers of clay, also known as clay seams, in-between far thicker layers of salt. These inhomogeneities are thought to have first-order effects on the closure of nearby drifts and potential roof collapses. Despite their importance, characterizations of the peak shear strength and residual shear strength of clay seams in salt are extremely rare in the published literature. A previous paper reported results from laboratory direct shear experiments on clay seam samples from the Permian Basin in New Mexico. These clay seams behaved similar to intact salt, which was attributed to the abundance of salt crystals intersecting the clay seams. None of those specimens contained a distinct ¼" - ½" (6 -12 mm) thick clay seam, as has been observed in drifts at the Waste Isolation Pilot Plant (WIPP). Due to the difficulty in obtaining WIPP samples with these types of clay seams, artificial seams of bentonite and brine sandwiched between sections of salt were created and shear tested. Eight 4" diameter samples were created with either a ¼" or ½" a thick seam and then consolidated at 3000 psi prior to shear testing. The direct shear tests on these samples were performed at nominal normal stresses representative of expected WIPP in-situ conditions (500 to 1500 psi). The resulting shear stress vs. shear displacement curves exhibited a peak followed by a gradual decay of shear strength. The shear stress never transitioned to a true residual shear stress plateau, so the final shear strength at the end of each test (0.75" of shear displacement) was analyzed instead. Both the peak shear strength and the final shear strength conformed to Mohr- Coulomb behavior with friction angles and cohesion strengths consistent with a saturated, highly consolidated, clay. These new artificial clay seam results and the previous clay-interspersed-with-salt results likely bound the expected shear behavior of WIPP clay seams.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Morphological and molecular characterization of a Sarcocystis bovifelis-like sarcocyst in American beef

Abstract Background Parasites in the apicomplexan genusSarcocystisinfect cattle worldwide. Assessing the economic importance of each such parasite species requires proper diagnosis.Sarcocystiscruzi,a thin-walled species, infects virtually all cattle. The prevalence of the other thin-walled parasite,Sarcocystisheydorni, remains less well established. The remaining six species all have thick (> 3 µm) cyst walls (Sarcocystishirsuta,S.hominis,S.bovifelis,S.bovini,S.sigmoideus, andS.rommeli). Thick-walled sarcocysts often induce inflammation in striated muscles (causing bovine eosinophilic myositis), leading to condemnation of carcasses at slaughter. One of these,S.hirsuta, can be seen macroscopically and lead to condemnation of beef. TwoSarcocystisspecies,S.hominisandS.heydorni, are zoonotic. AlthoughS.hominishas been reported as prevalent in Europe, the occurrence of thick-walled species in the US remains poorly known. Here, for the first time to our knowldge, we characterize a thick-walledSarcocystisspecies from a sample of beef from a local grocery store in Maryland. By morphological and genetic criteria, it closely, but not perfectly, resembles parasites previously ascribed toS.bovifelis. Methods Beef samples were examined forSarcocystisinfection, using acid-pepsin digestion to search for bradyzoites, microscopically by compression between a glass slide and coverslip, by histology of paraffin embedded sections stained with hematoxylin and eosin, and by transmission electron microscopy (TEM). Molecular characterization was attempted employing genetic markers:18SrRNA,28SrRNA,cox1,ITS1,gapdh1,ron3, andrpoB. Results Molecular evaluation revealed 100% identity withS.bovifelis-like sarcocysts from naturally infected cattle from Germany and Argentina; although the condition of the frozen material precludes complete characterization by TEM, we noted morphological features which differed from theS.bovifelisoriginally described from experimentally infected cattle from Germany. Conclusions A novelSarcocystisspecies is described from beef from the USA but not named until further evaluation. Graphical Abstract

Parasitology↗

Mechanical Properties of Permanent Foaming Fixatives for Deactivation and Decommissioning Activities

DOE-EM have identified an operational requirement for a fixative that can immobilize and/or encapsulate residual contamination in 3D void volumes (pipes, gloveboxes, waste containers, etc.) during D and D activities. Failure to safely and effectively immobilize residual contamination can: Put workers at risk, Contaminate the public and environment, Drive up operational costs. Commercial-off-the-shelf (COTS) polyurethane (PU) foams is one possible solution and is currently being investigated in collaboration with Savannah River National Lab (SRNL). Mechanical property testing will dictate how well PU foams can withstand physical stressors outlined in safety documents while immobilizing residual contamination. Results can provide a performance criteria for Section 5 of ASTM E3191: Standard Specification for Permanent Foaming Fixatives Used to Mitigate Spread of Radioactive Contamination. Polyurethanes consists of repeating units of urethanes which are produced from an exothermic reaction between a polyol (an alcohol with two or more hydroxyl groups in a molecule) and an isocyanate [2]. PUs consists of 3D cells that are formed by a blowing agent which is normally water. Water interacting with the isocyanate creates carbon dioxide and urea which contributes to cells' growth and expansion. The cross-linking between the polyol and isocyanate solidify the cell faces and walls. Micro scale properties that can influence mechanical properties include: Relative density (ratio between density of cellular material and density of the solid of which the cell walls are made of). Cells connectivity between edges and faces, and number of cells contact neighbors [3]. Whether a foam is open-celled or closed-celled. Closed-celled foams have a thin membrane that encloses each cell which can contribute to the stiffness of the foam. Incorporating fillers in the PU matrix like carbon-based nanoparticles in the form of expandable graphite (EG) can increase the thermal and mechanical performance [4]. When exposed to heat, EG produces a char layer that prevents heat and oxygen transfer which is known as intumescing. Mechanical performance is dependent on amount of EG loading since the cell sizes are linearly dependent on it. Overall, the rigid foams (I-R2) proved superior. SEM Analysis: I-R2 had the most consistent spherical sizes (average cell diameter: 489 μm), which enhance the relative density the most [5]. Tensile Testing Results: I-R2 experienced the largest breaking load (103.65 lbf) and stress (289.42 psi). I-R2 also had a higher Young's Modulus compared to R1 (2.99 ksi to 2.09 ksi). Compression Testing Results: I-R2 had the highest stress at 80% deflection (360.67 psi), load (1387.48 lbf) and modulus (3.92 ksi)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Deuteration Effects on the Physical and Optoelectronic Properties of Donor–Acceptor Conjugated Polymers

The significant differences in scattering cross sections between deuterium and protium are unique to neutron scattering techniques and have been a long-standing area of interest within the neutron scattering community. Researchers have explored selective deuteration to manipulate scattering contrast in soft matter systems, leading to the widespread use of deuterium labeling in materials development. As deuteration changes the atomic mass, it alters physical properties such as molecular volume, polarizability, and polarity, which in turn may affect noncovalent interactions and crystal ordering. Despite previous studies, there remains a limited understanding of how deuteration impacts donor–acceptor (DA) conjugated polymers. To address this, we synthesized deuterated DPP polymers and systematically investigated the effects of side-chain deuteration on their thermal stability, crystal packing, morphology, and optoelectronic properties. We found that deuteration increased the melting and crystallization temperatures of DPP polymers, although it did not significantly alter their morphology, molecular packing, or charge mobility. These properties were assessed by using atomic force microscopy (AFM), X-ray scattering, and thin-film transistor device measurements, respectively, for DPP polymers. Our work shows that deuterium labeling could be a powerful method for controlling scattering length density, enabling neutrons to study the structure and dynamics of conjugated polymers without impacting their electronic performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Model Development for Multi-Component Fuel Vaporization and Flash Boiling

The objectives of this project are to improve the multi-component fuel droplet and film vaporization models used in internal combustion engine simulation, and to develop a comprehensive model to predict the characteristics of multi-component flash boiling spray. This work explores two approaches to fuel composition treatment for modeling multi-component fuel vaporization: one based on discretization and surrogates, and the other based on continuous thermodynamic distribution of fuel properties. The experimental data collected for model validation are done under three fuel form factors: droplet, spray, and thin film. The study on sprays also include experimentation under non-flash and flash boiling conditions, a phenomenon that enhances fuel vaporization. The main goals of this work are: Design and develop a multi-component fuel droplet and wall film vaporization model using both discrete and continuous thermodynamics methods. Design and develop an analytical model for multi-component flash boiling. Integrate the multi-component droplet and film model into multi-dimensional engine calculations to predict the fuel vaporization process under engine operation condition. Conduct multi-component droplet and fuel film vaporization experiments in a non-combusting chamber to verify the proposed vaporization models. Characterize flash boiling phenomena of multi-component fuel sprays by optical and laser diagnostic techniques. This report will detail the experimental setup and the numerical basis for developing a model to achieve the main goals listed above. Key features of observed multi-component fuel vaporization will be summarized at the end of each experimental sections, and corresponding model performance evaluation will be presented at the end of each model development section.

33 ADVANCED PROPULSION SYSTEMS↗

Preliminary Design of Critical Experiments Involving Commercially Available B 4 C Neutron Absorber Plates with Low-Enriched UO 2 Fuel

The International Criticality Safety Benchmark Evaluation Project (ICSBEP) is an initiative to provide high-quality benchmark data in a standardized format for criticality safety analysts to use to validate calculational tools and nuclear data. In the last released 2022 version, the ICSBEP handbook contains over 5,000 critical experiment descriptions, results, and associated models. This paper describes the critical configurations proposed and calculations performed as part of the conceptual design phase of Integral Experiment Request (IER) 554 (IER-554). The goal of IER-554 is to add to the benchmark experiments available to the criticality safety community by designing critical experiments that can analyze how adding commercially available Boralcan plates to an assembly of low-enriched UO2 fuel rods affects the effective neutron multiplication factor (k eff ). Boralcan, a neutron absorber product developed by Rio Tinto, is made of B4C in an Al 1100 matrix and is commonly used for criticality suppression in fuel storage pools. In the current version of the ICSBEP handbook, only a few dated critical experiments involve B4C materials, and none involve Boralcan in a thin plate shape. The experiments designed as part of IER-554 are intended to be performed at the Sandia Pulsed Reactor Facility/Critical Experiments (SPRF/CX) apparatus at Sandia National Laboratories. SPRF/CX is a well-characterized assembly considered trustworthy by the benchmarking community because of the numerous high-quality evaluations with very low experimental uncertainties included in the ICSBEP handbook. Figure 1 illustrates the assembly for a particular configuration from LCT-078, one of the published benchmarks in the ICSBEP handbook. The experiments will be moderated and reflected by light water at ambient atmospheric pressure. Before the plates are inserted in the critical assembly, they will be characterized with x-ray computed tomography (XCT) to identify the sizes and distribution of the B 4 C powder particles inside the plates. The preliminary design calculations were performed with SCALE 6.3.0 using the KENO V.a sequence for the criticality calculations, the CE-TSUNAMI-3D sequence for the sensitivity and uncertainty studies, and the ENDF/B-VII.1 Continuous Energy cross section library. All the calculation results presented have 10 pcm statistical uncertainties. A set of critical experiments with Boralcan plates could increase the confidence of the criticality safety community in its modeling methods when using this type of neutron absorber material. Experiments would also help validate k eff calculations, and the industry could use these validations to change the B loading credit limits from the US Nuclear Regulatory Commission standard review plan for dry cask storage of spent nuclear fuel. This paper summarizes only part of the analysis documented in the preliminary design report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

5.5 Hybrid Additively Manufactured Tooling for Large Composite Structures

This program sought to lower tooling costs for tightly toleranced, large composite aerostructures by using large format additive manufacturing (LFAM). LFAM tooling has the potential to lower tooling costs, but the large and unpredictable thermal expansion of polymer-based tooling did not previously allow for the production of large structures made with high performance resins requiring 350 deg F cures. Geometric tolerance issues and demolding concerns continued to arise. The proposed approach for this work was to print a thin shell via additive manufacturing that would be used as a scaffold for a conventional tooling prepreg. The prepreg would be laminated and cured onto both sides of the shell, creating a tool with a sandwich construction. The cured prepreg would then be machined and serve as the tooling surface. In addition to providing a clean, pit-free surface, the prepreg stiffness and low thermal expansion would physically restrain the AM shell and prevent it from expanding during thermal cycling, thus preventing any geometric mismatch between the nominal and actual part dimensions. A stair-step approach was taken to prove out this approach. Coupon level testing was done to ensure a good bond was possible between the AM shell and the tooling prepreg. These samples were also used to determine the amount of prepreg needed to achieve the desired coefficient of thermal expansion (CTE). The project team than progressed to a subscale tool measuring two feet in length. The geometry used was a C-section spar from Airbus’ Wing of Tomorrow program. A hybrid tool, using the AM shell and tooling prepreg, was made, and a composite part was fabricated with the tool. Dimensional scans of the tool and part indicated that the desired CTE was achieved with the tool. A second tooling approach was taken to reduce risk. In this approach, a subscale tool of the same geometry as previously mentioned was created, but the tool was entirely constructed of the tooling prepreg. AM was used to print a “master” that was then used to fabricate the tool by creating a splash off of the master using tooling prepreg. The innovation was that the master was not machined, but rather, was used right off the printer after a small amount of surface preparation. Removing this machining step was thought to make this approach economically viable when compared to conventional master fabrication. As before, the tool was used to fabricate a part and tested for dimensional accuracy. For the conclusion of the program, a ten-foot tool was created using the hybrid tool approach. The geometry also came from the Airbus C-section spar previously mentioned. Some difficulty arose in accurately predicting the geometry of the tool after laminating the tooling prepreg, resulting in multiple material additions and a tool geometry change. A part was fabricated in an autoclave using the tool. A cost savings of almost 50% was achieved on the subscale tool in both the hybrid and master-style tool, but the savings dropped considerably as the tool length increased in the full-scale tool. Given the less than expected cost savings and added complexity of the tool construction, it is suggested that the master-style tool is best for immediate commercialization for larger tools (although it may be appropriate for smaller, table-top size tools). Since its construction is very similar to conventionally made composite tooling, there already exists a broad supply chain for building the tool, and project partner Additive Engineering Solutions (AES) is well acquainted with the design and build of the AM master needed.

36 MATERIALS SCIENCE↗

Imaging a solvent-swollen polymer gel network by open liquid transmission electron microscopy

Visualizing the network of a solvent-swollen polymer gel remains problematic. To address this challenge, open transmission electron microscopy (TEM) was applied to thin gel films permeated by a nonvolatile ionic liquid. The targeted physical gels were prepared by cooling concentrated solutions of poly(ethylene glycol) in 1-ethyl-3-methyl imidazolium ethyl sulfate [EMIM][EtSO 4 ]. During the cooling, gelation occurred by a frustrated crystallization of the dissolved polymer, leading to a percolated, solvent-permeated semicrystalline network in which nanoscale polymer crystals acted as crosslinks. Crystalline features ranging from ~5 to ~200 nm were observed, with the visible network strands dominantly consisting of long curvilinear crystallites of ~15–20 nm diameter. Nascent spherulites irregularly decorated the network, creating a complex structural hierarchy that complicated analyses. Lacking diffraction contrast, TEM did not visualize the many disordered, fully solvated PEG chains present in the voids between crystals. Finally, recognizing that a network's three dimensionality is ambiguous when assessed through two-dimensional microscopy projections, a small gel region was studied by TEM tomography, revealing a nearly isotropic three-dimensional arrangement of the curvilinear crystallites, which displayed remarkably uniform cylindrical cross sections.

36 MATERIALS SCIENCE↗

Electromagnetic coil optimization for reduced Lorentz forces

Abstract The reduction of magnetic forces on electromagnetic coils is an important consideration in the design of high-field devices such as the stellarator or tokamak. Unfortunately, these forces may be too time-consuming to evaluate by conventional finite element modeling within an optimization loop. Although mutual forces can be computed rapidly by approximating large-bore coils as infinitely thin, this approximation does not hold for self-forces as it leads to an unphysical divergence. Recently, a novel reduced model for the self-field, self-force, and self-inductance of electromagnetic coils based on filamentary models was rigorously derived and demonstrated to be highly accurate and numerically efficient to evaluate (Hurwitz et al 2024 IEEE Trans. Magn. 60 7001614). In this paper, we present an implementation of the reduced self-force model employing automatic differentiation within the simsopt stellarator design software and use it in derivative-based coil optimization for a quasi-axisymmetric stellarator. We show that it is possible to significantly reduce point-wise forces throughout the coils, though this comes with trade-offs to fast particle losses and the minimum distance between coils and the plasma surface. The trade-off between magnetic forces and coil-surface distance is mediated by the minimum coil–coil distance for coils near the inboard side of the ‘bean’ cross-section of the plasma. The relationship between forces and fast particle losses is mediated by the normal field error. Coil forces can be lowered to a threshold with minimal deterioration to losses. Importantly, the magnet optimization approach here can be used also for tokamaks, other fusion concepts, and applications outside of fusion.

Hurwitz, Siena (ORCID:0000000166599659)↗

Compatibility of Steels in Supercritical CO2 at 450°-650°C

Supercritical CO2 (sCO2) power cycles, particularly direct-fired cycles, have the possibility of revolutionizing clean fossil energy. However, in the lower temperature sections of the cycle, lower cost steels are needed in order to lower the cost of the sCO2 technology. Representative 9 and 12%Cr steels and conventional and advanced austenitic steels are being evaluated at 450-650°C using mass change, bulk carbon (C) content and room temperature tensile properties to determine the maximum use temperatures for both direct- and indirect-fired sCO2 cycles. After 1000 h exposures in research grade (RG) sCO2 at 300 bar and RG sCO2 with 1% O2 and 0.1% H2O additions, the results suggest that increasing the Cr content from 9 to 12% yielded no signficant benefit under these conditions but the higher Cr and Ni contents in S31025 provided better compatibility in RG sCO2 at 650°C but limited benefit at 550°C with impurities. For S31609, the formation of Fe-rich oxide after exposure to RG sCO2 at 650°C resulted in both an increase in the bulk C content and a large drop in room temperature ductility. The evidence suggests thin, protective oxides prevented C ingress in these conditions.

Pint, Bruce↗

Deformation behavior of crystalline/amorphous Al-Si nanocomposites with nanolaminate or nanofibrous microstructures

Deformation mechanisms in sputter-deposited crystalline Al/amorphous Si nanocomposites with nanolaminate or nanofibrous morphology are characterized by nanoindentation, micropillar compression testing and transmission electron microscopy (TEM). The nanofibrous composite having crystalline Al nanofibers with ~40–50 nm in length and 15–20 nm in diameter embedded in amorphous Si exhibits strain hardening to a maximum flow stress of 2.9 GPa and no shear band (SB) formation in compression up to plastic strain exceeding 24%. On the other hand, nanolaminate composite that is composed of 80 nm crystalline Al layers and 20 nm amorphous Si layers exhibits catastrophic SBs starting at plastic strains in the range of 5–10%. Cross-sectional TEM of the deformed samples reveals a high density of stacking faults and twin boundaries in Al nanofibers and no microshear bands in the nanofibrous composite, suggesting plastic deformation in amorphous Si phase and crystalline Al nanofibers. Further, molecular dynamics simulations revealed that the plastic deformation in amorphous Si phase in the cosputtered films could be favored by the decrease in flow strength of amorphous Si with increasing Al solute concentration trapped in Si.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

(Oxy)hydroxides Formed on Aluminum Fuel Materials After Irradiation and Long-Term Wet Storage - 20354

The aluminum cladding of research-reactor fuel experiences general corrosion when in contact with water during in-reactor service and post-discharge wet storage, resulting in the formation of adherent aluminum (oxy)hydroxide films. These (oxy)hydroxides contain chemically-bound water that poses challenges for extended dry storage due to the risk of thermal or radiolytic decomposition releasing free water and/or hydrogen and oxygen gases. This study describes characterization of the (oxy)hydroxides present on several aluminum materials used in reactor operation and subsequently stored wet in the L-Basin storage facility at the Savannah River Site (SRS) for an extended period. Characterization data providing insight into the loading, composition, and morphology of (oxy)hydroxides to be expected on service-exposed aluminum cladding provides valuable benchmarks for designing adequate drying and dry-storage approaches. This work is part of a broader investigation to address knowledge gaps and technical data needs for dry storage of aluminum-clad spent nuclear fuel (ASNF), which included in-lab growth of (oxy)hydroxide films on aluminum alloy substrates to investigate formation behavior, investigation of drying methods to remove existing (oxy)hydroxides from ASNF cladding, and measurement of radiolytic yield of hydrogen from (oxy)hydroxide powders and films. In this study, (oxy)hydroxide films were characterized for three aluminum-alloy materials used in reactors and subsequently stored wet for up to approximately 40 years in L-Basin at SRS: one cropping from a Missouri University Research Reactor (MURR) fuel element (Al-6061 alloy), one cropping from a Universal Sleeve Housing (USH) (Al-6063 alloy), and one Mark-16B fuel assembly (either Al-6061 or Al- 6063). The USH and Mark-16B were used in SRS production reactors. Characterization of the as-received (oxy)hydroxides included scanning electron microscopy (SEM) in both plan-view and cross-section to characterize the (oxy)hydroxide layer's morphology, thickness, and structure. X-ray diffraction (XRD) was used to identify the chemical composition and distinguish between the various aluminum (oxy)hydroxides known to form under reactor and storage conditions. XRD analysis revealed both bayerite (Al(OH)3) and boehmite (AlOOH) on the surface of the MURR and USH samples, as well as bayerite, boehmite, and gibbsite (another Al(OH)3 polymorph) on the surface of the Mark-16B sample. The aluminum trihydroxides, bayerite and gibbsite, are typically associated with corrosion in low-temperature (<80 deg. C) water, while boehmite is expected to form at higher water temperature (>80 deg. C). The presence of bayerite on the USH, which is believed to have operated close to 90 deg. C, suggests that boehmite formed during in-reactor exposure was not protective against further hydroxide growth in low-temperature wet storage. Cross-section scanning electron microscopy (SEM) showed total (oxy)hydroxide layer thicknesses of ∼5- 10 μm for the MURR and ∼5-15 μm for the Mark-16B. The thickness of the USH's (oxy)hydroxide layer was indiscernible by the current mounting and imaging method, despite plan-view SEM and XRD confirming the presence of an (oxy)hydroxide layer. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Nonlinear Shear Rheology of Entangled Polymer Rings

Steady-state shear viscosity η($\bar{γ}$) of unconcatenated ring polymer melts as a function of the shear rate $\bar{γ}$ is studied by a combination of experiments, simulations, and theory. Experiments using polystyrenes with Z ≈ 5 and Z ≈ 11 entanglements indicate weaker shear thinning for rings compared to linear polymers exhibiting power law scaling of shear viscosity η ~ $\bar{γ}$ –0.56 ± 0.02 , independent of chain length, for Weissenberg numbers up to about 10 2 . Nonequilibrium molecular dynamics simulations using the bead-spring model reveal a similar behavior with η ~ $\bar{γ}$ -0.57 ± 0.08 for 4 ≤ Z ≤ 57. Viscosity decreases with chain length for high $\bar{γ}$. In our experiments, we see the onset of this regime, and in simulations, which we extended to Wi ~ 10 4 , the nonuniversality is fully developed. In addition to a naive scaling theory yielding for the universal regime η ~ $\bar{γ}$ –0.57 , we developed a novel shear slit model explaining many details of observed conformations and dynamics as well as the chain length-dependent behavior of viscosity at large $\bar{γ}$. The signature feature of the model is the presence of two distinct length scales: the size of tension blobs and much larger thickness of a shear slit in which rings are self-consistently confined in the velocity gradient direction and which is dictated by the size of a chain section with relaxation time 1/$\bar{γ}$. These two length scales control the two normal stress differences. In this model, the chain length-dependent onset of nonuniversal behavior is set by tension blobs becoming as small as about one Kuhn segment. This model explains the approximate applicability of the Cox–Merz rule for ring polymers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗