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177 records · Page 10

Modeling and Design of Micro Flux Monitors for Neutron Fluence Measurements

Measuring neutron flux is critical to understanding the characteristics of nuclear reactors and can provide information on the energy spectrum, total neutron fluence, and operational history of a facility. Such measurements are typically performed by irradiating high-purity materials in an operating reactor for a known length of time. By measuring and identifying activation products in the irradiated materials and referencing the energy-dependent cross section of each isotope, the neutron energy spectrum and total fluence can be determined. Historical techniques use a variety of small, individually pressed foils or wires for dosimeter devices, which can result in excessively high levels of radioactivity and complications in handling after irradiation. The present work describes a new neutron dosimetry concept, named the micro flux monitor, that uses semiconductor device fabrication processes to deposit thin films of flux monitoring materials in precise geometries onto a SiC wafer. This approach allows multiple dosimetry materials to be located on a single device, simplifying irradiation and subsequent analysis. The geometry, and therefore mass, of each material can be custom-tailored for a specific application—considering the expected neutron flux, duration of irradiation, and device retrieval time of a facility. Additionally, hundreds of identical dosimetry monitors can be produced simultaneously, reducing fabrication costs. Finally, the extremely thin metal dimensions of these devices could improve the fidelity of neutron fluence measurements by reducing neutron self-shielding and gamma self-attenuation effects.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

59 Co(p,X) spallation reaction cross sections for 250 MeV to 2 GeV protons

Cobalt is an advantageous target for probing the physics of nuclear spallation, because it is a naturally mono-isotopic element ( 59 Co), and its per-nucleon binding energy (BE/A = 8.768 MeV) is near the maximum value for all nuclei. We measured nuclear spallation cross sections for the 59 Co(p,X) reaction at five kinetic energies ranging from 250 MeV to 2 GeV. Cross sections for the production of 58 Co, 57 Co, 57 Mn, 56 Co, 56 Mn, 56 Cr, 55 Fe, 53 Fe, 54 Mn, 52 Mn, 51 Cr, 49 Cr, 48 V, 47 Sc, 46 Sc, 44 Sc, and 44 Scm are reported. Where comparable data exist in the EXFOR reaction database, we find that our measured cross sections generally agree. In many cases, we provide data for reactions or energies not currently reported in EXFOR. Our cross sections also provide evidence for the presence of α-clusters within the 59 Co nucleus, a surprising result given the asymmetry in Z (27) and N (32) for this nucleus. Finally, we use our measurements to evaluate the accuracy of spallation cross section simulations from GEANT4-based radiation transport toolkit, performed with the INCLXX-, Bertini-, and Binary-ion-cascade (BIC) based physics lists. This benchmarking activity revealed that the simulations overestimated the cross sections by a factor of ∼2–4 on average, and that the INCL-XX physics list provides the most reliable results. This evaluation informs the selection of the GEANT4 physics lists used for the analysis of data from NASA’s Psyche mission, which will measure γ rays and neutrons resulting from spallation reactions occurring on the surface of an asteroid whose surface is thought to be rich in iron-nickel metal.

43 PARTICLE ACCELERATORS↗

Specifications of EBR-II Neutron Radiography Method Description and Digitization Approach

All neutron radiography (NRAD) images of fuel pins in Argonne’s collection were originally generated using the NRAD imaging facility established in the Hot Fuel Examination Facility (HFEF) at Idaho National Laboratory (INL). The NRAD reactor facility was built in 1977 and has been operating since. The reactor is a TRIGA-type reactor operating at a power level of 250 kWth to provide a neutron source for radiography imaging. The reactor is equipped with two beam tubes (i.e., east beam tube and north beam tube) to guide the neutron beams to two radiography stations. The east radiography station is directly under the HFEF main cell and is dedicated for specimens already in the HFEF hot cell. The north radiography station is outside of the main HFEF hot cell and allows NRAD imaging of non-irradiated items. The NRAD images of EBR-II irradiated metallic fuel pins were taken in the east radiography station. Thermal neutrons have the capability to transmit through most materials and are ideal for NRAD imaging. However, because of their high thermal neutron absorption cross-section, fissile materials (e.g., highly-enriched nuclear fuels) may not be as transmissible to thermal neutrons. This is also the case for oversize specimens with extraneous thickness. Epithermal neutron imaging is therefore used as a complement to thermal neutron NRAD imaging. At HFEF’s NRAD facility, both thermal and epithermal neutrons can be used for NRAD imaging. Irradiated nuclear fuels emit high levels of γ radiation that can easily darken X-ray films, so direct exposure NRAD cannot be used to image them. Instead, an indirect NRAD imaging method was developed at HFEF’s NRAD facility. In this method, foils made of materials that can be activated by neutrons (i.e., with large neutron absorption cross section) are used to collect transmitted neutron signals. Then the activated foils are then placed against X-ray films and enclosed in a vacuum cassette so that the γ decay from the activated foils can produce images on the X-ray films. Then, general X-ray film processing procedures are used to digitize and store the images. By using different foil materials, different energy neutrons can be used for NRAD imaging. At the HFEF NRAD station, two types of films are commonly used: dysprosium (Dy) foils with thickness of 130 microns are used to capture thermal neutron signal, while indium (In) foils with thickness of 130 microns are used to capture epithermal neutron signal. A cadmium or gadolinium foil is put before the indium foil to work as a thermal neutron filter. The thermal and epithermal NRAD images can be taken simultaneously by using a Dy/Cd/In sandwiched foil combination. The typical NRAD exposure time is approximately 20 minutes. Then the exposed foils are transferred to film vacuum cassettes. The vacuum ensures that there is no gap between the foil and the film. The foil-to-film exposure time is at least three half-lives of the corresponding radioisotopes, which are 3 hours for In and 7.5 hours for Dy, respectively. Exposed films are processed using an automatic film processor to produce completed NRAD images.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Evaluation of lithium as a tritium storage medium for betavoltaics

Lithium foils were demonstrated to absorb surrogate protium for tritium-powered betavoltaics. 20μm thick lithium foils were hole-punched from a ribbon of electrodeposited lithium on copper foil. The lithium foils were loaded with hydrogen in a custom Sievert apparatus where the pressure drop showed full hydriding at a hydrogen pressure of 2 bar and at all loading temperatures above the lithium melting point at 190, 200, 225, 250, and 300. Lithium hydride formation was confirmed with Raman spectroscopy after hydrogen loading. The kinetics of experimental hydride formation was compared to the diffusion-limited Mintz–Bloch model. While the Mintz–Bloch model showed good fit with the experimental loadings, the model overpredicted the loading kinetics starting at 250 °C and at higher temperatures. In conclusion, The overprediction was either caused by lithium hydride outgassing due to some reduction with some residual lithium hydroxide created from brief air exposure when sealing the lithium in the reactor or a transition from diffusion-limited hydride growth to surface or metal–hydride interface-limited hydride growth.

25 ENERGY STORAGE↗

Lithium-Sulfur Batteries with a Block Copolymer Electrolyte Analyzed by X-ray Microtomography

Most of the work on Lithium-sulfur (LiS) batteries use liquid electrolytes that have limited stability when coupled with Li metal anodes. We have studied LiS batteries with a solid block copolymer electrolyte which exhibits improved stability against Li anodes. Additionally, the electrolyte comprises a polystyrene-b-poly(ethylene oxide) (SEO) copolymer doped with a Li salt. Hollow carbon nanospheres impregnated with sulfur were used to build a composite cathode. Two types of sulfur-impregnated functionalized carbon nanospheres were used: One with carboxylic acid groups and the other with short lithium poly(4-styrenesulfonyl(trifluoromethylsulfonyl)imide) (PSTFSI-Li) chains. Cells with Li S dissolved in the SEO based electrolyte served as the baseline. After cycling, the reason for capacity fade was determined by imaging the batteries using synchrotron hard X-ray microtomography. It is generally assumed that LiS cells fail due to dissolution of polysulfide into the liquid electrolyte, i.e., the main problems related to the cathode. In our all-solid cells, failure was primarily due to delamination of the Li foil from the polymer electrolyte layer. Delamination is also observed at the sulfur cathode. It is likely that the large changes in volume of the active materials during cycling induce delamination in all-solid LiS cells. 2 8

25 ENERGY STORAGE↗

Architecting a Stable High-Energy Aqueous Al-Ion Battery

Aqueous Al-ion batteries (AAIBs) are the subject of great interest due to the inherent safety and high theoretical capacity of aluminum. The high abundancy and easy accessibility of aluminum raw materials further make AAIBs appealing for grid-scale energy storage. However, the passivating oxide film formation and hydrogen side reactions at the aluminum anode as well as limited availability of the cathode lead to low discharge voltage and poor cycling stability. Here, we proposed a new AAIB system consisting of an Al x MnO 2 cathode, a zinc substrate-supported Zn-Al alloy anode, and an Al(OTF) 3 aqueous electrolyte. Through the in situ electrochemical activation of MnO, the cathode was synthesized to incorporate a two-electron reaction, thus enabling its high theoretical capacity. The anode was realized by a simple deposition process of Al 3+ onto Zn foil substrate. The featured alloy interface layer can effectively alleviate the passivation and suppress the dendrite growth, ensuring ultralong-term stable aluminum stripping/plating. The architected cell delivers a record-high discharge voltage plateau near 1.6 V and specific capacity of 460 mAh g -1 for over 80 cycles. Finally, this work provides new opportunities for the development of high-performance and low-cost AAIBs for practical applications.

25 ENERGY STORAGE↗

Electron Kinetics Induced by Ultrafast Photoexcitation of Warm Dense Matter in a 30-nm-Thick Foil

We report on the study of electron kinetics induced by intense femtosecond (fs) laser excitation of electrons in the 5d band of Au. Changes in the electron system are observed from the temporal evolution of ac conductivity and conduction electron density. The results reveal an increase of electron thermalization time with excitation energy density, contrary to the Fermi-liquid behavior of the decrease of thermalization time associated with the heating of conduction electrons. This is attributed to the severe mitigation of photoexcitation by Auger decay. The study also uncovers the shortening of 5d hole lifetime with the increase of photoexcitation rates. Overall, these unique findings provide valuable insights for understanding electron kinetics under extreme nonequilibrium conditions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Influence of helium bubbles on the bulk equation of state of gold under static compression

Nuclear materials often evolve into two-phase systems comprising a bulk matrix with dispersed inert-gas bubbles. The presence of these bubbles can have consequences to the thermomechanical response of materials and is a key life-limiting factor in some nuclear fuel forms. Understanding the behavior of these two-phase, bubble-matrix systems is, thus, important to improved predictive models and frameworks for many nuclear materials applications. While temperature excursions of these two-phase systems have been characterized, fewer studies have focused on the evolution of inert-gas bubbles under pressure. Here, in this paper, we use x-ray tools to interrogate a He-implanted gold foil to determine the pressure-dependent evolution of the individual components (Au matrix + bubbles), and we compare that total pressure dependence to theoretical equation-of-state descriptions based on mixing rules.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Tensile properties of co-rolled Zr/U-10Mo fuel at ambient and elevated temperatures

The United States High Performance Research Reactor (USHPRR) initiative is currently interested in replacing high-enriched uranium fuel in research reactors with high-assay low-enriched uranium fuel. Here, this work aimed to assist in that mission by providing tensile and bend test data on bare U-Mo and tensile test data on co-rolled Zr/U-10Mo plates at differing thicknesses (0.285 mm, 0.300 mm, and 0.465 mm) and temperatures (293 K, 473 K, and 623 K). Yield strength and ultimate tensile strength values are reported along with an in-depth comparison of how temperature, rolling direction, thickness, and the presence of the Zr-interlayer affect mechanical properties. Results showed that yield strength and ultimate tensile strength in Zr/U-10Mo foils lower as temperature increases by approximately 300 MPa from 293 to 473 K, and another 100 MPa from 473 to 623 K. Additionally it was found that with increased temperature, there is less differentiation in fuel necking and delamination behavior, as well as a greater perceived elongation to fracture. The elastic modulus of co-rolled mini-plates does not follow the volumetric rule of mixtures in terms of averaged strength and is actually lower than the reported moduli of both Zr and U-10Mo.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Observation and Characterization of Vibrationally Active Surface Species Accessed with Nonthermal Nitrogen Plasmas

Polycrystalline Ni, Pd, Cu, Ag, and Au foils exposed to nonthermal plasma (NTP)-activated N 2 are found to exhibit a vibrational feature near 2200 cm –1 in polarization-modulation infrared reflection-absorption spectroscopy (PM-IRAS) observations that are not present in the same materials exposed to N 2 under nonplasma conditions. The feature is similar to that reported elsewhere and is typically assigned to chemisorbed N 2 . We employ a combination of temperature-dependent experiments, sequential dosing, X-ray photoelectron spectroscopy, isotopic labeling, and density functional theory calculations to characterize the feature. Results are most consistent with a triatomic species, likely NCO, with the C and O likely originating from ppm-level impurities in the ultrahigh-purity (UHP) Ar and/or N 2 gas cylinders. Here, this work highlights the potential for nonthermal plasmas to access adsorbates inaccessible thermally as well as the potential contributions of ppm-level impurities to corrupt the interpretation of plasma catalytic chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Experimental observation and integrated modelling of proton-beryllium fusion in He and D plasmas at JET

Validated integrated modelling of JET ITER-like wall experiments in which fusion performance is driven by reactions between fast ions and intrinsically present metal wall impurities is presented. A steady-state L-mode plasma with dominant proton-beryllium fusion and neutron yields of up to ≈ 6·10 13 s -1 is developed in He and D, via radiofrequency heating of a H minority. The fusion drive is unambiguously confirmed by the neutral particle analyser, fast ion loss detector, and γ-ray diagnostics. Experiments are analysed via an integrated modelling framework, developed to model the two-stage proton beryllium-fusion chain and produce high-fidelity fusion product source terms. The modelling chain comprises TRANSP and JETTO for plasma core modelling, LOCUST for full orbit product tracking and collisional slowing-down, DRESS to resolve two- and three-body fusion kinematics, and MCNP for neutron transport calculations. Modelling shows that the primary 9 Be(p,n) 9 B reaction is the dominant neutron emitter at naturally present concentrations of beryllium in these experiments. The yield contribution of secondary reactions between fusion products and beryllium, 9 Be(d,n) 10 B and 9 Be(α,n) 12 C, is found to be negligible. The proton-deuteron knock-on effect in D plasmas is modelled, which is calculated to contribute ≈ 25% to the total neutron yield. For both He and D discharges the total computed neutron rates match fission chamber (FC) measurements within the combined experimental and computational uncertainty, with an average discrepancy of ≈ ± 20%. Realistic proton-beryllium neutron sources are propagated through JET’s MCNP neutron transport model which shows that 235 U FCs’ response is sensitive to p–Be source changes, with up to ≈ 10% variation compared to a D–D neutron source. We show that the high-energy tail of the fast proton minority can be studied with multi-foil neutron activation. The framework is also applied to the study of interactions between fast protons and boron impurities, of relevance to ITER. We calculate that in JET conditions a significant alpha source with DT-like energies could be generated through 11 B(p, α)2α fusion, and detected via γ-emission in secondary interactions between fast alphas and boron. The work represents an important step towards validating predictive integrated modelling capabilities for non-standard fusion reactions.

JET↗

Progress Report on Performance of A709 and G91 Steels in Sodium

Specimens in six different processing and heat treatment conditions of A709 H58776 were exposed to sodium at 550, 600, and 650°C, respectively for various exposure times. G91 base metal was tested in sodium at 550, 600, and 650°C, and G91 weldment at 550 and 600°C, respectively. Parallel thermal aging experiments were conducted on G91 and A709 to obtain thermal aging data for comparison with sodium exposure results to separate the thermal and sodium effects. The corrosion data obtained on A709 steel continue to show low corrosion rates, which indicate good compatibility of A709 with sodium when oxygen content is controlled. G91 has also shown acceptable corrosion rates over the temperature range of 550-650°C in sodium. Thermal aging or sodium exposures reduced the tensile strength, uniform elongation, and total elongation for A709 ESR, AOD specimens. These specimens consistently showed higher yield stress and tensile strength and lower uniform and total elongations after sodium exposure than after thermal aging under comparable testing conditions. It implies that there was an additional effect of sodium exposure that gave rise to an increase in tensile strength of A709. Dynamic strain aginginduced flow serrations were completely removed by either thermal aging or sodium exposure at 650°C, which imply that carbon or nitrogen in solution was removed from the solution and formed precipitates during aging or sodium exposures. The tensile data ruled out the possibility of decarburization under the sodium exposure conditions. The HOMO specimens behaved somewhat differently from the ESR and AOD specimens in sodium. While thermal aging and sodium exposures at 550 and 600°C decreased the yield stress and the ultimate tensile strength of G91, there was virtually no additional effect resulting from sodium exposures at these two temperatures. In contrast, sodium exposures at 650°C had a drastic effect on the yield stress and the ultimate tensile strength of G91. It is suggested that G91 experienced decarburization in the 650°C sodium environments. Carbon concentrations in sodium in the SMT-1 and SMT-2 loops were determined by a foil equilibration method. The estimated carbon concentration was in the range of 0.8-1.2 ppm in the SMT-1 loop and 0.3-0.7 ppm in the SMT-2 loop. The carbon activity in sodium in the SMT-2 loop was estimated to be 0.03-0.08 at 600°C, and 0.08-0.2 at 550°C. The carbon activity in sodium at 650°C in the SMT-1 loop was 0.04-0.07. Equilibrium simulation of the carburization – decarburization processes was conducted for A709 and G91 steels exposed in sodium environments at temperatures of 550-700°C. The carbon activity-concentration relationship for G91 was re-evaluated by considering four phases in G91, i.e. bcc ferrite, M 23 C 6 , NbC and VC carbides. It was found that the carburization-decarburization process in G91 steel was dictated by M 23 C 6 carbides at high carbon activities, while NbC carbides dominated the process at low carbon activities. Formation of NbC increases the decarburization resistance of G91 steel. It remains to be understood whether the decarburization resistance provided by MC carbides in G91 can be maintained during long-term operations of SFRs. The carbon concentration-activity relationship for A709 was calculated based on the equilibrium of fcc-austenite and M 23 C 6 carbide phase. The calculations showed that A709 decarburizes at 650°C in the SMT-1 loop environments, which is different from the experimental findings. The carbon concentration-activity relationship in A709 was further evaluated by considering four phases, including fcc-austenite, M 23 C 6 , NbC, and TiC carbide phases. TiC is the most stable carbides among the three carbide phases. The carburization-decarburization process in A709 is dictated by M 23 C 6 carbides at high carbon activities and by TiC at low carbon activities. Formation of TiC increases the decarburization resistance of A709 steel. Because of the complexity of the precipitation process in A709 during sodium exposures, detailed characterization of precipitates in sodium-exposed specimens and improved thermodynamic models are needed to understand the carburization-decarburization behavior of A709. Kinetic analysis of carbon transfer will be investigated for G91 and A709 in future work.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Measurement bias in self-heating x-ray free electron laser experiments from diffraction studies of phase transformation in titanium

X-ray self-heating is a common by-product of X-ray Free Electron Laser (XFEL) techniques that can affect targets, optics, and other irradiated materials. Diagnosis of heating and induced changes in samples may be performed using the x-ray beam itself as a probe. However, the relationship between conditions created by and inferred from x-ray irradiation is unclear and may be highly dependent on the material system under consideration. Here, we report on a simple case study of a titanium foil irradiated, heated, and probed by a MHz XFEL pulse train at 18.1 keV delivered by the European XFEL using measured x-ray diffraction to determine temperature and finite element analysis to interpret the experimental data. We find a complex relationship between apparent temperatures and sample temperature distributions that must be accounted for to adequately interpret the data, including beam averaging effects, multivalued temperatures due to sample phase transitions, and jumps and gaps in the observable temperature near phase transformations. The results have implications for studies employing x-ray probing of systems with large temperature gradients, particularly where these gradients are produced by the beam itself. Finally, this study shows the potential complexity of studying nonlinear sample behavior, such as phase transformations, where biasing effects of temperature gradients can become paramount, precluding clear observation of true transformation conditions.

Crystallography↗

Shock compression of silver to 300 GPa: Wave profile measurements and melting transition

Recent in-situ x-ray diffraction (XRD) measurements on laser-shock compressed Ag foils demonstrated a face-centered-cubic to body-centered-cubic transformation at ~150 GPa and melting between 172 and 197 GPa [Phys. Rev. Lett. 124, 235701 (2020)]. As a complement to the XRD work, we conducted plate impact experiments to obtain shock velocity and wave profile measurements on thicker Ag samples shock-compressed to peak stresses between 30 and 300 GPa. The shock velocity–particle velocity results were fitted very well by a linear relation over the entire stress range, providing an accurate determination of the Ag Hugoniot (locus of the stress-volume states achieved under shock compression). For peak stresses below 187 GPa and above 210 GPa—corresponding to the solid and liquid phases, respectively—the wave profiles show clean single waves. No wave profile features related to the fcc-bcc transformation at ~150 GPa were observed, implying minimal volume change for the transformation. For stresses between 187 and 210 GPa, an initial jump was followed by a time-dependent increase in the particle velocity (20–80 ns risetime) to the peak state—corresponding to the solid-liquid mixed phase response. Unlike the solid and liquid response, the mixed-phase response cannot be readily analyzed analytically. Instead, numerical simulations incorporating an accurate multiphase equation of state for Ag—not currently available—are required to analyze the wave profiles measured at 187–210 GPa stresses. Furthermore, the present work shows the potential for using wave profile measurements to examine the melting transition under shock compression.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗