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At least 325 records · Page 18

Room temperature plasma-etching and surface passivation of far-ultraviolet Al mirrors using electron beam generated plasmas

The development of optical systems operating in the far ultraviolet range (FUV, λ=100-200 nm) is limited by the efficiency of passivated aluminum (Al) mirrors. Although it is presently possible to obtain high-reflectivity FUV mirrors through physical vapor deposition, the process involves deposition with substrates at high temperatures, which is technically challenging for large optical elements. A novel passivation procedure for bare Al mirrors is reported. The treatment consisted of using a low-temperature electron-beam generated plasma produced in a gas mixture of Ar and SF6 to etch away the native oxide layer from the Al film, while simultaneously promoting the generation of a thin aluminum tri-fluoride (AlF3) layer on the Al surface. In the first section we analyze the effect of varying both ion energy and SF6 concentration on the FUV reflectance, thickness, composition, and surface morphology of the resulting AlF3 protective layers. In the second section, the reflectivity of samples is optimized at selected important FUV wavelengths for astronomical observations. Notably, samples attained state-of-the-art reflectances of 75% at 108.5 nm (He Lyman γ), 91% at 121.6 nm (H Lyman α), 90% at 130.4 nm (OI), and of 95% at 155.0 nm (C IV). The stability over time of these passivated mirrors is also investigated.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effect of surface oxides on tritium entrance and permeation in FeCrAl alloys for nuclear fuel cladding: a review

Abstract Iron-chromium-aluminum (FeCrAl) alloys are being considered for the cladding of uranium dioxide fuel in light water reactors (LWRs). FeCrAl alloys have good mechanical properties at temperatures of 300 °C and higher, and have superlative resistance to attack by steam at temperatures of up to 1000 °C and higher. A concern has been raised that the use of FeCrAl for cladding would result in a higher content of tritium in the reactor coolant as compared with the current system where the cladding is a zirconium based alloy. This review shows that the flux of tritium from the fuel rod cavities to the coolant across the fuel cladding wall will be greatly reduced by the presence of oxides on the surface of the cladding. The review of current literature and permeation data show that (a) protective oxides are expected to be present on both sides of the FeCrAl cladding, and (b) depending on the characteristics of these oxide layers it is reasonable to expect about two–three orders of magnitude reduction in tritium permeation, relative to the permeation response in clean, unoxidized condition for FeCrAl steels of interest, around 277 °C–377 °C temperatures.

Electrochemistry↗

A Synchrotron-Based Vacuum Ultraviolet Photoionization Mass Spectrometer-Coupled Microreactor To Probe Thermocatalysis

Vacuum ultraviolet photoionization (VUV-PI) mass spectrometry offers an isomer-selective and universal ionization with minimal fragmentation detection of organics in complex chemical systems such as pyrolysis and combustion. Here, in this study, we report a state-of-the-art experimental setup of a universal catalytic microreactor combined with a molecular beam to investigate the thermocatalytic oxidation of a heterogeneous system relevant for probing reactions at gas–solid interfaces. In strong contrast to traditional off-line analytical methods, this technique is capable of identifying and quantifying short-lived species (radicals) as well as stable products to decipher initial reaction steps via the detection of nascent products. The thermocatalytic oxidative degradation of exo-tetrahydrodicyclopentadiene (JP-10), a high energy-density hydrocarbon fuel, over solid titanium–aluminum–boron reactive mixed metal nanopowder (Ti-Al-B RMNP) is exploited to showcase potential applications. Overall, some 59 nascent gas-phase products are identified via photoionization efficiency (PIE) curves, including oxygenated species and hydrocarbons comprising closed-shell molecules and radicals. The critical temperature for complete oxidative decomposition of JP-10 was lowered by 450 K from 1400 K to 950 K, indicating an efficient thermocatalytic action of Ti-Al-B nanoparticles on JP-10. The enabling of a universal chemical microreactor along with VUV-PI mass spectrometry broadens the applicability of this technique to hydrocarbon fuel oxidation and pyrolysis characterization. This isomer-selective sensitive probing along with the detection of radical transients makes the aforementioned technique superior to other conventional analytical techniques such as microflow tube and pyrolysis-gas chromatography coupled with mass spectrometry for investigating similar pyrolysis reactions and comprehensive quantification.

Paul, Dababrata [Univ. of Hawaii at Manoa, Honolul↗

Czochralski Growth and Characterization of a Compositionally Complex Rare Earth Aluminum Garnet Scintillator: (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce

Compositionally complex oxides have garnered increasing interest for their enhanced phase stability and tunable functional properties, yet their development as bulk single crystal scintillators remains limited. Herein, we report the Czochralski growth and characterization of (Gd 1/4 Y 1/4 Tb 1/4 Lu 1/4 ) 3 Al 5 O 12 :Ce (GYTLAG), a compositionally complex garnet incorporating four dodecahedrally coordinated principal rare earth elements. The garnet phase was confirmed by powder and single crystal X-ray diffraction, and macroscopic defects are described. X-ray absorption near-edge structure measurements confirm the 3+ oxidation state of all rare earths and support their occupation of the same crystallographic site; white line intensity variations correlate with the anticipated segregation behavior. Elemental segregation is quantified by SEM/EDS and ICP-OES, and a linear trend was established between the segregation coefficient and the difference between each rare earth’s ionic radius (r) and the average ionic radius (AIR) of the dodecahedral site. This trend offers a predictive framework for compositional control in future REAG crystals grown by the Czochralski method. Photoluminescence and radioluminescence measurements reveal both Ce 3+ and Tb 3+ emission. Scintillation pulses exhibit four-component decay with dominant ~230 µs and ~1.2 ms components, and the light yield is estimated to be up to 43,000 ph/MeV under 137Cs γ-ray excitation. GYTLAG also demonstrates a strong radioluminescence efficiency and 50% lower afterglow at 20 ms compared to a LuAG:Ce reference, underscoring its promise for scintillator applications.

Compositionally complex oxide, high entropy oxide,↗

Synergy of Graphene Nanoribbons and Graphene Sheets for High-Rate Lithium-Sulfur Batteries

According to the increasing demands for shortening the battery charging time, high current rate (C-rate) performances become more significant in practical applications. With a higher theoretical capacity, lithium-sulfur batteries are treated as promising candidates for the next-generation batteries. In this work, the utilization of graphene nanoribbons (GNRs) exhibits the benefits in conductivity and other electrochemical performances, especially for high-rate applications. With air-controlled electrospray as the method, carbon encapsulated sulfur particles, poly(acrylic acid), reduced graphene oxide (rGO) sheets, and GNRs are mixed and directly deposited onto the carbon coated aluminum collector, to employ as the cathode. The scanning electron microscopy (SEM) imaging exhibits that the two-dimensional structure of GNRs helps construct inter-connected networks. This improved structure of cathode can increase the electroconductivity, confirmed by the electrochemical impedance spectroscopy (EIS), and modify the porosity, indicated through pore size distribution profiles. In this way, the polysulfides can be more efficiently trapped and utilized, realizing the promising behavior with faster charge transfer. In terms of the cycling performance at 0.2 C, the batteries with GNRs can perform 18% higher in capacity than those without GNRs, without decreasing the charge retention. According to the rate-capability tests, systems with GNRs can achieve enhanced performance compared to batteries with precursor carbon nanotubes (CNTs), especially at high C-rates. At 2 C, with 80 wt % of graphene-based materials as GNRs, batteries can achieve an increase in capacity by 78% and 41% compared with systems without GNRs and those with CNTs, respectively. Accordingly, the results testify the synergy of GNRs and rGO sheets in Li-S batteries.

25 ENERGY STORAGE↗

Impact of target-derived and ambient oxygen on gas-phase oxidation in laser ablation plumes

Gas-phase oxidation in a laser-produced plasma is significantly influenced by the availability of oxygen in and around the plume. In this study, we investigate the role of target-derived and ambient oxygen on AlO formation in plasmas generated from aluminum (Al) and Al 2 O 3 targets in air and argon, respectively. Our results highlight that gas-phase oxidation occurs early during the evolution of Al 2 O 3 plasmas in argon, in contrast to Al plasmas in air, where the initial exclusion of oxygen from the plume delays the chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermal Model of Oxide Growth for Full Size Fuel Plate Experiments in the Advanced Test Reactor

The full-size plate number one (FSP-1) irradiation test designed for irradiation testing of plate type fuel is planned to be irradiated in the Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL). This FSP-1 experiment is a non-instrumented drop-in test where aluminum-clad fuel plates are cooled directly by the ATR Primary Coolant System (PCS) water. This experiment is one of a series of experiments being irradiated at ATR for the United States High Performance Research Reactor (USHPRR) program. This fueled experiment contains aluminum-clad fuel full-size plates consisting of monolithic U-10Mo. Previous thermal analyses have been documented concerning oxide growth [1] and thermal safety margins [2] for similar U-10Mo mini plate experiments. This analysis is part of the thermal safety analysis of the experiment to be irradiated in ATR. Departure from nucleate boiling ratio (DNBR) and flow instability ratio (FIR) have been calculated for the flow coastdown condition 2 and the reactivity insertion accident condition-2 (RIA2) transient. The purpose of this paper is to investigate the thermal margin of the fuel meat during a RIA2 transient when oxide has accumulated on the plate surfaces acting as an insulator.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A perspective on the electro-thermal co-design of ultra-wide bandgap lateral devices

Fundamental research and development of ultra-wide bandgap (UWBG) semiconductor devices are under way to realize next-generation power conversion and wireless communication systems. Devices based on aluminum gallium nitride (AlxGa1-xN, x is the Al composition), ..beta..-phase gallium oxide (..beta..-Ga2O3), and diamond give promise to the development of power switching devices and radio frequency power amplifiers with higher performance and efficiency than commercial wide bandgap semiconductor devices based on gallium nitride (GaN) and silicon carbide (SiC). However, one of the most critical challenges for the successful deployment of UWBG device technologies is to overcome adverse thermal effects that impact the device performance and reliability. Overheating of UWBG devices originates from the projected high power density operation and poor intrinsic thermal properties of AlxGa1-xN and ..beta..-Ga2O3. This Perspective delineates the need and process for the "electro-thermal co-design" of laterally configured UWBG electronic devices and provides a comprehensive review of current state-of-the-art thermal characterization methods, device thermal modeling practices, and both device- and package-level thermal management solutions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Material exploration towards high quality factor microwave resonators

Niobium and aluminum have been widely used to realize superconducting resonators and qubits. However, the native oxide at the metal air interface limits the devices results. This layer is highly disordered, and it induces losses limiting the performances of the resonators or qubits. Recently, tantalum led to great improvement in qubit relaxation time. This improvement has been attributed to a thinner and less disordered oxide layer compared to Nb and Al. This study is aimed to limit the formation of the oxide layer, by the introduction of novel superconducting materials such as rhenium or by encapsulating the Nb surface with other superconducting materials such as Ta, Al, Re or other non-superconducting materials such as Au. To better understand the results, we are realizing these studies on coplanar waveguide resonators where the relation between surface losses and quality factor is clear. We are also analyzing different fabrication techniques to completely characterize our devices, linking material properties to the performances. In this work we are also varying the participation ratio of the devices in order to extract with higher fidelity and precision the losses introduced by the involved interfaces.

Crisa, F.↗

Thermite and intermetallic projectiles examined experimentally in air and inert gas environments

Intermetallic (aluminum and zirconium) and thermite (aluminum and molybdenum trioxide) projectiles were launched using a high velocity impact ignition testing system. The experiments were designed to simulate reactivity in high (argon) and low (air) altitude environments. The projectiles were launched into a chamber that included a steel target plate for projectile penetration before impacting a rear witness plate. The chamber was semi-sealed and instrumented for quasi-static pressure data. The results provide an understanding of energy release from the projectile materials and of the environmental influence on performance. The transient pressure traces provide insight into reaction kinetics. A bifurcation in transient pressure rise was an indication of a shift in reaction kinetics from the inherent reactive material to metal oxidation with the environment. The bifurcation was delayed by about 0.15 ms for the intermetallic relative to the thermite, evidence that the thermite reaction proceeded faster upon impact than the intermetallic. The two-step process (impact ignition of the reactive material followed by metal oxidation) was shown to produce higher energy conversion efficiencies than projectiles composed of pure fuel (i.e., aluminum) reported previously. Both reactive materials showed energy conversion efficiencies greater than 30% (for air) and 50% (for argon), and an explanation of underestimated efficiency and energy losses is provided. These results have implications for advancing formulations for ballistic applications. Structural reactive materials can be used to modify the effective reactivity of metal-containing formulations in varied atmospheric environments.

36 MATERIALS SCIENCE↗

Enhanced Laser Damage Threshold in Optically Addressable Light Valves via Aluminum Nitride Photoconductors

Abstract Optically addressable light valves (OALVs) are specialized optical components utilized for spatial beam shaping in various laser‐based applications, including optics damage mitigation, and enhanced functionality in diode‐based additive manufacturing requiring high intensities. Current state‐of‐the‐art OALVs employ photoconductors such as Bismuth Silicon Oxide (BSO) or Bismuth Germanium Oxide (BGO), which suffer from limited laser‐induced damage thresholds (LiDT) and inadequate thermal conductivities, thus restricting their use in high peak and average power applications. Aluminum nitride (AlN), an emerging ultra‐wide band gap (UWBG) III–V semiconductor, offers promising optoelectronic properties and superior thermal conductivity (>300 Wm −1 K −1 at 298° K, compared to BSO's 3.29 Wm −1 K −1 ). In this study, the first AlN‐based OALVs are designed, fabricated, and experimentally demonstrated using commercially available single‐crystal AlN substrates. These AlN‐based OALVs have shown clear superiority over BSO and BGO‐based devices. Design considerations for OALVs incorporating UWBG photoconductors are discussed, and the photoresponsivity from defect‐mediated sub‐bandgap absorption in AlN crystals is verified as sufficient for OALVs operating under high light fluences. The optimum driving voltage for the AlN‐based OALV is determined to be ≈ 45 V pp at 100 Hz, achieving a transmittance of 91.3%, an extinction ratio (ER) of more than 100, and a 51:1 image contrast.

36 MATERIALS SCIENCE↗

Evaluation of Copper Catalytic Effects in Cable Insulation Polymers

This paper summarizes work performed to evaluate a phenomenon that occurs in electrical cable insulation polymers subjected to accelerated aging while in contact with copper metal. This effect, commonly known as the copper catalytic effect, is a result of chemical reactions that occur when copper ions diffuse into insulation polymers. This diffusion process is observed in various types of polymeric materials exposed to elevated temperatures and happens at the interface between the insulation and metallic components (e.g., conductor, shielding, etc.) in a cable. This polymer-metal interaction has only been observed in cables constructed with copper components (i.e., no interactions observed in cables with aluminum or other metal conductor/shielding) and results in a significant catalytic effect that increases the oxidation rate (e.g., aging) of the material. Under this research, the copper catalytic effects observed in cross-linked polyethylene, cross-linked polyolefin and ethylene propylene rubber insulated cables subjected to thermal accelerated aging were evaluated. These evaluations involved applying infrared spectroscopy, microscopy, and energy dispersive X-ray spectroscopy cross-sectional depth profiling to obtain an in-depth understanding of the aging characteristics of the materials under accelerated conditions. Based on the results of these assessments, the copper catalytic effect can have a significant impact on the mechanical, thermal, chemical, and electrical properties of cable insulation polymers. Here, the results acquired from this research provided the information needed to characterize the copper catalytic effects observed in these polymers, analyze how this phenomenon affected the polymer degradation process, and compare and understand the differences in the properties of the materials.

42 ENGINEERING↗

Fabrication and Characterization of Plutonium Targets for Irradiation in the Flattop Critical Assembly

In FY16, Pu targets were fabricated in support of the Nuclear Physics: Cumulative Fission Product Yields (Fission R-values) task of the F2016 venture project; these targets are suitable for irradiation in the Flattop critical assembly at the Nevada National Security Site (NNSS). This report documents an overview of the target design, preparation of the Pu metal materials by removing the oxide layer and appropriate sizing for the target holders, target fabrication including filling an inner aluminum cup with the Pu material and the sealing of an outer stainless steel capsule, target assay using gamma spectroscopy, and the He leak testing of the final targets. Four targets were fabricated with two containing 99% 239 Pu metal and two containing 93% 239 Pu metal. Additional samples of each material were set aside for mass spectrometric analysis at PNNL and Los Alamos National Laboratory.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Cycling protocol for alkaline batteries

A method of operating a battery comprises discharging a cathode comprising manganese dioxide to within a 2nd electron capacity of the manganese dioxide at a C-rate of equal to or slower than C/10, recharging the battery, and cycling the battery during use a plurality of times. The cathode is in a battery, and the battery comprises the cathode, an anode, a separator disposed between the anode and the cathode, and an electrolyte. The cathode comprises the manganese dioxide and a conductive carbon. The anode comprises: a metal component and a conductive carbon. The metal component can be a metal, metal oxide, or metal hydroxide, and the metal of the metal component can be zinc, lithium, aluminum, magnesium, iron, cadmium and a combination thereof.

Kolhekar, Snehal↗

A Nuclear Magnetic Resonance Study of Cation and Anion Dynamics in Polymer–Ceramic Composite Solid Electrolytes

Polymer–ceramic composite electrolytes are promising for the application of all-solid-state lithium-ion batteries with high energy density and improved safety. In this work, we employ temperature-dependent 7 Li and 19 F NMR to examine the chemical environment and the dynamics of Li + cation and triflate anion in poly(ethylene oxide) (PEO)–lithium triflate (LiTf) polymer electrolyte and a composite electrolyte containing 55 vol % doped lithium aluminum titanium phosphate (LICGC). The line shape analysis and spin–lattice relaxation (T 1 ) measurements suggest both the Li + cations and the Tf – anions reside in two distinct environment: a mobile environment and an immobile environment. In the semicrystalline state, a large ratio (>70%) of immobile Li + and Tf – is observed. In the melt state, the ratio of mobile cations and anions significantly increases. With the presence of LICGC ceramic, an increased ratio of immobile Li + and Tf – and reduced mobility of the mobile components are observed, indicating that the ceramic negatively impacts the transport of both the cations and the anions. NMR characterizations are corroborated by conductivity results, which reveal that the intrinsic ionic conductivity of the polymer phase of the composite electrolyte was only 0.15 of the ceramic-free polymer electrolyte at room temperature. These results shed light on the challenges inherent to composite electrolytes with the goal of achieving both enhanced Li + transference number and ionic conductivity.

25 ENERGY STORAGE↗

Thermal Optimization of a Silicon Carbide, Half-Bridge Power Module

This project describes the modeling process to design the packaging and heat exchanger for a half-bridge wide-bandgap (WBG) power semiconductor module. The module uses two silicon carbide, metal-oxide-semiconductor field-effect transistor (MOSFET) devices per switch position that are soldered to an aluminum nitride, direct-bond copper (DBC) substrate. A baseplate cooling configuration (e.g., no thermal grease) is used along with a water-ethylene glycol, jet-impingement-style heat exchanger. The heat exchanger was designed to be fabricated using prototyping equipment from the National Renewable Energy Laboratory, complies with automotive standards (for minimal channel sizes, flow rates, and coolant), and considers reliability aspects (i.e., erosion/corrosion). Device-scale computational fluid dynamics (CFD) is used first to design the slot jet impingement cooling configuration and compute the effective heat transfer coefficient (HTC) of the concept. The computed HTCs are then used as boundary conditions for a finite element study to optimize the package geometry (e.g., device layout and baseplate thickness) to minimize thermal resistance and minimize temperature variation between the module's four devices. Finally, a fluid manifold is designed to generate the slot jets and cool the devices. Module-scale CFD predicts a relatively low junction-to-fluid thermal resistance of 16.7 mm2 K/W, a 1.4 degrees C temperature variation between devices, and a total pressure drop of 5,860 Pa (0.85 psi) for the design. The thermal resistance of the module design is about 67% lower than the 2015 BMW i3 power electronics/modules thermal resistance.

DIRECT ENERGY CONVERSION↗

In-situ anodic precipitation process for highly efficient separation of aluminum alloys

Electrorefining process has been widely used to separate and purify metals, but it is limited by deposition potential of the metal itself. Here we report in-situ anodic precipitation (IAP), a modified electrorefining process, to purify aluminium from contaminants that are more reactive. During IAP, the target metals that are more cathodic than aluminium are oxidized at the anode and forced to precipitate out in a low oxidation state. This strategy is fundamentally based on different solubilities of target metal chlorides in the NaAlCl4 molten salt rather than deposition potential of metals. The results suggest that IAP is able to efficiently and simply separate components of aluminum alloys with fast kinetics and high recovery yields, and it is also a valuable synthetic approach for metal chlorides in low oxidation states.

36 MATERIALS SCIENCE↗

Impacts of aluminum-cerium alloy deployment on different cerium commodities

An imbalance problem exists in the rare earth element (REE) market with cerium and lanthanum being more abundant and less valuable than REEs used in permanent magnets such as neodymium, praseodymium, and dysprosium. Research has been conducted on new applications for abundant REEs to improve mining economics. However, potential market impacts of these applications on individual REE commodities are unknown. A system dynamics model was built to investigate the impacts of a new aluminum-cerium (Al-Ce) alloy that can theoretically utilize three separate cerium forms: cerium carbonate, cerium oxide, or cerium metal. Cerium carbonate currently possesses the lowest price of the three available forms making it initially the most favorable choice. However, model results showed that cerium oxide could provide the best economics for future Al-Ce alloy deployment because its larger market size buffers major shocks to price.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗