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At least 307 records · Page 17

Space Test of Bare-Wire Anode Tethers

An international team, lead by Tokyo Metropolitan University, is developing a mission concept for a suborbital test of orbital-motion-limited (OML) bare-wire anode current collection for application to electrodynamic tether propulsion. The tether is a tape with a 50-mm width, 0.05-mm thickness, and 1-km length. This will be the first space test of the OML theory. In addition, by being an engineering demonstration (of space tethers), the mission will demonstrate electric beam generation for "sounding" determination of the neutral density profile in the ionospheric "E-layer." If selected by the Institute of Space and Astronautical Science/Japanese Aerospace Exploration Agency (JAXA), the mission will launch in early 2009 using an $520 Sounding Rocket. During ascent, and above =100 km in attitude, the 1-km tape tether will be deployed at a rate of 8 m/s. Once deployed, the tape tether will serve as an anode, collecting ionospheric electrons. The electrons will be expelled into space by a hollow cathode device, thereby completing the circuit and allowing current to flow.This paper will describe the objectives of the proposed mission, the technologies to be employed, and the application of the results to future space missions using electrodynamic tethers for propulsion or power generation.

Johnson, L.↗

Design Considerations for Practical Li-S Batteries for Electric Aviation

The development of high-energy, high-safety, and high-power batteries beyond electric automotive standards is critical for future electric aviation applications. Non-volatile solid-state electrolytes (SSE) offer many promising advantages over traditional flammable liquid electrolytes. Solid-state electrolytes may be an enabling technology for certain battery chemistries by preventing detrimental interactions with liquid electrolytes, for example prevention of the dissolution of intermediates in lithium-sulfur common in traditional liquid organic solvents. However, significant manufacturing challenges must be overcome before the adoption of such technology. This research was conducted to identify processing techniques for producing solid-state battery components with practical dimensions and weights for enabling high specific energy cells. Traditional research has identified a range of very high theoretical ionic conductivities but are impractical due to their instability or inability to be manufactured. Electrolytes explored in this study were produced as sulfide-polymer composites with densified thicknesses below 40 micron using a tape-casting technique and thermoplastic elastomer binder. The combination of high chemical compatibility and flexibility produced robust films that had moderate impact on the ionic conductivity but was capable of dramatically reducing the parasitic mass. Despite minimal conductivity losses, films were produced 10-15 times thinner than comparable bulk powder electrolytes thus leading to overall lower film resistance. Conductivity is maintained above 0.2mS/cm for composite electrolytes. Through the analysis of materials based on their physical properties, such as density, practical cells can be designed. Based on this, low density sulfide-solid-state electrolytes are a promising candidate for achieving the energy and safety metrics for electric aviation, however, further optimization of cathode microstructure and composite processing will be required to achieve the high power metrics and will be the focus of further studies. Additionally, fabrication challenges arise when utilizing metallic lithium foil, due to its soft nature, as overflow and mechanical short circuit can occur on assembly which remains a challenge to overcome before metallic lithium anodes can be fully realized.

batteries↗

Ultrasmooth Epitaxial Pt Thin Films Grown by Pulsed Laser Deposition

Platinum (Pt) thin films are useful in applications requiring high-conductivity electrodes with excellent thermal and chemical stability. Ultrasmooth and epitaxial Pt thin films with single-crystalline domains have the added benefit of providing ideal templates for the subsequent growth of heteroepitaxial structures. Here, we grow epitaxial Pt (111) electrodes (ca. 30 nm thick) on sapphire (α-Al 2 O 3 (0001)) substrates with pulsed laser deposition. This versatile technique allows control of the growth process and fabrication of films with carefully tailored parameters. X-ray scattering, atomic-force microscopy, and electron microscopy provide structural characterization of the films. Various gaseous atmospheres and temperatures were explored to achieve epitaxial growth of films with low roughness. A two-step (500 °C/300 °C) growth process was developed, yielding films with improved epitaxy without compromising roughness. The resulting films possess ultrasmooth interfaces (<3 Å) and high electrical conductivity (6.9 × 10 6 S/m). Finally, Pt films were used as current collectors and templates to grow lithium manganese oxide (LiMn 2 O 4 (111)) epitaxial thin films, a cathode material used in Li-ion batteries. In conclusion, using a solid-state ionogel electrolyte, the films were highly stable when electrochemically cycled in the 3.5-4.3 V vs Li/Li + range.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solvent-Free Manufacturing of Lithium-Ion Battery Electrodes via Cold Plasma

Slurry casting has been used to fabricate lithium-ion battery electrodes for decades, which involves toxic and expensive organic solvents followed by high-cost vacuum drying and electrode calendering. This work presents a new manufacturing method using a nonthermal plasma to create inter-particle binding without using any polymeric binding materials, enabling solvent-free manufacturing electrodes with any electrochemistry of choice. The cold-plasma-coating technique enables fabricating electrodes with thickness (>200 μm), high mass loading (>30 mg cm -2 ), high peel strength, and the ability to print lithium-ion batteries in an arbitrary geometry. This crosscutting, chemistry agnostic, platform technology would increase energy density, eliminate the use of solvents, vacuum drying, and calendering processes during production, and reduce manufacturing cost for current and future cell designs. Here, lithium iron phosphate and lithium cobalt oxide were used as examples to demonstrate the efficacy of the cold-plasma-coating technique. It is found that the mechanical peel strength of cold-plasma-coating-manufactured lithium iron phosphate is over an order of magnitude higher than that of slurry-casted lithium iron phosphate electrodes. Full cells assembled with a graphite anode and the cold-plasma-coating-lithium iron phosphate cathode offer highly reversible cycling performance with a capacity retention of 81.6% over 500 cycles. For the highly conductive cathode material lithium cobalt oxide, an areal capacity of 4.2 mAh cm -2 at 0.2 C is attained. We anticipate that this new, highly scalable manufacturing technique will redefine global lithium-ion battery manufacturing providing significantly reduced plant footprints and material costs.

25 ENERGY STORAGE↗

Modification of LiMn 2 O 4 surfaces by controlling the Acid–Base surface chemistry of atomic layer deposition

In this combined theoretical and experimental study, we report the effects of Al precursor selection on the growth chemistry, interfacial structure, and electrochemistry of Al 2 O 3 coatings on spinel LiMn 2 O 4 (LMO) surfaces by atomic layer deposition (ALD). Five Al precursors, exhibiting a range of Lewis acid-base properties, were used to establish trends in the ALD Al 2 O 3 growth chemistry on LMO powders in comparison to redox-inactive planar silicon substrates. We show that the Lewis acid-base properties of the Al precursor ligands can be used to tune both the Mn oxidation states and the Al 2 O 3 coverage on the LMO surface. Density functional theory calculations are used to examine the reaction mechanism of each precursor on LMO surfaces, elucidating a correlation between the Lewis acidity of the ligands and the decomposition thermochemistry. In-depth X-ray photoelectron spectroscopy and in situ Fourier transform infrared spectroscopy measurements support these theoretical predictions and further reveal how different Al precursors modify the atomic and electronic structure near the LMO surface during ALD. While the Mn oxidation state is strongly influenced by the Lewis acidity of the precursor ligand, the surface coverage and thickness of the Al 2 O 3 coating are a more representative descriptor of the electrochemical performance measured in coin cell experiments. Finally, we show how the ligand acid-base properties of ALD precursors can be used to rationally tailor atomic layer growth mechanisms, which may enable atomic level control over the structure of functionalized interfaces for various applications related to catalysis, semiconductors, and energy storage.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Transforming nanoscale VO 2 (B) into a scalable sodium-ion electrode

The intermittent nature of renewable energies requires highly reliable grid-level energy storage approaches. A critical consideration in developing this technology is the areal capacity which determines battery performance and influences the cost of battery technology. Of related importance is finding new ways of developing scalable electrodes. In recent years, three-dimensional (3D) printing of conductive scaffolds has emerged as an alternative to overcome the scalability limitations of commercial tape cast electrodes. The research carried out in the current study demonstrates a successful scalability pathway for nanoscale VO 2 (B), a desirable cathode for sodium-ion batteries which has a nano-flower morphology with a crystallite size < 20 nm. By electrodepositing VO 2 (B) onto a graphene aerogel scaffold, we were able to achieve mass loading of over 100 mg·cm −2 and still possess an areal capacity of 10 mAh·cm −2 at a current density of 5 mA·cm −2 . Moreover, after 1000 cycles, these electrodes retained 75% to 80% of their initial capacity. Even at high loading levels, the electrodeposited VO 2 (B) exhibits pseudocapacitive material signatures such as a box-like voltammetry response, linear galvanostatic response, and no phase change upon lithiation. The scalability of the VO 2 (B) electrode is demonstrated in a series of experiments which show the areal capacity to scale upon increase in both mass loading and electrode thickness, with only small changes in specific capacity. Furthermore, this study establishes that nanoscale materials can be scaled up to achieve thick electrodes without compromising their electrochemical properties.

additive manufacturing↗

A new cyclic carbonate enables high power/ low temperature lithium-ion batteries

The modern lithium-ion battery (LIB) configuration was enabled by the "magic chemistry" between ethylene carbonate (EC) and graphitic carbon anode. Despite the constant changes of cathode chemistries with improved energy densities, EC-graphite combination remained static during the last three decades. While the interphase generated by EC protects the fragile graphitic structure, the intrinsic disadvantages of EC (high viscosity, high melting point, excessive interphase growth) lead to mediocre power density and poor performances of LIB at sub-zero temperatures, where lithium depositions form upon charging. Such performance compromises arise from the fundamental dilemma between requiring effective interphase protection and high impedance from excessive growth of interphase. In this work, we designed and synthesized a "double EC" molecule as electrolyte additive to resolve the above dilemma. Erythritol bis(carbonate) (EBC) possesses lower LUMO energy level than EC and hence tends to decompose prior to EC reduction, but its weak solvation toward Li + restricts the extent of its reduction, thus minimizing the interphase thickness and the corresponding impedances. Electrolytes containing EBC enables both the charging and discharging of ampere-size LIB pouch cells at sub-zero temperatures from 0 to -20°C, demonstrating that the key approach to improve low temperature performances lies in how to tailor interphasial chemistry rather than the bulk electrolyte composition.

25 ENERGY STORAGE↗

Imaging Phase Segregation in Nanoscale Li x CoO 2 Single Particles

Li x CoO 2 (LCO) is a common battery cathode material that has recently emerged as a promising material for other applications including electrocatalysis and as electrochemical random access memory (ECRAM). During charge– discharge cycling LCO exhibits phase transformations that are significantly complicated by electron correlation. While the bulk phase diagram for an ensemble of battery particles has been studied extensively, it remains unclear how these phases scale to nanometer dimensions and the effects of strain and diffusional anisotropy at the single-particle scale. Understanding these effects is critical to modeling battery performance and for predicting the scalability and performance of electrocatalysts and ECRAM. Here we investigate isolated, epitaxial LiCoO 2 islands grown by pulsed laser deposition. After electrochemical cycling of the islands, conductive atomic force microscopy (c-AFM) is used to image the spatial distribution of conductive and insulating phases. Above 20 nm island thicknesses, we observe a kinetically arrested state in which the phase boundary is perpendicular to the Li-planes; we propose a model and present image analysis results that show smaller LCO islands have a higher conductive fraction than larger area islands, and the overall conductive fraction is consistent with the lithiation state. Thinner islands (14 nm), with a larger surface to volume ratio, are found to exhibit a striping pattern, which suggests surface energy can dominate below a critical dimension. When increasing force is applied through the AFM tip to strain the LCO islands, significant shifts in current flow are observed, and underlying mechanisms for this behavior are discussed. The c-AFM images are compared with photoemission electron microscopy images, which are used to acquire statistics across hundreds of particles. Finally, the results indicate that strain and morphology become more critical to electrochemical performance as particles approach nanometer dimensions.

25 ENERGY STORAGE↗

SPUTTERED THIN FILMS FOR VERY HIGH POWER, EFFICIENT, AND LOW-COST COMMERCIAL SOFCS

The aim of this project was to leverage the low area specific resistance (ASR) of Redox’s GDC electrolyte-based cell architecture and increase solid oxide fuel cell (SOFC) efficiency (i.e., open circuit voltage, or OCV) without significantly increasing cell resistance. The key to achieving the increased SOFC efficiency is the introduction of a thin sputtered yttria stabilized zirconia (YSZ) electron-blocking layer and a thin sputtered gadolinia doped ceria (GDC) barrier layer on top of the half-cell substrate (i.e., anode and GDC electrolyte). A key initial effort of the project was to improve the quality of the half-cell substrate surface so that any remaining defects were significantly smaller than the desired film thickness. During lab-scale trials, we had to overcome challenges with film cracking during post-sputtering treatments (e.g., thermal anneals) as well as damage to the sputtering targets. After the initial lab-scale trials, the focus shifted toward the use of commercial scale sputtering equipment with a sputtering equipment manufacturer in the microelectronics industry. Using the commercial sputtering equipment, we deposited films with different variations of power, PO2, sputtering time, platen speed, etc. We then determined the combinations of sputtering conditions and post-sputtering treatments that yielded high-quality films without cracks or other significant defects. While thin films were deposited on cells as large as 10 cm by 10 cm, the processing was optimized using 4 cm by 4 cm cells. Cell performance was evaluated in stainless-steel test fixtures between 500 °C and 700 °C with hydrogen fuel fed to the anode and air fed to the cathode. Extensive studies allowed us to determine that modified cathode and cathode contact firing processes were required to achieve theoretical OCV. Moreover, use of the new firing processes resulted in the need for a modified cathode contact to achieve a low ASR. In summary, the project demonstrated the performance of high OCV (1.13 V at 650 °C) from sputtered layers and a low ASR (~0.25 Ohms-cm2 at 650 °C) resulting from a modification of cathode/contact processing and the introduction of alternative contact layers that are sufficient to yield a Gen-1 cell with a maximum power density of approximately 1.2 W/cm2. At an operating voltage of 0.74 V, this would yield a cell power density of ~1.1 W/cm2. While not utilized in this project, a Redox Gen-2 cell has a catalyst-infiltrated porous anode that reduces the ASR by more than 50% from that of the Gen-1 cells used in this project. Therefore, if the sputtered YSZ electron-blocking layer and GDC barrier layer are added to a Gen-2 half cell with a similar increase in OCV to the theoretical value of ~1.13 V at 650 °C, and if the same improvement in ASR (from that demonstrated in this project) is achieved when using the Gen-2 half-cell architecture as a sputtered cell substrate, then the power density at 0.74 Vop could be as high as ~2.6 W/cm2. The impact of such power density gains, while still maintaining high cell efficiency, and thus high system efficiency, is a dramatic decrease in system cost because the stack represents ~30-40% of the SOFC system cost.

01 COAL, LIGNITE, AND PEAT↗

Ultra‐Thin Single‐Particle‐Layer Sodium Beta‐Alumina‐Based Composite Polymer Electrolyte Membrane for Sodium‐Metal Batteries

Inorganic/organic composite polymer electrolytes (CPEs) with good flexibility and electrode contact have been pursued for solid-state sodium-metal batteries. However, the application of CPEs for high energy density solid-state sodium-metal batteries is still limited by the low Na + conductivity, large thickness, and low ion transference number. Herein, an ultra-thin single-particle-layer (UTSPL) composite polymer electrolyte membrane with a thickness of ≈20 µm straddled by a sodium beta-alumina ceramic electrolyte (SBACE) is presented. A ceramic Na + -ion electrolyte that bridges or percolates across an ultra-thin and flexible polymer membrane provides: 1) the strength and flexibility from the polymer membrane, 2) excellent electrolyte/electrode interfacial contact, and 3) a percolation path for Na + -ion transfer. Owing to this novel design, the obtained UTSPL-35SBACE membrane exhibits a high Na+-ion conductivity of 0.19 mS cm -1 and a transference number of 0.91 at room temperature, contributing to long-term cycling stability of symmetric sodium cells with a small overpotential. The assembled quasi-solid-state cell with the as-prepared UTSPL-35SBACE membrane displays superior cycling performance with a discharge capacity of 105 mAh g -1 at 0.5 °C rate after 100 cycles and excellent rate performance (82 mAh g -1 at 5 °C rate) at room temperature with the potassium manganese hexacyanoferrate (KMHCF)@CNTs/CNFs cathode, where KMHCF refers to potassium manganese hexacyanoferrate.

25 ENERGY STORAGE↗

Revealing the role of redox reaction selectivity and mass transfer in current–voltage predictions for ensembles of photocatalysts

Photocatalysts are conceptually simple reaction units where nanoscale semiconductors integrated with catalysts drive a pair of redox reactions on illumination. However, the proximity of reaction sites performing cathodic and anodic reactions poses dire challenges to realize large light-to-fuel conversion efficiencies. In this study, a powerful, yet straightforward, equivalent-circuit detail-balance modeling framework is developed and applied to evaluate the performance of photocatalytic systems featuring multiple light absorbers. Specifically, low bandgap iridium-doped strontium titanate is modeled as a Z-scheme photocatalyst to achieve desirable hydrogen evolution and iron-based redox shuttle oxidation reactions. Our model has unique capabilities to simulate competing redox reactions and address mass-transfer limitations. In a significant departure from state-of-the-art circuit models, our study develops tools to perform load-line analyses by incorporating a net electrochemical load curve that includes both desired and competing redox reactions. Consequently, reaction selectivity is predicted from equivalent circuit models for photocatalytic and photoelectrochemical systems. Our investigation into ensembles comprised of multiple, semi-transparent light absorbers reveals their potential to outperform a single, optically thick light absorber, particularly when operated under mass-transfer-limited conditions. However, this outcome hinges on minimizing mass-transfer rates of select redox species to prevent undesired reactions of hydrogen oxidation and/or redox shuttle reduction. Our findings demonstrate that reaction selectivity can be achieved by tuning asymmetry in redox species mass-transfer even with perfectly symmetric electrocatalytic charge-transfer coefficients. The influences of various kinetic, mass-transfer, and thermodynamic parameters are explored to offer crucial insights for synthesis of the next-generation of photocatalysts and selective coatings, and reactor designs.

25 ENERGY STORAGE↗

Moisture-Induced Alumina Scale Spallation: The Hydrogen Factor

For some time our community has been concerned with interfacial spallation of protective alumina scales, not just upon immediate cooldown, but as a time-delayed phenomenon. Moisture-induced delayed spallation (MIDS) and desktop spallation (DTS) of TBC's refer to this process. It is most apparent for relatively adherent alumina scales that have survived cool down in a dry environment, built up considerable thickness and strain energy, and have been somewhat damaged, such as by cyclic oxidation cracking. Indeed, a "sweet zone" can be defined that maximizes the observed effect as a function of all the relevant factors. Moisture has been postulated to serve as a source of interfacial hydrogen embrittlement derived from reaction with aluminum in the alloy at an exposed interface. The purpose of this monograph is to trace the close analogy of this phenomenon to other hydrogen effects, such as embrittlement of aluminides and blistering of alloys and anodic alumina films. A formalized, top-down, logic tree structure is presented as a guide to this discussion. A theoretical basis for interfacial weakening by hydrogen is first cited, as are demonstrations of hydrogen as a reaction product or detected interfacial species. Further support is provided by critical experiments that produce the same moisture effect, but by isolating hydrogen from other potential causative factors. These experiments include tests in H2-containing atmospheres or cathodic hydrogen charging.

Smialek, James L.↗

Moisture-Induced Alumina Scale Spallation: The Hydrogen Factor

For some time the oxidation community has been concerned with interfacial spallation of protective alumina scales, not just upon immediate cool down, but as a time-delayed phenomenon. Moisture-induced delayed spallation (MIDS) and desktop spallation (DTS) of thermal barrier coatings (TBCs) refer to this process. It is most apparent for relatively adherent alumina scales that have survived initial cool down in a dry environment, have built up considerable thickness and strain energy, and have been somewhat damaged, such as by cyclic oxidation cracking. Indeed, a "sensitive zone" can be described that maximizes the observed effect as a function of all the relevant factors. Moisture has been postulated to serve as a source of interfacial hydrogen embrittlement. Hydrogen is derived from reaction with aluminum in the alloy at an exposed interface. The purpose of this monograph is to trace the close analogy of this phenomenon to other hydrogen-induced effects, such as embrittlement of aluminides and blistering of alloys and anodic alumina films. A formalized, top-down, logic-tree structure is presented as a guide to this discussion. A theoretical basis for interfacial weakening by hydrogen is first cited, as are demonstrations of hydrogen detection as a reaction product or interfacial species. Further support is provided by critical experiments that recreate the moisture effect, but by isolating hydrogen from other potential causative factors. These experiments include tests in H 2-containing atmospheres or cathodic hydrogen charging. Accordingly, they strongly indicate that interfacial hydrogen, derived from moisture, is the key chemical species accounting for delayed alumina scale spallation.

Smialek, James L.↗

A Guideline to Mitigate Interfacial Degradation Processes in Solid‐State Batteries Caused by Cross Diffusion

Abstract Diffusion of transition metals across the cathode–electrolyte interface is identified as a key challenge for the practical realization of solid‐state batteries. This is related to the formation of highly resistive interphases impeding the charge transport across the materials. Herein, the hypothesis that formation of interphases is associated with the incorporation of Co into the Li 7 La 3 Zr 2 O 12 lattice representing the starting point of a cascade of degradation processes is investigated. It is shown that Co incorporates into the garnet structure preferably four‐fold coordinated as Co 2+ or Co 3+ depending on oxygen fugacity. The solubility limit of Co is determined to be around 0.16 per formula unit, whereby concentrations beyond this limit causes a cubic‐to‐tetragonal phase transition. Moreover, the temperature‐dependent Co diffusion coefficient is determined, for example, D 700 °C = 9.46 × 10 −14 cm 2 s −1 and an activation energy E a = 1.65 eV, suggesting that detrimental cross diffusion will take place at any relevant process condition. Additionally, the optimal protective Al 2 O 3 coating thickness for relevant temperatures is studied, which allows to create a process diagram to mitigate any degradation with a minimum compromise on electrochemical performance. This study provides a tool to optimize processing conditions toward developing high energy density solid‐state batteries.

Chemistry↗

Amphipathic Binder Integrating Ultrathin and Highly Ion-Conductive Sulfide Membrane for Cell-Level High-Energy-Density All-Solid-State Batteries

Current sulfide solid-state electrolyte (SE) membranes utilized in all-solid-state lithium batteries (ASLBs) have a high thickness (0.5–1.0 mm) and low ion conductance (<25 mS), which limit the cell-level energy and power densities. Therefore, based on ethyl cellulose's unique amphipathic molecular structure, superior thermal stability, and excellent binding capability, this work fabricates a freestanding SE membrane with an ultralow thickness of 47 µm. With ethyl cellulose as an effective disperser and a binder, the Li 6 PS 5 Cl is uniformly dispersed in toluene and possesses superior film formability. In addition, an ultralow areal resistance of 4.32 Ω cm -2 and a remarkable ion conductance of 291 mS (one order higher than the state-of-the-art sulfide SE membrane) are achieved. The ASLBs assembled with this SE membrane deliver cell-level high gravimetric and volumetric energy densities of 175 Wh kg -1 and 675 Wh L -1 , individually.

25 ENERGY STORAGE↗

Activated transport in AMTEC electrodes

Transport of alkali, metal atoms through porous cathodes of alkali metal thermal-to-electric converter (AMTEC) cells is responsible for significant reducible losses in the electrical performance of these cells. Experimental evidence for activated transport of metal atoms at grain surfaces and boundaries within some AMTEC electrodes has been derived from temperature dependent studies as well as from analysis of the detailed frequency dependence of ac impedance results for other electrodes, including thin, mature molybdenum electrodes which exhibit transport dominated by free molecular flow of sodium gas at low frequencies or dc conditions. Activated surface transport will almost always exist in parallel with free molecular flow transport, and the process of alkali atom adsorption/desorption from the electrode surface will invariably be part of the transport process, and possibly a dominant part in some cases. The temperature dependence of the diffusion coefficient of the alkali metal through the electrode in several cases provides an activation energy and preexponential, but at least two activated processes may be operative, and the activation parameters should be expected to depend on the alkali metal activity gradient that the electrode experiences. In the case of Pt/W/Mn electrodes operated for 2500 hours, limiting currents varied with electrode thickness, and the activation parameters could be assigned primarily to the surface/grain boundary diffusion process.

Williams, R. M.↗

Sulfur and Moisture Effects on Alumina Scale and TBC Spallation

It has been well established that a few ppmw sulfur impurity may segregate to the interface of thermally grown alumina scales and the underlying substrate, resulting in bond degradation and premature spallation. This has been shown for NiAl and NiCrAl-based alloys, bare single crystal superalloys, or coated superalloys. The role of reactive elements (especially Y) has been to getter the sulfur in the bulk and preclude interfacial segregation. Pt additions are also very beneficial, however a similar thermodynamic explanation does not apply. The purpose of the present discussion is to highlight some observations of these effects on Rene'142, Rene'N5, PWA1480, and PWA1484. For PWA1480, we have mapped cyclic oxidation and spallation in terms of potential sulfur interfacial layers and found that a cumulative amount of about one monolayer is sufficient to degrade long term adhesion. Depending on substrate thickness, optimum performance occurs if sulfur is reduced below about 0.2-0.5 ppmw. This is accomplished in the laboratory by hydrogen annealing or commercially by melt-fluxing. Excellent 1150 C cyclic oxidation is thus demonstrated for desulfurized Rene'142, Rene'N5, and PWA1484. Alternatively, a series of N5 alloys provided by GE-AE have shown that as little as 15 ppmw of Y dopant was effective in providing remarkable scale adhesion. In support of a Y-S gettering mechanism, hydrogen annealing was unable to desulfurize these alloys from their initial level of 5 ppmw S. This impurity and critical doping level corresponds closely to YS or Y2S3 stoichiometry. In many cases, Y-doped alloys or alloys with marginal sulfur levels exhibit an oxidative sensitivity to the ambient humidity called Moisture-Induced Delayed Spallation (MIDS). After substantial scale growth, coupled with damage from repeated cycling, cold samples may spall after a period of time, breathing on them, or immersing them in water. While stress corrosion arguments may apply, we propose that the underlying cause is related to a hydrogen embrittlement reaction: Al alloy + 3 H2O = Al(OH)3 + 3H(+) + 3e(-). This mechanism is derived from an analogous moisture-induced hydrogen embrittlement mechanism originally shown for Ni3Al and FeAl intermetallics. Consequently, a cathodic hydrogen charging technique was used to demonstrate that electrolytic de-scaling occurs for these otherwise adherent alumina scales formed on Y-doped Rene'N5, in support of hydrogen effects. Finally, some TBC observations are discussed in light of all of the above. Plasma sprayed 8YSZ coatings, produced on PWA1484 without a bond coat, were found to survive more than 1000 1-hr cycles at 1100 C when desulfurized to below 0.1 ppmw. At higher sulfur (1.2 ppmw) levels, moisture sensitivity and delayed TBC failure, referred to as Desk Top Spallation, occurred at just 200 hr. Despite a large degree of scatter, a factor of 5 in life improvement is indicated for desulfurized samples in cyclic furnace tests, confirming the beneficial effect of low sulfur alloys on model TBC systems. (DTS and moisture effects are also observed on commercially applied PVD 7YSZ coatings on Rene'N5+Y with Pt-aluminide bond coats). These types of catastrophic failure were subverted on the model system by segmenting the substrate into a network of 0.010 high ribs, spaced in. apart, prior to plasma spraying. No failures occurred after 1000 cycles at 1150 C or after 2000 cycles at 1100 C, even after water immersion. The benefit is described in terms of elasticity models and a critical buckling stress.

Smialek, James L.↗

The Impact of Anomalous Resistivity in Vacuum Contaminant Plasmas on the Electrothermal Instability

This manuscript presents an assessment of the electrothermal instability (ETI) in the presence of anomalous resistivity (AR) in vacuum contaminant plasmas (VCP) when applied to a magnetized liner inertial fusion (MagLIF)-like load.Pulsed-power driven dielectrically coated metallic liners, like in MagLIF, experience the current-driven electrothermal instability which occurs when a material’s resistivity changes with temperature and is subject to ohmic heating. Large scale pulsed-power facilities that use magnetically insulated transmission lines (MITL) have been shown to generate low-density plasma which enters the target chamber and coalesces around the load. The low-density high-temperature vacuum contaminant plasmas (VCP) can parasitically divert current from the load through causing a short in the anode-cathode gap inside the target chamber. Resistive magnetohydrodynamic (MHD) simulations of these VCP experience unphysical runaway ohmic heating due to under predicting the resistivity by using a purely collisional resistivity model.AR provides a physics-based way to address this runaway heating through increasing the resistivity in a proportional way with the drift speed. In this work, 1D simulations probe the effect that AR in VCP has on the magnetic diffusion rate, and 2D simulations show how this effect manifests in the nonlinear striation form of the ETI for a MagLIF-like load. Beryllium and aluminum dielectrically coated liners are used for the 1D and 2D simulations in this work. The1D simulations show that a VCP causes a delay in the current delivery to the load by upwards of 8 ns at 60 ns into atypical current pulse for an 1 × 10 7 A scale pulsed-power accelerator. The 2D simulations show the delay observed in the 1D simulations is reduced substantially (4 ns) by 2D turbulence that disrupts the VCP layer early in time. Here, the 2Dsimulated ETI growth varies across AR models, more so for the beryllium liner than the aluminum liner because the beryllium liner shows an enhanced rate of penetration for the magnetic diffusion wave in comparison to the aluminum liner. The 2D simulations show the bulk dielectric thickness varies across AR models with the Davidson AR model beingthe largest and the Buneman AR model being the smallest, and in connection with the thickness the Rayleigh-Taylor bubble-spike distances varies correspondingly.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗