Search NASA⌕ Search

SEARCH · Search NASA

Results for “High-temperature XRD”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 37 records · Page 2

Interdiffusion and Formation of Intermetallic Compounds in High-Temperature Power Electronics Substrate Joints Fabricated by Transient Liquid Phase Bonding

Power electronics packages typically comprise a dielectric substrate bonded to a metal layer and attached to heat sinks using a low-thermal-conductivity solder. These multiple layers increase the effective thermal resistance of the package and are responsible for package failures under cyclic thermal loads. Bonding the aluminum nitride dielectric layer (AlN) directly to a low coefficient of thermal expansion (CTE) aluminum silicon carbide (AlSiC) cold plate using copper-aluminum (Cu-Al) transient liquid phase (TLP) bonding has been shown to improve the mechanical reliability of the power electronic packages while making the package more compact by bringing the cooling solutions closer to the devices. This study aims to characterize the Cu-Al bonds formed during the TLP bonding of AlSiC with three different power electronics substrates: pure aluminum nitride (AlN), aluminum (DBA), and copper (DBC). The material compositions and microstructures of the bonds were analyzed using scanning electron microscopy (SEM), x-ray spectroscopy (EDS), confocal scanning acoustic microscopy (C-SAM), and x-ray diffraction (XRD). ..alpha..-Al solid compound was identified as the dominant phase in AlN-AlSiC and Al-AlSiC, with a notable presence of SiC particles. In contrast, three intermetallic phases - ..theta..-CuAl2, ..eta..-CuAl, and ..gamma..'- Cu9Al4 - were observed in the Cu-AlSiC bond. A computational solid-state diffusion model was developed to predict the intermetallic compounds (IMCs) formed during Cu-Al TLP bonding in each system, which supported the observation that an initial Cu volume fraction of 20 % in the material layers produced a final bond composition of >95 % Al with minimal IMC growth. However, increased Cu concentrations produced higher concentration gradients, leading to increased growth of IMCs, Kirkendall voids, and interstitial cracks.

DIRECT ENERGY CONVERSION↗

Alkali Vapor Corrosion of Spinel (MgAl 2 O 4 ) and Gahnite (ZnAl 2 O 4 ) Refractories—A Comparative Study

Alkali vapor corrosion is critical for refractories used in the kilns and furnaces of diverse high-temperature processing and manufacturing sectors such as gasifiers, cement production, and glass making. Gahnite (ZnAl 2 O 4 ) is being investigated as a potential chrome-free refractory because of its similarity with the structure and properties of magnesium aluminate (MgAl 2 O 4 ) spinel. The alkali vapor corrosion of ZnAl 2 O 4 , MgAl 2 O 4 , and Mg 0.5 Zn 0.5 Al 2 O 4 was studied, according to ASTM C987-10, at 1371°C for 24 h using sodium carbonate (Na 2 CO 3 ). The surface and the polished cross-sections of the corroded ZnAl 2 O 4 , MgAl 2 O 4 , and Mg 0.5 Zn 0.5 Al 2 O 4 specimens were analyzed using x-ray diffraction (XRD), microscopy, and energy-dispersive spectroscopy (EDS) techniques. MgO in MgAl 2 O 4 , ZnO in ZnAl 2 O 4 , Mg 0.77 Zn 0.23 O, and NaAlO 2 were detected as the corrosion products for these specimens. The extent of corrosion substantially varied among the specimens despite the similarity in the corrosion products. The corrosion resistance increased in the following order: Mg 0.5 Zn 0.5 Al 2 O 4 > MgAl 2 O 4 > ZnAl 2 O 4 . The formation of a dense MgO and Mg 0.77 Zn 0.23 O layer for MgAl 2 O 4 and Mg 0.5 Zn 0.5 Al 2 O 4 , respectively, contributed to their superior resistance to alkali vapor corrosion. The underlying corrosion mechanisms are discussed based on experimental observations supported by thermodynamic analysis. Additionally, the results suggest that a partial Zn 2+ substitution for Mg 2+ in MgAl 2 O 4 can enhance the resistance to alkali vapor corrosion.

alkali corrosion↗

Evolution of Microstructure and Surface Characteristics of FeCrAl alloys when Subjected to Flow Boiling Testing

FeCrAl alloys are candidate materials for manufacturing accident-tolerant fuel (ATF) cladding intended for light water reactors to increase fuel reliability and safety during design-basis and beyond-design-basis accident scenarios. The evolution of the materials' surface characteristics, microstructure, and mechanical properties when exposed to the Critical Heat Flux (CHF) in flow boiling testing is crucial for safety analysis while providing insights into their thermal-hydraulic performance in nuclear reactors. After CHF, the surface chemistry of two FeCrAl alloys, APMT and C26M, was studied to understand their evolution at the early stage of high-temperature excursions in short time periods. The results indicated a thin layer composed of oxides and hydroxides of Al, Cr, and Fe with varying proportions at different depths in the layer, as indicated by X-ray photoelectron spectroscopy (XPS) and depth profiling. The cross-sections prepared by focused ion beam (FIB) revealed the growth of an oxide layer, in the range of 90-180 nm thick, on the alloys' surfaces. The evolution of the materials' surface chemistry also led to a noticeable post CHF excursion increase in their wettability, with a slight increase in roughness. Further, the investigation of the materials' mechanical properties indicated a modest increase in hardness by 10-15% as well as an increase in their yield strength, as evidenced by the microindentation and ring compression tests conducted before and after CHF testing. Scanning electron Microscopy (SEM) and X-ray diffraction (XRD) were used to investigate microstructural features of the materials and their changes after CHF treatment.

36 MATERIALS SCIENCE↗

Improving Structural Integrity of Direct Laser-Deposited Ni – Co – Cr – Al – Y Superalloys by Alloy Modification

Abstract Ni- and Co-based M–Cr–Al–Y (M = Ni and/or Co), dual phase β and γ/γ′, β—Ni–Al, γ—Ni(Co, Cr), and γ′—Ni3–Al superalloys exhibit several beneficial high-temperature (>1000 °C) (2012 °F) strength and corrosion resistance properties. Our study investigates the feasibility of fabricating a commercially available Ni–Co–Cr–AlY alloy (tradename “Amdry 386”) using laser directed energy deposition (laser-DED). A significant challenge for laser fabrication of bulk Amdry 386 (A386) structures stems from the presence of relatively higher amounts of the β phase than γ/γ′ phases. While prior studies report laser fabrication of these materials in coating and cladding configurations, bulk structures have not been realized. To investigate these challenges, this study was developed to systematically evaluate the effects of modifying the A386 alloy by adding 10, 20, and 30% by weight of a Ni–20%Cr (Ni–Cr) alloy (mainly γ/γ′). Laser-DED-fabricated A386 coupons exhibited a metastable, rapidly solidified β-rich microstructure typical to laser processes. The A386 + Ni–Cr mixtures were processed using laser-DED, and small coupons from each composition were evaluated using SEM, XRD, and microhardness to characterize the as-processed microstructure. Thermodynamic modeling was performed to determine the phase evolution as a function of the alloy composition. The dominating phase switches from β to γ/γ’ between the A386 and A386 + 10% Ni–Cr mixtures, but the increase in structural integrity is not observed until the Ni–Cr additions reach a minimum of 20%. Our results show that the alloy chemistry can be successfully modified to improve the structural integrity of laser-processed structures.

Engineering↗

Synthetic Accessibility and Sodium Ion Conductivity of the Na8–x A x P2O9 (NAP) High-Temperature Sodium Superionic Conductor Framework

Advancement of solid-state electrolytes (SSEs) for all solid-state batteries typically focuses on modification of a known structural framework to improve conductivity, e.g., cation substitution for an immobile ion or varying the concentration of the mobile ions. Novel frameworks can be disruptive by enabling fast ion conduction aided by different structure and diffusion mechanisms, thereby unlocking optimal conductors with different properties. Herein, we perform a high-throughput survey of a structural framework for sodium ion conduction, Na8–x A x P2O9 (NAP), to understand the family’s thermodynamic stability, synthesizability, and ionic conduction. We show that the parent phase Na4TiP2O9 (NTP) undergoes a structural distortion (with accompanying conductivity transition) due to unstable phonons arising from pseudo-Jahn–Teller mode in the 1D titanium chains. Screening compounds in which Ti is substituted by other metals computationally reveal a number of candidates that are predicted to be low in formation energy and have high predicted ionic conductivities. High-throughput experimental and subsequent methodology optimization trials deliver one new compound, Na4SnP2O9 (NSP). X-ray diffraction (XRD), microscopy, and spectroscopy characterization indicate that the room-temperature structure of NSP is similar to the high-temperature, orthorhombic NTP phase but with some small unresolved structural differences. These uncharacterized structural details are speculated to limit the ion conductivity. Temperature-dependent XRD and electrochemical impedance spectroscopy indicate multiple coupled conductivity–structure transitions at a high temperature. We demonstrate the challenges with synthesis development and a priori identification of promising SSE phases as a major bottleneck in new (energy) materials development.

Chemical reactions↗

Solving the “Coloring Problem” in InPd 3– x Ag x ( x = 0–0.7) by Phase Diagrams Modeling and Diffraction Experiments

Here, a series of InPd 3–x Ag x (x = 0–1) compositions were synthesized by conventional high-temperature synthesis, and as-synthesized samples were characterized by powder X-ray diffraction experiments. Up to x = 0.7, InPd 3–x Ag x adopts the ternary substitutional variant of the InPd 3 structure (TiAl 3 -type), when x > 0.7, elemental Ag starts to segregate along with the main phase. Accurate structural characterization in InPd 3–x Ag x faces a critical challenge due to the narrow X-ray scattering contrast among constituents In, Pd, and Ag and nearly identical neutron scattering lengths of Pd and Ag. To overcome this “coloring problem”, a combination of calculation of phase diagrams modeling (CALPHAD) and diffraction techniques (X-ray and neutron) was employed. In the compositional range 0 ≤ x ≤ 0.7, InPd 3–x Ag x presents a ternary variant of the TiAl 3 -type structure, where Ag atoms selectively substitute one (the 2b Wyckoff site) of the two Pd sites in InPd 3 . Notably, in contrast to the isologous InPd 3–x Cu x (x = 0–1) system, Ag substitution does not form an ordered VRh 2 Sn-type structure at the limiting composition. The distinct site preference in InPd 3–x Ag x is elucidated by charge population analysis, electronic structure calculations, and orbital-resolved chemical bonding investigations, and the extent of substitution is supported by formation free energy calculations.

36 MATERIALS SCIENCE↗

High hardness and oxidation-resistant Cr-containing medium entropy ZrTaW diboride

This study reports the successful synthesis of a Cr-containing (Zr 0.30 Ta 0.34 Cr 0.06 W 0.30 )B 2 medium-entropy boride (MEB) via an in-situ reactive borothermal reduction route from oxide precursors. High-energy ball milling was employed to homogenize the precursor mixture prior to reactive densification. X-ray diffraction confirmed the formation of a predominantly AlB₂-type hexagonal diboride structure together with a secondary (W X , M 1-X )B monoboride phase. Microstructural characterization revealed compositional heterogeneity and localized W-rich regions associated with the secondary phase. The synthesized medium-entropy boride exhibited enhanced mechanical properties, which are attributed to lattice distortion and solid-solution strengthening effects. Thermogravimetric analysis revealed complex multistage oxidation behavior, and the oxidation resistance was compared with conventional ultra-high-temperature diborides. The results demonstrate the strong relationship between oxide-derived processing, compositional complexity, phase evolution, and oxidation behavior, highlighting the potential of medium-entropy borides for high-temperature structural applications

36 MATERIALS SCIENCE↗

The Thermo-Elastic Properties and Damping of U-6wt%Nb

While thermal expansion data exists for quenched (as well as aged) U-6wt%Nb, there is wide variation in the reported room temperature elastic moduli. To better understand the room temperature elastic behavior and to address the complete absence of data on the temperature dependence of the elastic moduli, room temperature and in-situ elevated temperature resonant ultrasonic spectroscopy (RUS) was performed along with x-ray diffraction (XRD) and dilatometry using a thermomechanical analyzer (TMA). An in-situ small- and wide-angle x-ray scattering (SAXS/WAXS) experiment was performed on a companion sample to help interpret the results. The room temperature polycrystalline dynamic moduli were measured to be E = 95.4 ± 4.5 GPa and G = 35.2 ± 0.2 GPa, respectively. As the temperature is raised, the stiffness slowly decreases, consistent with the empirical rule proposed by Varshni, up to the point of precipitation of the equilibrium α-U phase, which is stiffer than the martensitic phases. Homogenization theory of composites can be used to rationalize the observed response at high temperatures and after high-temperature exposures. Further, aging of the material at low temperatures (≤200°C) does not affect the linear elastic stiffness, but does impact the damping behavior which can be measured through RUS. This change in damping provides another perspective on the microstructure changes induced by low-temperature aging which also result in significant strengthening.

36 MATERIALS SCIENCE↗

Energetics of oxidation and formation of uranium monocarbide

To enable better implementation of uranium monocarbide (UC) as an advanced nuclear fuel for future high-temperature reactors, it is essential to have a thorough knowledge of its thermal and thermodynamic properties under reactor operational conditions. In this work, we studied thermal bulk oxidation of UC by simultaneous thermal analysis consisting of thermogravimetric analysis – differential scanning calorimetry coupled with evolved gas mass spectrometry (TGA-DSC-MS), and we examined the thermodynamic stability of UC using high temperature oxide melt drop solution calorimetry. Further, in air, our studied UC sample (which contains ~5 mol% UO 2 ) was found to undergo a step-wise thermal oxidation process consisting of consecutive oxidations and thermal decomposition reactions: 0.95UC·0.05UO 2 → UO 3 ·0.29(C x O y ) + 0.66CO 2 → UO 3 ·0.20(C x O y ) + 0.09CO 2 → UO 3 ·0.03(C x O y ) + 0.17CO 2 → U 3 O 8 + 0.03CO 2 + 0.166O 2 . DSC was further used to determine the enthalpies of reactions associated with this series of oxidation reactions. Synchrotron X-ray diffraction (XRD) and extended X-ray absorption spectroscopy (EXAFS) were performed to characterize both the long- and short-range structures of UC. The standard enthalpy of formation (ΔH° f ) of UC was determined to be –50.7 ± 10.8 kJ/mol·atom, in good agreement with previous values measured by bomb calorimetry. Lastly, the enthalpic landscape of U-C compounds, including UC, U 2 C 3 , and α-UC 1.94 , were established based on the enthalpy normalized per mole atom, which suggests that U-C phases are thermodynamically stable at lower C/U ratios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Phase stability and microstructure of neutron-irradiated substoichiometric yttrium dihydrides

The impact of the neutron-displacement damage on phase stability and microstructure of substoichiometric yttrium dihydrides (YH x , x <2) were investigated to assess their use as solid moderator in high-temperature nuclear reactors. YH x specimens were, thus, subjected to neutron irradiations in the range of 0.1–2 displacements per yttrium atom (dpa-Y) in the temperature range of 536–878°C at the Oak Ridge National Laboratory's (ORNL's) High Flux Isotope Reactor (HFIR). YH x specimens were initially prepared at stoichiometry (H/Y) ratios of 1.69 and 1.83. HFIR-irradiated specimens were characterized by variety of techniques to investigate H retention characteristics including dimensional analysis, optical microscopy, scanning electron microscopy electron back scatter diffraction (EBSD), transmission electron microscopy, thermal desorption spectroscopy (TDS), and high-energy x-ray diffraction (HE-XRD) characterizations. Overall, YH x exhibited notable structural and phase stability under short-term neutron-irradiation, except for the samples with significant silicon carbide (SiC) interaction at high doses and temperatures. Basic dimensional and mass measurements were misleading for accurate assessment of H retention, as confirmed by EBSD phase maps, XRD line profiles, and TDS signals. Thus, it was discussed that a robust H retention metric is needed to assess irradiated hydrides. Further, nanoscale cavities were observed as a result of the neutron irradiation in all samples. Although no clear impact of dose and irradiation temperature was determined, the initial H/Y ratio had an impact on the cavity number density where low H/Y specimens had high-resistance to cavity formation. The Y-vacancy cluster formation at the collision stage of the displacement cascade and their stabilization by H were considered to be the likely underlying mechanisms for the observed cavity microstructure.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

From phase decomposition to evaporation: A multi-modal evaluation of thermally degraded model lightweight high-entropy alloy

Lightweight high-entropy alloys (LHEAs) have the potential to replace conventional lightweight materials due to their superior mechanical properties and thermal stability. However, the thermal degradation pattern of LHEAs from phase decomposition to evaporation is not clear. We develop a new Al-based dual phase (FCC + HCP) LHEA—AlTi 0.45 CuZn, and further investigate its thermal degradation behavior for potential high-temperature structural applications. Using multimodal advanced characterization techniques such as differential scanning calorimetry/thermogravimetric analysis, scanning/transmission electron microscopy, and synchrotron X-ray diffraction/pair distribution function (XRD/PDF), a sequence of thermal degradation events beyond the thermal phase stability limit—between 250 and 360 °C—is observed. These include phase decomposition at ~360 °C, Zn evaporation at ~750 °C, and LHEA melting at 880 °C which results in ~25% cumulative weight loss. The formation of Al-Ti phase off the AlTi 0.45 CuZn matrix is due to the largest negative mixing enthalpy for Al-Ti than other binary pairs. Similarly, Zn evaporation from AlTi 0.45 CuZn LHEA is due to its faster evaporation rate than other constituent elements. The high-resolution synchrotron XRD and PDF results support the aforementioned observations; in addition, they reveal local atomic arrangements, local strain, and sluggish grain growth in the LHEA. Among other LHEAs of close density range (5.55 ≤ ρ ≤ 5.85 g/cc), the investigated LHEA exhibits outstanding nano-indentation hardness values due to the coupled grain size effect and HCP phase strengthening of the FCC matrix. As the search for LHEAs for lightweight applications grows, this study shows the potential use of AlTi 0.45 CuZn LHEA for structural applications even at elevated temperatures.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Chemical compatibility of hollow ceramic cenospheres as thermal insulation for high-temperature thermal energy storage applications with molten nitrate salt

An effective insulation material that is both thermally and chemically stable in molten salts could transform the design of molten-salt-based thermal energy storage (TES) tanks. Most current molten salt TES tanks hold the metallic tank structure in direct contact with hot salt inventory, a design which leads to thermal expansion of the tank and triggers stresses that can lead to thermomechanical failures. With an internal insulation to lower the temperature at the tank structure, the extent of thermal expansion can be reduced, thereby reducing expansion-induced stresses and allowing for consideration of lower-cost tank structure materials. Conventional insulation materials are either 1) too porous and allow molten salts to permeate into the matrix, which significantly increases the thermal conductivity or 2) too dense and have a thermal conductivity that cannot provide sufficient thermal insulation. This paper presents an alternative thermal insulation concept using cenospheres which have an alumino-silicate structure. The cost analysis suggests that the low-density cenospheres can be one of the cheapest materials to provide cost-effective thermal insulation. The chemical compatibility of cenospheres is investigated in molten 60 wt% NaNO3/40 wt% KNO3 salt which is close to industrial-grade Solar Salt. This paper shows that diffusion of the sodium and potassium cations from the salt into the cenospheres occurs based on weight analysis, energy dispersive spectroscopy (EDS), X-ray diffraction (XRD) and Fourier-transform infrared (FTIR) spectroscopy. The cation diffusion breaks the bridging oxygen bonds and causes volume expansion of the microstructure which is responsible for the failure of the cenosphere particles. The chemical composition of the cenospheres is found to affect their compatibility with molten nitrate salt. A cenosphere product with low iron content showed the best compatibility with an average survival rate of 77.9% +/- 9.8% after 7 days of immersion in the molten nitrate salt. While even the low-iron cenospheres appear to require protection from direct molten salt contact, their slow degradation rate, closed-cell porosity, and low cost hold potential for effective use as internal tank insulation.

14 SOLAR ENERGY↗

Polymorphism and phase transitions in Na 2 U 2 O 7 from density functional perturbation theory

Polymorphism and phase transitions in sodium diuranate, Na 2 U 2 O 7 , are investigated with density functional perturbation theory (DFPT). Thermal properties of crystalline α-, β- and γ-Na 2 U 2 O 7 polymorphs are predicted from DFPT phonon calculations, i.e., the first time for the high-temperature γ-Na 2 U 2 O 7 phase (R$\bar{3}$ with combining macron]m symmetry). The standard molar isochoric heat capacities predicted within the quasi-harmonic approximation are C p (298.15K)= 219.4 and 220.9 J K -1 mol -1 mfor P21/a α-Na 2 U 2 O 7 and C2/m β-Na 2 U 2 O 7 , respectively. Gibbs free energy calculations reveal that α-Na 2 U 2 O 7 (P2 1 /a) and β-Na 2 U 2 O 7 (C2/m) are almost energetically degenerate at low temperature, with β-Na 2 U 2 O 7 becoming slightly more stable than α-Na 2 U 2 O 7 as temperature increases. Here these findings are consistent with XRD data showing a mixture of α and β phases after cooling of γ-Na 2 U 2 O 7 to room temperature and the observation of a sluggish α → β phase transition above ca. 600 K. A recently observed α-Na 2 U 2 O 7 structure with P21 symmetry is also shown to be metastable at low temperature. Based on Gibbs free energy, no direct β → γ solid-solid phase transition is predicted at high temperature, although some experiments reported the existence of such phase transition around 1348 K. This, along with recent experiments, suggests the occurrence of a multi-step process consisting of initial β-phase decomposition, followed by recrystallization into γ-phase as temperature increases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Correlations Between In-Line X-ray Diffraction Data and In-Field Critical Current of Long, 4-μm Thick Film REBCO Tapes Made by Advanced MOCVD

REBa 2 Cu 3 O 7-δ (REBCO, RE = rare earth) tapes with high critical current can be very impactful in high magnetic field applications at low temperatures and power applications at high temperatures. A pilot-scale Advanced Metal Organic Chemical Vapor Deposition (MOCVD) method was used to fabricate 50-m-long, 4+μm-thick REBCO tape in a single pass. Critical currents 3.3x that of commercial HTS tapes were achieved at 20 K, 12 T in these 50-m-long tapes. An in-line 2D X-ray Diffraction (XRD) system has been used to assess the quality of the long tapes in real-time, during manufacturing. The key peaks of REBCO, REO, and BZO phases were identified and utilized for tape quality analysis. Furthermore, a 20-m tape made by Advanced MOCVD was tested over its entire length by reel-to-reel (R2R) scanning Hall-probe microscopy (SHPM) at 65 K, 0.25 T, 2 T, and 4 T. 4-mm-wide strands of Advanced MOCVD tapes showed mean critical currents at 65 K of 530 A, 200 A, and 104 A at 0.25 T, 2 T, and 4 T respectively. The combined use of in-line and offline characterization techniques provides a reliable approach for assessing long REBCO tapes during manufacturing, serving as an effective feedback source for quality control in scaled-up REBCO tape deposition processes. This advancement contributes to the production of longer and more uniform high-performance REBCO tapes for large-scale, high-field superconducting applications

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Influence of pre-existing defects on thermal transport in nuclear graphite

Nuclear graphite is a critical material in high-temperature nuclear reactors due to its superior thermal and mechanical properties. The manufacturing process leaves multi-scale ‘pre-existing’ defects that can affect thermal transport characteristics. Because these defects are remnant of graphitization temperature, they cannot be thermally annealed. This study employs a non-thermal electron wind force (EWF) annealing technique to avoid this obstacle. 2 min of EWF treatment of the as-received graphite IG-110 at temperatures below 100 °C led up to 67% increase in thermal diffusivity and ~ 35% decrease in electrical resistivity in average. Differential scanning calorimetry also showed similar outcome for specific heat. X-ray diffraction characterization was performed by fitting a bi-modal crystallite size distribution model to reveal the enhancement in crystallinity after the EWF treatment. The findings emphasize the potential of EWF annealing for optimizing thermal performance in nuclear graphite and its implications for reactor efficiency and safety.

Annealing↗

Oxygen Reduction on Platinum-Nickel and Platinum-Cobalt Alloy Based Catalysts for High Temperature Proton Exchange Membrane Fuel Cells

Catalyst layers, with commercial PtNi/TKK (TECNiE52; platinum 46.5 wt%), PtCo/TKK (TEC36E52; platinum 45.8 wt%) catalysts, and an in-house catalyst PtNi-NC (platinum 38.4 wt%), synthesised using acoustic mixer and a tube furnace, are prepared using three different ionomers: 20 wt% Nafion®, 60 wt% polytetrafluoroethylene (PTFE), and an in-house 5 wt% ionomer (‘Ionomer X’). These inks are bar-coated onto carbon paper gas diffusion layers (GDLs), which are cut into 3 cm × 5 cm pieces. The coated layers are tested for oxygen reduction in a commercial gas diffusion electrode (GDE) test cell, FlexCell® (Gaskatel GmbH, Germany), using 85 wt% phosphoric acid at both room temperature and at 155°C. This study evaluates the polynorbornene (PNB)-based in-house ionomer performance as binder and in-house catalyst oxygen reduction reaction (ORR) activity in comparison to commercial products. The catalyst layers are characterised using X-ray diffraction (XRD) analysis, X-ray photoelectron spectroscopy (XPS), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). Among the catalyst layers prepared with PTFE ionomer and tested at 155°C, the in-house catalyst demonstrates the highest ORR activity. Ionomer X proves to be a good candidate to be used as a per- and polyfluoroalkyl-free binder for high-temperature (HT) proton exchange membrane fuel cell (PEMFC) applications.

85 wt% phosphoric acid↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Modified Calcium Manganites for Thermochemical Energy Storage Applications

CaAl 0.2 Mn 0.8 O 3-δ (CAM28) and CaTi 0.2 Mn 0.8 O 3-δ (CTM28) are perovskite metal oxides developed for high-temperature thermochemical energy storage (TCES) applications, e.g., in support of air Brayton power generation. Previous reports for these compounds focus on the equilibrium non-stoichiometry (δ) as a function of temperature and oxygen partial pressure (pO 2 ) and the endotherm (or exotherm) accompanying changes in δ resulting from thermal reduction (or re-oxidation). Herein, we report results for elemental substitution and doping (Al, Co, Fe, La, Sr, Ti, Y, Zn, and Zr) of calcium manganites (CM) that establish the preference for CAM28 and CTM28. Techniques employed include conventional (screening and equilibrium) and ballistically heated multi-cycle thermogravimetric analysis (TGA), conventional and high temperature ( in-situ ) X-ray diffraction (XRD), and differential scanning calorimetry (DSC). Forward-looking results for A-site Y-doped materials, e.g., Ca 0.9 Y 0.1 MnO 3-δ (CYM910), establish a route to increasing the reduction enthalpy relative to CAM28 and CTM28, albeit at the expense of increased reduction temperatures and raw materials costs. A thermodynamic model presented for CAM28, but extendable to related materials, provides values for the reaction enthalpy and extent of reduction as a function of temperature and oxygen partial pressure for use in design efforts. Taken as a whole, the results support the choice of Al-doped CaMnO 3-δ as a low-cost material for TCES in a high temperature air Brayton application, but point the way to achieving higher stored energy densities that could lead to overall cost savings.

Miller, James E.↗