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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.

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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Highly Oxidized Oxide Surface toward Optimum Oxygen Evolution Reaction by Termination Engineering

The oxygen evolution reaction (OER) is a critical step for sustainable fuel production through electrochemistry process. Maximizing active sites of nanocatalyst with enhanced intrinsic activity, especially the activation of lattice oxygen, is gradually recognized as the primary incentive. Since the surface reconfiguration to oxyhydroxide is unavoidable for oxygen-activated transition metal oxides, developing a surface termination like oxyhydroxide in oxides is highly desirable. In this work, we demonstrate an unusual surface termination of (111)-facet Co 3 O 4 nanosheet that is exclusively containing edge-sharing octahedral Co 3+ similar to CoOOH that can perform at approximately 40 times higher current density at 1.63 V (vs RHE) than commercial RuO 2 . It is found that this surface termination has an oxidized oxygen state in contrast to standard Co-O systems, which can serve as active site independently, breaking the scaling relationship limit. Finally, this work forwards the applications of oxide electrocatalysts in the energy conversion field by surface termination engineering.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Formation of Branched Ruthenium Nanoparticles for Improved Electrocatalysis of Oxygen Evolution Reaction

Branched nanoparticles are one of the most promising nanoparticle catalysts as their branch sizes and surfaces can be tuned to enable both high activity and stability. Understanding how the crystallinity and surface facets of branched nanoparticles affect their catalytic performance is vital for further catalyst development. In this work, a synthesis is developed to form highly branched ruthenium (Ru) nanoparticles with control of crystallinity. It is shown that faceted Ru branched nanoparticles have improved stability and activity in the oxygen evolution reaction (OER) compared with polycrystalline Ru nanoparticles. Here, this work achieves a low 180 mV overpotential at 10 mA cm –2 for hours, demonstrating that record–high stability for Ru nanocrystals can be achieved while retaining high activity for OER. The superior electrocatalytic performance of faceted Ru branched nanoparticles is ascribed to the lower Ru dissolution rate under OER conditions due to low–index facets on the branch surfaces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Ostwald ripening of faceted Si particles in an Al-Si-Cu melt

The microstructural evolution of an Al-Si-Cu alloy during Ostwald ripening is imaged via synchrotron-based, four-dimensional (i.e., space and time resolved) X-ray tomography. Samples of composition Al-32 wt%Si-15 wt%Cu were annealed isothermally at 650 °C, in the two-phase solid-liquid regime, while tomographic projections were collected in situ over the course of five hours. Advances in experimental methods and computational approaches enable us to characterize the local interfacial curvatures and velocities during ripening. The sequence of three-dimensional reconstructions and interfacial shape distributions shows highly faceted Si particles in a copper-enriched liquid, that become increasingly isotropic or rounded over time. In addition, we find that the coarsening rate constant is approximately the same in the binary and ternary systems. By coupling these experimental measurements with CALPHAD modeling and ab initio molecular dynamics simulation, we assess the influence of Cu on the coarsening process. Lastly, we find the unusual “pinning” of microstructure at the junction between rough and smooth interfaces and suggest a mechanism for this behavior.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Irradiation-induced grain boundary facet motion: In situ observations and atomic-scale mechanisms

Metals subjected to irradiation environments undergo microstructural evolution and concomitant degradation, yet the nanoscale mechanisms for such evolution remain elusive. Here, we combine in situ heavy ion irradiation, atomic resolution microscopy, and atomistic simulation to elucidate how radiation damage and interfacial defects interplay to control grain boundary (GB) motion. While classical notions of boundary evolution under irradiation rest on simple ideas of curvature-driven motion, the reality is far more complex. Focusing on an ion-irradiated Pt Σ3 GB, we show how this boundary evolves by the motion of 120° facet junctions separating nanoscale {112} facets. Our analysis considers the short- and mid-range ion interactions, which roughen the facets and induce local motion, and longer-range interactions associated with interfacial disconnections, which accommodate the intergranular misorientation. We suggest how climb of these disconnections could drive coordinated facet junction motion. These findings emphasize that both local and longer-range, collective interactions are important to understanding irradiation-induced interfacial evolution.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2013

Hydrogen adsorption and desorption at the Pt(110)-(1×2) surface: experimental and theoretical study

The interaction of hydrogen with the Pt(110)-(1×2) surface is studied using temperature programmed desorption (TPD) measurements and density functional theory (DFT) calculations. The ridges in this surface resemble edges between micro-facets of Pt nano-particle catalysts used for hydrogen evolution (HER) and hydrogen oxidation reactions (HOR). The binding energy and activation energy for desorption are found to depend strongly on hydrogen coverage. At low coverage, the strongest binding sites are found to be the low coordination bridge sites at the edge and this is shown to agree well with the He-atom interaction and work function change which have been reported previously. At higher hydrogen coverage, the higher coordination sites on the micro-facet and in the trough get populated. The simulated TPD spectra based on the DFT results are in close agreement with our experimental spectra and provide microscopic interpretation of the three measured peaks. The lowest temperature peak obtained from the surface with highest hydrogen coverage does not correspond to desorption directly from the weakest binding sites, the trough sites, but is due to desorption from the ridge sites, followed by subsequent, thermally activated rearrangement of the H-adatoms. The reason is low catalytic activity of the Pt-atoms at the trough sites and large reduction in the binding energy at the ridge sites at high coverage. The intermediate temperature peak corresponds to desorption from the micro-facet. The highest temperature peak again corresponds to desorption from the ridge sites, giving rise to a re-entrant mechanism for the thermal desorption.

Gudmundsdóttir, Sigrídur↗
DOE OSTI2023

High-Resolution Thermal Profiling of a High-Power Diode Laser Facet During Aging

Here, we study the facet temperature distribution of a high-power diode laser over its lifetime using a noncontact, high spatial resolution CCD-based thermoreflectance technique. Based on the known correlation between non-radiative defects and heating, thermal maps can provide valuable information regarding the formation and evolution of small point defects that are at or near the facet during aging. In the laser under study in this work we measure the appearance of local hot spots on the facet, including concentrated hot spots that appear just before or just after COD and are correlated with loss of local light emission. The locations of these hot spots do not exhibit morphology changes in high-resolution SEM imaging of the facet, indicating that the related defects are too small to be observable in SEM or are located at some depth under the facet. Prior to COD, we measure a gradual facet temperature increase accompanied by a gradual optical power decrease and gradual facet optical absorption increase, indicating gradual degradation of the laser.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Probing Structural Reconstruction of Metal Nanoparticles under Annealing and Water Vapor Conditions: A Theoretical Study

Knowing the structural reconstruction of metal nanoparticles (NPs) under working conditions is of great importance to catalytic processes. Here, using Wulff construction combined with density functional theory (DFT) and molecular dynamics (MD) simulation, we investigated truncated octahedron-based Rh and Ir NPs (3.5, 5.5, and 9.5 nm in size) with different morphology for their structural reconstruction under annealing and water vapor conditions. Our MD results show that the NPs with lower average atomic coordination number ($\overline{CN}$) of surface atoms have lowered structural transformation inertness and thermal stability, resulting in more severe structural transition especially for smaller-sized NPs and Ir NPs. Under water vapor conditions, the competition between the interfacial tension ($γ^{\overline{int}}_{hkl}$) of (111) and (110) facets plays a major role in driving the shape evolution of Rh and Ir NPs by minimizing the total surface tension. It is revealed that annealing in vacuum/water vapor condition is an irreversible/reversible process on Rh and Ir NPs. We identified that the total adsorbate–metal ($γ^{\overline{int}}_{hkl}$) can serve as a key stability parameter for describing the potential energy surface of adsorbate–metal NP system in a variable gaseous environment (P, T).

36 MATERIALS SCIENCE↗
DOE OSTI2019

The Gulf Nuclear Energy Infrastructure Institute (GNEII): Origins, Objectives, and Operations—A Joint Report

The Gulf Nuclear Energy Infrastructure Institute (GNEII—pronounced "genie") seeks to develop expertise among future leaders of Gulf-region nuclear power programs in global standards, norms and best practices in nuclear energy programs. More specifically, the institute aims to contribute to the enhancement of nuclear security, safety, and safeguards (the so-called nuclear "3S") by providing an avenue for regional nuclear interaction, technical collaboration, lessons-learned discussions, and best-practices sharing. It is a multidisciplinary human capacity development institute offering education, research and technical services to support responsible nuclear energy programs in the Gulf and Middle East regions. In this Joint Report, Chapter 2 discusses GNEII's origins (including drivers, milestones, and design principles), Chapter 3 discusses GNEII's objectives (including goals, mission, and vision), Chapter 4 discusses GNEII's operations (including education, research, and technical service pillars), Chapter 5 discusses major insights and next steps, and Chapter 6 provides a list of publications offering additional depictions and details of GNEII's evolution. Though only one piece of a multi-faceted, multi-national effort to develop human infrastructure needs for nascent nuclear energy programs, GNEII offers a model that addresses the socio-technical attributes of nuclear 3S that can be replicated globally.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗
DOE OSTI2022

Building the Next Generation Through 20 Years of Solar Decathlon: From Collegiate Prize to Multifaceted Clean Energy Workforce Program: Preprint

The U.S. Department of Energy Solar Decathlon, initiated in 2002 as a collegiate competition that challenges student teams to design and build high-performance, low-carbon buildings powered by renewables, has always been about developing students to be the next generation of buildings professionals. As we celebrate the 20th anniversary of the Solar Decathlon in 2022, this paper highlights its evolution from a singular prize to a multi-faceted platform preparing the broader buildings workforce to address the challenges of climate change. The original program challenged students to design and construct a residence. To improve the accessibility of the competition, the Design Challenge -- a 1-2 semester design-only competition-- was added to the Solar Decathlon platform. The Solar Decathlon has also scaled globally with events in Europe, the Middle East, China, Latin America and the Caribbean, Africa, and India. In 2021, the Solar Decathlon broadened its reach once again by introducing Solar Decathlon Pro, a zero-energy design practicum for professional architects and engineers. This paper utilizes participation data, surveys, alumni profiles, project submissions, and more to understand how changes to the program have expanded program reach to minority-serving institutions, environmental justice communities, and impacted the building industry's capacity to construct high performance and zero energy buildings. As one of the oldest federal government prizes, the Solar Decathlon offers a roadmap for dramatically increasing prize impact and demonstrates that it continues to push boundaries to tackle decarbonization and environmental justice.

build↗
DOE OSTI2016

Self-decorated Au nanoparticles on antireflective Si pyramids with improved hydrophobicity

Post-deposition annealing mediated evolution of self-decorated Au nanoparticles (NPs) on chemically etched Si pyramids is presented. A distinct transformation of Si surfaces from hydrophilic to hydrophobic is initially found after chemical texturing, showing an increase in contact angle (CA) from 58° to 98° (±1°). Further improvement of hydrophobicity with CA up to ∼118° has been established after annealing a 10 nm thick Au-coated Si pyramids at 400 °C that led to the formation of Au NPs on Si facets along with self-ordering at the pyramid edges. Detailed x-ray diffraction studies suggest the evolution of crystalline Au NPs on strained Si facets. Microstructural studies, however, indicate no mixing of Au and Si atoms at the Au/Si interfaces, instead of forming Au nanocrystals at 400 °C. The improved hydrophobicity of Si pyramids, even with Au NPs can be explained in the light of a decrease in solid fractional surface area according to Wenzel's model. Moreover, a sharp drop in specular reflectance from Si pyramids in the range of 300–800 nm, especially in the ultraviolet region up to ∼0.4% is recorded in the presence of Au NPs by ultraviolet-visible spectroscopy, reflecting the possible use in photovoltaic devices with improved antireflection property.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Influence of Annealing Temperature on the OER Activity of NiO(111) Nanosheets Prepared via Microwave and Solvothermal Synthesis Approaches

Earth-abundant transition metal oxides are promising alternatives to precious metal oxides as electrocatalysts for the oxygen evolution reaction (OER) and are intensively investigated for alkaline water electrolysis. OER electrocatalysis, like most other catalytic reactions, is surface-initiated, and the catalyst performance is fundamentally determined by the surface properties. Most transition metal oxide catalysts show OER activities that depend on the predominantly exposed crystal facets/surface structure. Therefore, the design of synthetic strategies to obtain the most active crystal facets is of significant research interest. In this work, rock salt NiO OER catalysts with (111) predominantly exposed facets were synthesized by a solvothermal (ST) method either heated under supercritical or microwave-assisted (MW) conditions. Particular emphasis was placed on the influence of the post annealing temperature on the structural configuration and OER activity to compare their catalytic performances. The as-prepared electrocatalysts are pure α-Ni hydroxides which were converted to rock salt NiO (111) nanosheets with hexagonal pores after heat treatment at different temperatures. The OER activity of the electrodes has been evaluated in 0.1 M KOH using geometric and intrinsic current densities via normalization by the disk area and BET area, respectively. The lowest overpotential at a geometric current density of 10 mA/cm 2 is found for samples pretreated by heating between 400 and 500 °C with a catalyst loading of 115 μg/cm 2 . Despite the very similar nature of the catalysts obtained from the two methods, the ST electrodes show a higher geometric and intrinsic current density for 500 °C pretreatment. The MW electrodes, however, achieve an optimal geometric current density for 400 °C pretreatment, while their intrinsic current density requires pretreatment over 600 °C. Interestingly, pretreated electrodes show consistently higher OER activity as compared to the poorly crystalline/less ordered hydroxide as-prepared electrocatalysts. Thus, our study highlights the importance of the synthesis method and pretreatment at an optimal temperature.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Exploring Cr and molten salt interfacial interactions for molten salt applications

Molten salts play an important role in various energy-related applications such as high-temperature heat transfer fluids and reaction media. However, the extreme molten salt environment causes the degradation of materials, raising safety and sustainability challenges. A fundamental understanding of material–molten salt interfacial evolution is needed. This work studies the transformation of metallic Cr in molten 50/50 mol% KCl–MgCl 2 via multi-modal in situ synchrotron X-ray nano-tomography, diffraction and spectroscopy combined with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Notably, in addition to the dissolution of Cr in the molten salt to form porous structures, a δ-A15 Cr phase was found to gradually form as a result of the metal–salt interaction. This phase change of Cr is associated with a change in the coordination environment of Cr at the interface. DFT and AIMD simulations provide a basis for understanding the enhanced stability of δ-A15 Cr vs. bcc Cr, by revealing their competitive phase thermodynamics at elevated temperatures and probing the interfacial behavior of the molten salt at relevant facets. This study provides critical insights into the morphological and chemical evolution of metal–molten salt interfaces. Finally, the combination of multimodal synchrotron analysis and atomic simulation also offers an opportunity to explore a broader range of systems critical to energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Emergence of complex-regular eutectic patterns in Al–Ge: Observations from correlative nano-imaging

Eutectic solidification exemplifies nonequilibrium pattern formation, making it a well-studied moving boundary problem. Yet the mechanisms behind the formation of complex-regular microstructures – particularly in highly anisotropic systems with a significant volume fraction of a faceted phase – remain poorly understood. Our understanding of such systems is made complicated by the nonlinear interface kinetics and unique growth dynamics characteristic of faceted phases. To address these challenges, we investigate a model Al–Ge eutectic system, where the faceted Ge phase constitutes a substantial volume fraction (~0.35) and where the two solid phases arrange into so-called “fishbone” or “feather” complex-regular patterns. Using synchrotron-based x-ray nano-imaging and nanotomography with high spatial resolution (22 nm per pixel), we capture in real-time the evolution of the solid–liquid interfaces and the resulting three-dimensional microstructures in this faceted/non-faceted eutectic system. By integrating these observations with electron backscattered diffraction, we elucidate the crystallographic biases on the solidification process and the mechanisms driving the formation of such complex-regular microstructures. These findings inform a new growth model for irregular eutectics in (near-)symmetrical phase diagrams, offering insight on advanced microstructural design and processing strategies. More broadly, we demonstrate how interfacial curvature is generated in irregular eutectic alloys and how it depends on the volume fraction of the faceted phase.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Direct Visualization and Control of Atomic Mobility at {100} Surfaces of Ceria in the Environmental Transmission Electron Microscope

We report that ceria is one of the world’s most prominent material for applications in heterogeneous catalysis, as catalyst support or catalyst itself. Despite an exhaustive literature on the structure of reactive facets of CeO 2 in line with its catalytic mechanisms, the temporal evolution of the atomic surface structure exposed to realistic redox conditions remains elusive. Here, we provide a direct visualization of the atomic mobility of cerium atoms on {100} surfaces of CeO 2 nanocubes at room temperature in high vacuum, O 2 , and CO 2 atmospheres in an environmental transmission electron microscope. Lastly, through quantification of the cationic mobility, we demonstrate the control of the surface dynamics under exposure to O 2 and CO 2 atmospheres, providing opportunities for a better understanding of the intimate catalytic mechanisms.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Planarizing Spalled GaAs(100) Surfaces by MOVPE Growth

III-V photovoltaic devices have demonstrated exceptional performance across various applications, with controlled crystal fracturing, known as controlled spalling, emerging as a promising method to reduce costs by enabling substrate reuse. Spalling GaAs(100) substrates, a commonly used substrate in III-V photovoltaics, results in faceted ridges that must be planarized to grow high-quality photovoltaic devices. Here, in this study, we demonstrate that a GaAs(100) wafer offcut toward [$0\bar{11}$] and spalled toward [$011$] can be efficiently planarized by growing C:GaAs by metal-organic vapor phase epitaxy (MOVPE) on the surface, with up to 95% of the nominally deposited material used to fill the valleys between ridges. We find that reducing the offcut to 2° enhances the planarizing capability of C:GaAs. A surface morphology model indicates that the density of surface dangling bonds significantly influences the growth evolution of undoped GaAs surfaces. In contrast, the model suggests that the effectiveness of C:GaAs as a smoothing layer stems from modifying the atomic surface structure and, consequently, the associated sticking coefficients of the facets, which can alter the evolution of surface morphology. Our findings provide guidelines for the epitaxial planarization of semiconductor surfaces and improve the understanding of MOVPE growth on nonplanar surfaces.

14 SOLAR ENERGY↗
DOE OSTI2022

Electrochemical Control of the Morphology and Functional Properties of Hierarchically Structured, Dendritic Cu Surfaces

Electrodeposited dendritic copper foams have been extensively studied as an electrocatalyst for CO 2 reduction reaction (CO 2 RR). Many parameters, such as dendrite size, porosity, pore size, and crystal faceting, define the hierarchical properties of these structures and their subsequent bubble evolution and CO 2 RR capabilities. Herein, the effects the electrodeposition conditions (potential, pH) have on the resulting crystallinity, microstructure, and macroporosity of the copper foam are studied. These morphological differences and the corresponding effects on electrocatalytic activity are characterized. It is shown that the composition of the electrodeposition bath can have significant effects on the mechanics of bubble formation and detachment at the surface during hydrogen evolution reaction in acidic solutions. Similarly, the electrodeposition conditions for the synthesis of the foam affect the product selectivity during CO 2 RR electrocatalysis. As a result, foams deposited in alkaline electrodeposition solutions show high faradaic efficiency and specificity toward C 2 H 6 , an uncommon product of CO 2 RR, at modest applied potentials (−0.8 V versus reversible hydrogen electrode.

14 SOLAR ENERGY↗
DOE OSTI2014

Strain relaxation of GaAs/Ge crystals on patterned Si substrates

We report on the mask-less integration of GaAs crystals several microns in size on patterned Si substrates by metal organic vapor phase epitaxy. The lattice parameter mismatch is bridged by first growing 2-μm-tall intermediate Ge mesas on 8-μm-tall Si pillars by low-energy plasma enhanced chemical vapor deposition. We investigate the morphological evolution of the GaAs crystals towards full pyramids exhibiting energetically stable (111) facets with decreasing Si pillar size. The release of the strain induced by the mismatch of thermal expansion coefficients in the GaAs crystals has been studied by X-ray diffraction and photoluminescence measurements. The strain release mechanism is discussed within the framework of linear elasticity theory by Finite Element Method simulations, based on realistic geometries extracted from scanning electron microscopy images.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Multiple Reaction Pathways for the Oxygen Evolution Reaction May Contribute to IrO 2 (110)’s High Activity

Density functional theory calculations in conjunction with statistical mechanical arguments are performed on the rutile IrO 2 (110) facet in order to characterize multiple reaction pathways on the surface at the highest active limit (the stoichiometric surface with all metal sites available) and at the lowest active limit (the oxygen-terminated surface). Alternative pathways to the oxygen evolution reaction (OER) are found, with multiple pathways determined at each step of the four proton-coupled electron transfer reaction. Of particular interest is the detailed characterization of a co-adsorption pathway utilizing neighboring, adsorbed O, OH species in order to evolve oxygen; activation energies of this pathway are <0.5 eV and therefore easily surmountable at the high operating potentials of OER. We also determined that surface Ir atoms can potentially participate in deprotonating an OOH* intermediate; the activation energy to this is 0.67 eV on the oxygen-terminated surface. These theoretical findings explain in part the high activity present in iridium oxide catalysts and also provide insight into the mechanistic pathways available on metal oxide catalysts, which may require the concerted interaction of nearest neighbor co-adsorbates to produce chemicals of interest.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗