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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 1,693 records · Page 94
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

One-Step Synthesis and Operando Electrochemical Impedance Spectroscopic Characterization of Heterostructured MoP–Mo 2 N Electrocatalysts for Stable Hydrogen Evolution Reaction

Here this study presents a novel synthesis of self-standing MoP and Mo 2 N heterostructured electrocatalysts with enhanced stability and catalytic performance. Facilitated by the controlled phase and interfacial microstructure, the seamless structures of these catalysts minimize internal resistivity and prevent local corrosion, contributing to increased stability. The chemical synthesis proceeds with etching step to activate the surface, followed by phosphor-nitriding in a chemical vapor deposition chamber to produce MoP-Mo 2 N@Mo heterostructured electrocatalysts. X-ray diffraction analyses confirm the presence of MoP, Mo 2 N, and Mo phases in the electrocatalyst. Morphology studies using scanning electron microscopy characterizes the hierarchical growth of structures, indicating successful formation of the heterostructure. X-ray photoelectron spectroscopy (XPS) analyses of the as-synthesized and post-catalytic activity samples reveal the chemical shift in terms of binding energy (BE) of Mo 3d XPS peak, especially after catalytic activity. The XPS BE shifts attributed to changes in oxidation state, electron transfer, and surface reconstruction during catalysis. Electrochemical evaluation of the catalysts demonstrates the superior performance of the MoP-Mo 2 N@Mo heterostructured catalyst in hydrogen evolution reactions (HER), with lower overpotentials and enhanced Tafel slopes. Stability tests reveal changes in double layer capacitance over time, suggesting surface reconstruction and increased active surface area during catalysis. Operando electrochemical impedance spectroscopy (EIS) further elucidates the dynamic changes in resistance and charge transfer during HER. Overall, comprehensive understanding of the synthesis, characterization, and electrochemical behavior of the developed MoP-Mo 2 N@Mo heterostructured electrocatalyst as presented in this paper highlights their potential utilization in sustainable energy applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Coupled Marangoni-Benard/Rayleigh-Benard Instability with Temperature Dependent Viscosity

The onset of convection induced by coupled surface tension gradient and buoyancy forces is investigated with temperature dependent viscosity. Both surface tension and viscosity are assumed to vary linearly with temperature. The limiting case, Ma=0, is the buoyancy driven convection problem typically referred to as the Rayleigh-Benard stability problem. The other limiting case, Ra=0, is the surface tension (gradient) driven flow problem referred to as the Marangoni-Benard problem. The equations and boundary conditions obtained from the linear analysis are solved numerically as a generalized eigenvalue problem. Neutral stability curves for different viscosity slopes have been generated for the Marangoni-Benard and Rayleigh-Benard problems. It is shown that the curves can be collapsed to a single curve by appropriately scaling the results for each of the limiting cases. The critical Marangoni number is determined as a function of the slope of the viscosity temperature variation, epsilon, for different values of the Rayleigh number. When the viscosity decreases linearly with temperature, the coupled buoyancy-surface tension problem, including the limiting cases of Ra=0 and Ma=0, is found to be more stable than the constant viscosity case.

Skarda, J. Raymond Lee↗
DOE OSTI2023

Ab Initio Molecular Dynamics Study of Pd Nucleation on a γ-Al 2 O 3 Surface

We perform ab initio molecular dynamics (AIMD) free energy simulations to investigate the stability and dynamics of dispersed Pd atoms and subnanometer clusters on γ-Al 2 O 3 . We consider nucleation for varying Pd loadings on dry γ-Al 2 O 3 (100), dry γ-Al 2 O 3 (110) and wet γ-Al 2 O 3 (110) and examine temperature, entropy and water coverage effects on the stability and dynamics of Pd clusters. At low Pd loading (1.07 Pd atoms/nm 2 on the (100) and 0.75 Pd/nm 2 on the (110)), association of the Pd atoms is thermodynamically unfavorable on the dry surfaces and almost thermoneutral on the wet (110) owing to water blocking of the AlIII defect sites. In agreement with past studies, the Pd atoms are quite mobile but the diffusion free energy barriers do not increase with the water coverage, as previously suggested, but rather remain similar in magnitude owing to translational entropy at finite temperatures. At these Pd loadings, oxidized Pd(II) atoms on the wet (110) surface are dispersed and immobile. At higher Pd loading (1.12 and 1.5 Pd atoms/nm 2 ) on the (110) surface, Pd 3 and Pd 4 clusters are thermodynamically very stable and form fast. At the 1.12 Pd atoms/nm 2 loading, the formation of the Pd 3 cluster is two orders of magnitude slower when the surface is hydroxylated as the system becomes somewhat trapped before the dinuclear cluster Pd 2 collides with a Pd atom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Non-encapsulation approach for high-performance Li–S batteries through controlled nucleation and growth

Sulfur encapsulation in high surface area, nanoporous carbon is currently the most widely studied approach to improve the cycling stability of Li-S batteries. However, the relatively large amount of high surface area carbon decreases the overall volumetric energy density in the system and makes it difficult to compete with other battery chemistries. In this paper, we report a new approach that does not depend on sulfur encapsulation and high surface area carbon. We investigate the nucleation and deposition of sulfur using low surface area carbon in the cathode (surface area 17 m2 g-1). Optimization of the solvent properties and the deposition condition produce large spherical porous agglomerated particles rather than thin films. A solution mediated nucleation and growth mechanism is identified to form the large porous polysulfide particles. This new mechanism leads to close to 100% sulfur utilization, almost no capacity fading, over 99% coulombic efficacy, and high energy density (2350 Wh kg-1 and 2600 Wh L-1 based on overall mass/volume of cathode). This study may open a fundamentally new approach of using a low surface area carbon host for designing high energy Li-S battery by controlling the nucleation/growth pathway and morphology of sulfur species.

Environmental Molecular Sciences Laboratory↗
NASA NTRS2021

Evidence that Horizontal Moisture Advection Regulates the Ubiquitous Amplification of Rainfall Variability over Tropical Oceans

The column moist static energy (MSE) budget equation approximates the processes associated with column moistening and drying in the tropics, and is therefore predictive of precipitation amplification and decay. We use ERA-Interim (ERA-I) and TRMM 3B42 data to investigate day-to-day convective variability and distinguish the roles of horizontal MSE (or moisture) advection versus vertical advection, sources, and sinks. Over tropical convergence zones, results suggest that horizontal moisture advection is a primary driver of day-to-day precipitation fluctuations; when drying via horizontal moisture advection is smaller (greater) than Chikira’s “column process,” precipitation tends to amplify (decay). In the absence of horizontal moisture advection, precipitation tends to increase spontaneously almost universally through a positive column process feedback. This bulk positive feedback is characterized by negative effective gross moist stability (GMS), which is maintained throughout the tropical convergence zones. How this positive feedback is achieved varies geographically, depending on the shape of vertical velocity (omega) profiles. In regions where omega profiles are top-heavy, the effective GMS is negative primarily owing to strong feedbacks between convection and diabatic MSE sources (radiative and surface fluxes). In these regions, vertical MSE advection stabilizes the atmosphere (positive vertical GMS). Where omega profiles are bottom-heavy, by contrast, a positive feedback is primarily driven by import of MSE through a shallow circulation (negative vertical GMS). The diabatic feedback and vertical GMS are in a seesaw balance, offsetting one another. Our results suggest that ubiquitous convective variability is amplified by the same mechanism as moisture-mode instability.

horizontal moisture advection↗
NASA NTRS1992

Ranging performance of satellite laser altimeters

Topographic mapping of the earth, moon and planets can be accomplished with high resolution and accuracy using satellite laser altimeters. These systems employ nanosecond laser pulses and microradian beam divergences to achieve submeter vertical range resolution from orbital altitudes of several hundred kilometers. Here, we develop detailed expressions for the range and pulse width measurement accuracies and use the results to evaluate the ranging performances of several satellite laser altimeters currently under development by NASA for launch during the next decade. Our analysis includes the effects of the target surface characteristics, spacecraft pointing jitter and waveform digitizer characteristics. The results show that ranging accuracy is critically dependent on the pointing accuracy and stability of the altimeter especially over high relief terrain where surface slopes are large. At typical orbital altitudes of several hundred kilometers, single-shot accuracies of a few centimeters can be achieved only when the pointing jitter is on the order of 10 mu rad or less.

Gardner, Chester S.↗
NASA NTRS1992

Ranging performance of satellite laser altimeters

Detailed expressions for the range and pulse width measurement accuracies are developed and used to evaluate the ranging performances of several satellite laser altimeters currently under development by NASA for launch during the next decade. The analysis includes the effects of the target surface characteristics, spacecraft pointing jitter, and waveform digitizer characteristics. The results show that ranging accuracy is critically dependent on the pointing accuracy and stability of the altimeter especially over high relief terrain where surface slopes are large. At typical orbital altitudes of several hundred kilometers, single-shot accuracies of a few centimeters can be achieved only when the pointing jitter is on the order of 10 microrad or less.

Gardner, Chester S.↗
DOE OSTI2018

Speciation and Electronic Structure of La 1-x Sr x CoO 3-δ During Oxygen Electrolysis

Cobalt-containing perovskite oxides are promising electrocatalysts for the oxygen evolution reaction (OER) in alkaline electrolyzers. However, a lack of fundamental understanding of oxide surfaces impedes rational catalyst design for improved activity and stability. We couple electrochemical studies of epitaxial La 1-x Sr x CoO 3-δ films with in situ and operando ambient pressure X-ray photoelectron spectroscopy to investigate the surface stoichiometry, adsorbates, and electronic structure. Additionally, in situ investigations spanning electrode compositions in a humid environment indicate that hydroxyl and carbonate affinity increase with Sr content, leading to an increase in binding energy of metal core levels and the valence band edge from the formation of a surface dipole. The maximum in hydroxylation at 40% Sr is commensurate with the highest OER activity, where activity scales with greater hole carrier concentration and mobility. Furthermore, operando measurements of the 20% Sr-doped oxide in alkaline electrolyte indicate that the surface stoichiometry remains constant during OER, supporting the idea that the oxide electrocatalyst is stable and behaves as a metal, with the voltage drop confined to the electrolyte. Furthermore, hydroxyl and carbonate species are present on the electrode surface even under oxidizing conditions, and may impact the availability of active sites or the binding strength of adsorbed intermediates via adsorbate–adsorbate interactions. For covalent oxides with facile charge transfer kinetics, the accumulation of hydroxyl species with oxidative potentials suggests the rate of reaction could be limited by proton transfer kinetics. This operando insight will help guide modeling of self-consistent oxide electrocatalysts, and highlights the potential importance of carbonates in oxygen electrocatalysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Changes in extremely hot days under stabilized 1.5 and 2.0 °C global warming scenarios as simulated by the HAPPI multi-model ensemble

Abstract. The half a degree additional warming, prognosis and projected impacts (HAPPI) experimental protocol provides a multi-model database to compare the effects of stabilizing anthropogenic global warming of 1.5 °C over preindustrial levels to 2.0 °C over these levels. The HAPPI experiment is based upon large ensembles of global atmospheric models forced by sea surface temperature and sea ice concentrations plausible for these stabilization levels. This paper examines changes in extremes of high temperatures averaged over three consecutive days. Changes in this measure of extreme temperature are also compared to changes in hot season temperatures. We find that over land this measure of extreme high temperature increases from about 0.5 to 1.5 °C over present-day values in the 1.5 °C stabilization scenario, depending on location and model. We further find an additional 0.25 to 1.0 °C increase in extreme high temperatures over land in the 2.0 °C stabilization scenario. Results from the HAPPI models are consistent with similar results from the one available fully coupled climate model. However, a complicating factor in interpreting extreme temperature changes across the HAPPI models is their diversity of aerosol forcing changes.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1995

The role of haptic cues from rough and slippery surfaces in human postural control

Haptic information is critically important in complex sensory-motor tasks such as manipulating objects. Its comparable importance in spatial orientation is only beginning to be recognized. We have shown that postural sway in humans is significantly reduced by lightly touching a stable surface with a fingertip at contact force levels far below those physically necessary to stabilize the body. To investigate further the functional relationship between contact forces at the hand and postural equilibrium, we had subjects stand in the tandem Romberg stance while being allowed physically supportive (force contact) and non-physically supportive (touch contact) amounts of index fingertip force on surfaces with different frictional characteristics. Mean sway amplitude (MSA) was reduced by over 50% with both touch and force contact of the fingertip, compared to standing without fingertip contact. No differences in MSA were observed when touching rough or slippery surfaces. The amplitude of EMG activity in the peroneal muscles and the timing relationships between fingertip forces, body sway and EMG activity suggested that with touch contact of the finger or with force contact on a slippery surface long-loop "reflexes" involving postural muscles were stabilizing sway. With force contact of the fingertip on a rough surface, MSA reduction was achieved primarily through physical support of the body. This pattern of results indicates that light touch contact cues from the fingertip in conjunction with proprioceptive signals about arm configuration are providing information about body sway that can be used to reduce MSA through postural muscle activation.

NASA Discipline Neuroscience↗
DOE OSTI2022

Epitaxial Dirac Semimetal Vertical Heterostructures for Advanced Device Architectures

Exploiting the extraordinary transport and optical properties of 3D topological semimetals for device applications requires epitaxial integration with semiconductors to carefully control carrier transport, yet no studies have established heteroepitaxy on top of any topological semimetals to date. Here, a novel approach toward fabricating heterostructures is demonstrated by epitaxially incorporating the Dirac semimetal Cd 3 As 2 between Zn x Cd 1-x Te and CdTe layers via molecular beam epitaxy on GaAs (001) substrates. The approach utilizes the higher energy (001) surface of Cd 3 As 2 to stabilize 2D epitaxy of zinc blende semiconductors. To demonstrate the impact heterostructure formation offers to device performance, an all-epitaxial, barrier-type vertical photodetector is fabricated that accesses a different carrier separation mechanism than previously reported non-epitaxial junctions and consequently exhibits significantly reduced dark currents. Finally, the results highlight the important role that epitaxial integration can play in accessing advanced architectures for topological semimetal-based devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A Beehive Inspired Hydrogen Photocatalytic Device Integrating a Carbo–Benzene Triptych Material for Efficient Solar Photo–Reduction of Seawater

The dream to produce green, clean and sustainable hydrogen from earth-abundant and free resources such as seawater and sunlight is highly motivating because of the interest for desirable economical and societal applications in energy. However, it remains challenging to develop an efficient and unassisted photocatalytic device to split seawater molecules with just sunlight without any external bias. For the first time, a such novel hierarchical material has been developed, based on thin film technology that integrates TiO 2 semiconductor layers, embedded gold nanoparticles and a photosensitive carbo-benzene layer. The design of the triptych device placing the photocatalyst in be-to-be increases the photoactive surface area by a factor 2. Its stability (>120 successive hours of hydrogen production and >5 days in a day/night representative alternation) and efficiency (STH 0.06%) are measured in NaCl-salted water. Here, the chloride ions act as hole scavengers and induce an increase of pH increasing in turn the sun-driven hydrogen production rate.

42 ENGINEERING↗
DOE OSTI2017

Designing Efficient Catalysts through Bimetallic Architecture: Rh@Pt Nanocubes as a Case Study

Bimetallic nanocatalysts often have increased activities and stabilities over their monometallic counterparts due to surface strain effects and electron transfer between the two metals. We demonstrate that the performance of a nanocatalyst can be precisely manipulated in shape-controlled nanocrystals through a bimetallic core@shell architecture. This ability is achieved in a model core@shell Rh@Pt nanocube system through control of shell thickness. The enhanced performance with thin-shelled nanocrystals is correlated with the weakening of surface–adsorbate interactions. In these thin-shelled Rh@Pt nanocubes, the maximum current density achieved during formic acid oxidation was over 2 times greater than that achieved with similarly sized Pt nanocubes, with a decreased CO poisoning ratio as well. Finally, the strategy employed here should also enhance the performance of many other bimetallic nanomaterials composed of more cost-effective metals too.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Silver-Mediated Squaric Acid Reduction as a Facile, Ambient-temperature and Seedless Route to Tunable Bimetallic Au/Ag Nanostars and Nanosnowflakes

In this work, bimetallic Au/Ag nanoparticles were successfully synthesized using a facile and reproducible method involving rapid, room temperature mixing of aqueous solutions of HAuCl 4 and AgNO 3 in the presence of squaric acid as both the reducing agent and surface capping ligand. Variation in the initial Au:Ag molar ratio yielded a tunable anisotropic shape and affiliated surface plasmon resonance. The nanoparticles displayed excellent stability in water for at least 10 weeks and showed robust catalytic activity in the borohydride-assisted reduction of the model substrate 4-nitrophenol.

36 MATERIALS SCIENCE↗
DOE OSTI2019

On the Stability of Nanobubbles in Water

Conditions of stability of charged air nanobubbles in water are considered. Ranges of values of the charge and radius in which coalescence and division predominate are theoretically determined. The stability region is revealed in which the given processes are thermodynamically improbable. A comparison of the theory with the available experiment is performed. Based on the results of our analysis, it is concluded that the main stabilizing factor for nanosized particles is their surface charge.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Multiscale operando X-ray investigations provide insights into electro-chemo-mechanical behavior of lithium intercalation cathodes

The electrochemical performance and cycle life of lithium-ion batteries (LIBs) depend on the electrochemical, chemical, and mechanical behavior of electrodes and electrolytes. Despite extensive studies conducted previously, challenges exist to decouple these behaviors, capture the evolution of electro-chemo-mechanical behavior in realistic conditions, and correlate atomic-scale stress evolution to micro-scale bulk mechanical degradation. Here, we report multiscale operando techniques to investigate polydisperse battery electrodes by integrating volume-averaged quantitative synchrotron X-ray scattering with high-resolution transmission X-ray microscopy (TXM). The former provides us information spanning a wide spatial range, from Angstrom-level atomic structures to micrometer-level particle scales, while the latter provides time-resolved 2D images of the particles during cycling. The complementarity of the two operando techniques is demonstrated by an over-lithiation test of LiCoO 2 electrodes, where particles crack and eventually pulverize. Additionally, the techniques are applied to study LiCoO 2 cycling stability from 3.0 V to 4.5 V. Operando X-ray scattering result shows nanometer-scale features keep forming in LiCoO 2 electrodes during cycling, resulting in an increased projected area observed by the TXM experiment. The formation of such features is inhibited by a polymer coating on the electrode, leading to vastly improved cycling stability. The polymer coating alleviates LiCoO 2 surface deterioration, reduces side product generation, and inhibits LiCoO 2 particles volume expansion during the cycling test. These operando multimodal X-ray techniques presented herein thus offer a novel, multiscale diagnostic modality for studying existing and emerging battery materials, aiding the development of next-generation LIBs.

25 ENERGY STORAGE↗
DOE OSTI2021

Ultrathin platinum nanowire based electrodes for high-efficiency hydrogen generation in practical electrolyzer cells

Significant reduction of noble metal catalyst loading and simplification of electrode fabrication are urgently needed in order to lower the cost of proton exchange membrane electrolyzer cells (PEMECs) for large-scale hydrogen production. Herein, we report an integrated electrode design comprising in-situ grown platinum nanowires (PtNW) on ultrathin titanium liquid/gas diffusion layers (LGDLs) via a cost-effective and green chemical synthesis approach. The ultrathin integrated PtNW electrodes showed a low cell voltage of 1.643 V and high efficiency of 90.08% at 1000 mA cm -2 using about 15 times lower catalyst loadings than a conventional catalyst-coated membrane in PEMEC tests. Ex-situ electrochemical characterizations and microscale visualizations further reveal that PtNW electrodes display highly efficient hydrogen evolution reactions and excellent electrode durability due to high active surface area, favorable bubble detachment, and structural stability. This work provides new insights into catalyst layer design and facile ultrathin electrode fabrication for more compact and low-cost PEM electrolyzers, fuel cells and other systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Mechanistic understanding of support effect on the activity and selectivity of indium oxide catalysts for CO 2 hydrogenation

Herein we present a mechanistic study on the support effect (ZrO 2 and CeO 2 ) of In 2 O 3 catalysts in CO 2 hydrogenation by a combined experimental and computational approach. Kinetic experiments and surface characterization suggested that the activity of In 2 O 3 catalysts cannot be simply correlated with the abundance of surface oxygen vacancies (O v ) formed by either H 2 -reduction or thermal treatment, which has been frequently invoked in previous studies. The support effect should originate from the electronic interactions between In 2 O 3 and the support oxide, rather than geometric factors or the difference in the particle size of In 2 O 3 . Theoretical modelling revealed that surface O v facilitate the formation and stabilization of the formate (HCOO*) intermediate. While a carbonate-like structure is favored for CO 2 adsorption on CeO 2 -supported or unsupported In 2 O 3 catalysts, CO 2 tends to bind strongly in a bent configuration on the O v site at the In 2 O 3 -ZrO 2 interface. The distinct CO 2 adsorption structures on different supported In 2 O 3 catalysts may account for the different reaction energy profiles in the subsequent hydrogenation reactions, especially the rate-limiting step, i.e., hydrogenation of HCOO* to CH 2 O* and methoxy (CH 3 O*). The relatively higher methanol selectivity of In 2 O 3 catalyst supported on ZrO 2 with respect to that on CeO 2 are suggested to stem from the greater energy difference (Δ$E_a$) between the parallel hydrogenation and C-O bond cleavage of HCOO*, which leads to the formation of methanol and CO, respectively. We report this study underlines the important role of metal-oxide-interface in determining the catalytic behavior of oxide-supported In 2 O 3 catalysts in CO 2 conversion.

30 DIRECT ENERGY CONVERSION↗