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DOE OSTI2024

Oxide-Encapsulated Ruthenium Oxide Catalysts for Selective Oxygen Evolution in Unbuffered pH-Neutral Seawater

Direct seawater electrolysis is a promising approach to producing green hydrogen in water-scarce environments using renewable energy. However, the undesirable chlorine evolution reaction and hypochlorite evolution reaction compete with the desired oxygen evolution reaction (OER) at the anode electrocatalyst. This issue is most pronounced in unbuffered pH-neutral solutions due to local acidification resulting from the OER. To overcome this challenge, this study provides a comprehensive evaluation of the use of silicon oxide (SiO x ) and titanium oxide (TiO x ) nanoscale overlayers coated on metallic ruthenium (Ru) and ruthenium oxide (RuO x ) thin film electrodes and their ability to block chloride ions from reaching active sites during operation in an unbuffered 0.6 M NaCl electrolyte. Using a combination of (electro)analytical techniques, encapsulated RuO x anodes are shown to effectively suppress Cl - transport to buried catalyst active sites while allowing for the desired OER to occur, leading to increases in OER faradaic efficiency at moderate overpotentials. Evidence for the ability of SiO x overlayers to block Cl - ions from reaching the active buried interface was obtained by monitoring the ν(O-H) stretching mode of OH adsorbates using in situ Raman spectroscopy. Here, this study also reports trade-offs between the activity, selectivity, and stability of bare and encapsulated Ru and RuO x electrocatalysts, finding that the magnitude of these trade-offs strongly depends on the complex interplay between electrode architecture, material properties, and catalytic performance, especially in unbuffered pH-neutral seawater.

58 GEOSCIENCES↗

NASA NTRS2008

NASA Tech Briefs, November 2008

Topics covered include: Digital Phase Meter for a Laser Heterodyne Interferometer; Vision System Measures Motions of Robot and External Objects; Advanced Precipitation Radar Antenna to Measure Rainfall From Space; Wide-Band Radar for Measuring Thickness of Sea Ice; Vertical Isolation for Photodiodes in CMOS Imagers; Wide-Band Microwave Receivers Using Photonic Processing; L-Band Transmit/Receive Module for Phase-Stable Array Antennas; Microwave Power Combiner/Switch Utilizing a Faraday Rotator; Compact Low-Loss Planar Magic-T; Using Pipelined XNOR Logic to Reduce SEU Risks in State Machines; Quasi-Optical Transmission Line for 94-GHz Radar; Next Generation Flight Controller Trainer System; Converting from DDOR SASF to APF; Converting from CVF to AAF; Documenting AUTOGEN and APGEN Model Files; Sequence History Update Tool; Extraction and Analysis of Display Data; MRO DKF Post-Processing Tool; Rig Diagnostic Tools; MRO Sequence Checking Tool; Science Activity Planner for the MER Mission; UAVSAR Flight-Planning System; Templates for Deposition of Microscopic Pointed Structures; Adjustable Membrane Mirrors Incorporating G-Elastomers; Hall-Effect Thruster Utilizing Bismuth as Propellant; High-Temperature Crystal-Growth Cartridge Tubes Made by VPS; Quench Crucibles Reinforced with Metal; Deep-Sea Hydrothermal-Vent Sampler; Mars Rocket Propulsion System; Two-Stage Passive Vibration Isolator; Improved Thermal Design of a Compression Mold; Enhanced Pseudo-Waypoint Guidance for Spacecraft Maneuvers; Altimetry Using GPS-Reflection/Occultation Interferometry; Thermally Driven Josephson Effect; Perturbation Effects on a Supercritical C7H16/N2 Mixing Layer; Gold Nanoparticle Labels Amplify Ellipsometric Signals; Phase Matching of Diverse Modes in a WGM Resonator; WGM Resonators for Terahertz-to-Optical Frequency Conversion; Determining Concentration of Nanoparticles from Ellipsometry; Microwave-to-Optical Conversion in WGM Resonators; Four-Pass Coupler for Laser-Diode-Pumped Solid-State Laser; Low-Resolution Raman-Spectroscopy Combustion Thermometry; Temperature Sensors Based on WGM Optical Resonators; Varying the Divergence of Multiple Parallel Laser Beams; Efficient Algorithm for Rectangular Spiral Search; Algorithm-Based Fault Tolerance Integrated with Replication; Targeting and Localization for Mars Rover Operations; Terrain-Adaptive Navigation Architecture; Self-Adjusting Hash Tables for Embedded Flight Applications; Schema for Spacecraft-Command Dictionary; Combined GMSK Communications and PN Ranging; System-Level Integration of Mass Memory; Network-Attached Solid-State Recorder Architecture; Method of Cross-Linking Aerogels Using a One-Pot Reaction Scheme; An Efficient Reachability Analysis Algorithm.

Source record↗

NASA NTRS2012

Aqueously Dispersed Silver Nanoparticle-Decorated Boron Nitride Nanosheets for Reusable, Thermal Oxidation-Resistant Surface Enhanced Raman Spectroscopy (SERS) Devices

The impurity-free aqueous dispersions of boron nitride nanosheets (BNNS) allowed the facile preparation of silver (Ag) nanoparticle-decorated BNNS by chemical reduction of an Ag salt with hydrazine in the presence of BNNS. The resultant Ag-BNNS nanohybrids remained dispersed in water, allowing convenient subsequent solution processing. By using substrate transfer techniques, Ag-BNNS nanohybrid thin film coatings on quartz substrates were prepared and evaluated as reusable surface enhanced Raman spectroscopy (SERS) sensors that were robust against repeated solvent washing. In addition, because of the unique thermal oxidation-resistant properties of the BNNS, the sensor devices may be readily recycled by short-duration high temperature air oxidation to remove residual analyte molecules in repeated runs. The limiting factor associated with the thermal oxidation recycling process was the Ostwald ripening effect of Ag nanostructures.

Lin, Yi↗

DOE OSTI2024

Deep-Learning-derived Boundary Layer Height from Meteorological Data over the SGP, GOAMAZON, CACTI

The planetary boundary-layer (PBL) height (PBLH) is an important parameter for various meteorological and climate studies. This study presents a multi-structure deep neural network (DNN) model, designed to estimate PBLH by integrating morning temperature profiles with surface meteorological observations. The DNN model is developed by leveraging a rich data set of PBLH derived from long-standing radiosonde records and augmented with high-resolution micropulse lidar and Doppler lidar observations. We access the performance of the DNN with an ensemble of 10 members, each featuring distinct hidden layer structures, which collectively yield a robust 27-year PBLH data set over the Southern Great Plains from 1994 to 2020. The influence of various meteorological factors on PBLH is rigorously analyzed through the importance test. Moreover, the DNN model's accuracy is evaluated against radiosonde observations and juxtaposed with conventional remote-sensing methodologies, including Doppler lidar, ceilometer, Raman lidar, and micropulse lidar. The DNN model exhibits reliable performance across diverse conditions and demonstrates lower biases relative to remote-sensing methods. In addition, the DNN model, originally trained over a plain region, demonstrates remarkable adaptability when applied to the heterogeneous terrains and climates encountered during the GoAmazon (tropical rainforest) and CACTI (middle-latitude mountain) campaigns. These findings demonstrate the effectiveness of deep learning models in estimating PBLH, enhancing our understanding of boundary-layer dynamics with implications for enhancing the representation of PBL in weather forecasting and climate modeling.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS2007

Retrievals with the Infrared Atmospheric Sounding Interferometer

The Infrared Atmospheric Sounding Interferometer (IASI) on the MetOp satellite was launched on October 19, 2006. The Joint Airborne IASI Validation Experiment (JAIVEx) was conducted during April 2007 mainly for validation of the IASI on the MetOp satellite. IASI possesses an ultra-spectral resolution of 0.25/cm and a spectral coverage from 645 to 2760/cm. Ultraspectral resolution infrared spectral radiance obtained from near nadir observations provide atmospheric, surface, and cloud property information. An advanced retrieval algorithm with a fast radiative transfer model, including cloud effects, is used for atmospheric profile and cloud parameter retrieval. Preliminary retrievals of atmospheric soundings, surface properties, and cloud optical/microphysical properties with the IASI observations during the JAIVEx are obtained and presented. These retrievals are further inter-compared with those obtained from airborne FTS system, such as the NPOESS Airborne Sounder Testbed Interferometer (NAST-I), dedicated dropsondes, radiosondes, and ground based Raman Lidar. The capabilities of satellite ultra-spectral sounder such as the IASI are investigated.

Zhou, Daniel K.↗

NASA NTRS2011

A New SBUV Ozone Profile Time Series

Under NASA's MEaSUREs program for creating long term multi-instrument data sets, our group at Goddard has re-processed ozone profile data from a series of SBUV instruments. We have processed data from the Nimbus 7 SBUV instrument (1979-1990) and data from SBUV/2 instruments on NOAA-9 (1985-1998), NOAA-11 (1989-1995), NOAA-16 (2001-2010), NOAA-17 (2002-2010), and NOAA-18 (2005-2010). This reprocessing uses the version 8 ozone profile algorithm but now uses the Brion, Daumont, and Malicet (BMD) ozone cross sections instead of the Bass and Paur cross sections. The new cross sections have much better resolution, and extended wavelength range, and a more consistent temperature dependence. The re-processing also uses an improved cloud height climatology based on the Raman cloud retrievals of OMI. Finally, the instrument-to-instrument calibration is set using matched scenes so that ozone diurnal variation in the upper stratosphere does not alias into the ozone trands. Where there is no instrument overlap, SAGE and MLS are used to estimate calibration offsets. Preliminary analysis shows a more coherent time series as a function of altitude. The net effect on profile total column ozone is on average an absolute reduction of about one percent. Comparisons with ground-based systems are significantly better at high latitudes.

McPeters, Richard↗

NASA NTRS2008

Absorption in Extended Inhomogeneous Clouds

The launch of several different sensors, including CloudSat, into the A-train constellation of satellites allows us for the first time to compute absorption that can occur in realistic vertically inhomogeneous clouds including multiple cloud decks. CloudSat data show that these situations are common. Therefore, understanding vertically inhomogeneous clouds is important from both climate and satellite atmospheric composition remote sensing perspectives. Satellite passive sensors that operate from the near IR to the UV often rely on radiative cloud pressures derived from absorption in oxygen bands (A, B, gamma, or O2-O2 bands) or from rotational-Raman scattering in order to retrieve information about atmospheric trace gases. The radiative cloud pressure is distinct from the physical cloud top derived from thermal infrared measurements. Therefore, the combination of information from different passive sensors yields some information about the cloud vertical profile. When either or both the clouds or atmospheric absorbers (trace gases and aerosols) are vertically inhomogeneous, the use of an effective cloud pressure derived from these approaches may lead to errors. Here, we focus on several scenarios (deep convective clouds and distinct two layer clouds) based on realistic cloud optical depth vertical profiles derived from the CloudSatfMODIS combination. We focus on implications for trace-gas column amount retrievals (specifically ozone and NO2) and derived surface UV irradiance from the Ozone Monitoring Instrument (OMI) on the Atrain Aura platform.

Joiner, Joanna↗

NASA NTRS2002

Parametric Study of Carbon Nanotube Production by Laser Ablation Process

Carbon nanotubes form a new class of nanomaterials that are presumed to have extraordinary mechanical, electrical and thermal properties. The single wall nanotubes (SWNTs) are estimated to be 100 times stronger than steel with 1/6th the weight; electrical carrying capacity better than copper and thermal conductivity better than diamond. Applications of these SWNTs include possible weight reduction of aerospace structures, multifunctional materials, nanosensors and nanoelectronics. Double pulsed laser vaporization process produces SWNTs with the highest percentage of nanotubes in the output material. The normal operating conditions include a green laser pulse closely followed by an infrared laser pulse. Lasers ab late a metal-containing graphite target located in a flow tube maintained in an oven at 1473K with argon flow of 100 sccm at a 500 Torr pressure. In the present work a number of production runs were carried out, changing one operating condition at a time. We have studied the effects of nine parameters, including the sequencing of the laser pulses, pulse separation times, laser energy densities, the type of buffer gas used, oven temperature, operating pressure, flow rate and inner flow tube diameters. All runs were done using the same graphite target. The collected nanotube material was characterized by a variety of analytical techniques including scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman and thermo gravimetric analysis (TGA). Results indicate trends that could be used to optimize the process and increase the efficiency of the production process.

Arepalli, Sivaram↗

NASA NTRS2002

An Experimental Study of Nonlinear Standing Waves in Resonators with Numerical Comparison

Lawrenson et. al. [Journal of the Acoustic Society of America, Nov. 1998] described the generation of shock-free high-amplitude pressure waves in closed cavities using large equipment and resonators to produce the reported effects. An attempt is made to generate shock-free high-amplitude pressure waves using relatively small resonators. Ambient air is used as the working fluid. A small cylindrical resonator is tested resulting in the lack of a shocked waveform while a larger model of the same shape produces shock waves. A small conical resonator produces shock-free pressure waves at resonance, but the amplitude of these waves is small. A larger cone resonator model produces shock-free pressure waves of higher amplitude. A large horn-cone resonator also produces shock-free high amplitude pressure waves, A numerical model is used to compare the experimental results to theoretical results. The effects of structural resonances on the production of shock-free high-amplitude pressure waves are discussed, especially concerning difficulties encountered when these resonances were in the frequency ranges of interest. Identifying features of a structural resonance are presented.

Finkbeiner, Joshua R.↗

DOE OSTI2025

Chemical Vapor Deposition-Grown Hexagonal Boron Nitride and Graphene for Tandem Dielectric Capacitive Polymer Devices

To address the low energy density of polymeric capacitors, this work explores how tandem combinations of antagonistic properties can enhance energy storage. We introduce multilayer architecture integrating chemical vapor deposition (CVD)-grown ≈2 nm hexagonal boron nitride (hBN) and graphene with ferroelectric polyvinylidene fluoride (PVDF) and linear polyetherimide (PEI) layers to suppress leakage paths, reduce loss, and promote Maxwell–Wagner–Sillars polarization. Raman spectroscopy, X-ray diffraction (XRD), atomic force microscopy (AFM), scanning electron microscopy (SEM), and plasma focused ion beam (PFIB) analyses confirm robust material integration. In conclusion, for the tandem device, E BD ≈600 V/μm, while individual layers show lower values (PVDF|Graphene (Gr)|PVDF ≈ 50 V/μm and PEI|hBN|PEI ≈ 275 V/μm), yielding an overall ≈6000% enhancement and demonstrating the effectiveness of the 2D multilayer design.

Chemical vapor deposition (CVD)↗

DOE OSTI2024

Synergistic Effects of the Electric Field Induced by Imidazolium Rotation and Hydrogen Bonding in Electrocatalysis of CO 2

The roles of the ionic liquid, 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM][BF₄]), and water in controlling the mechanism, energetics, and electrocatalytic activity of CO₂ reduction to CO on silver in non-aqueous electrolytes were investigated. The first electron transfer occurs to CO₂ at reduced overpotentials when it is trapped between the planes of [EMIM]⁺ ring and electrode surface due to cation re-orientation as determined from voltammetry, in-situ surface-enhanced Raman spectroscopy, and density functional theory calculations. Within this interface, water up to 0.5 M does not induce significant faradaic activity, opposing the notion of it as a free proton source. Instead, water acts as a hydrogen bond donor and the proton is sourced from [EMIM]⁺. Furthermore, this study demonstrates that alcohols with varying acidity tune the hydrogen bonding network in the interfacial microenvironment to lower the energetics required for CO₂ reduction. Here, the hydrogen bonding suppresses the formation of inactive carboxylate species, thus preserving the catalytic activity of [EMIM]⁺. The ability to tune the hydrogen bonding network opens new avenues for advancing IL-mediated electrocatalytic reactions in non-aqueous electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Correlating surface adsorbate configuration and electrochemical performance of IrO 2 during seawater-relevant electrolysis

Seawater electrolysis alleviates freshwater demand to produce clean hydrogen while eliminating the need for water purification steps. The anodic process, seawater oxidation, typically requires high overpotentials and yields low selectivity to oxygen via the oxygen evolution reaction (OER), primarily due to the competing chlorine evolution reaction (CER) and hypochlorite evolution reaction (HCER) in pH-neutral conditions. Here, combining in situ surface-enhanced Raman characterization, grand canonical density functional theory-based calculations, and kinetic Monte Carlo simulations, we report the evolution of surface adsorbate configurations driven by applied potential and pH during seawater-relevant OER over IrO 2 , a highly OER-active and chloride-corrosion-resistant catalyst. As a result, the chemical properties of active sites, and thereby the kinetics of OER and CER/HCER, are effectively tuned. However, it is revealed that there is no optimal combination of potential and pH to achieve both high activity and high selectivity for seawater-relevant OER. To address this limitation, we establish a correlation between activity/selectivity and surface adsorbate configurations, enabling the optimization of highly active and OER-selective IrO 2 -based catalysts in seawater-relevant oxidation by modulating the local adsorbate environment of active sites.

08 HYDROGEN↗

DOE OSTI2024

Structural properties of plastically deformed SrTiO 3 and KTaO 3

Dislocation engineering has the potential to open new avenues toward the exploration and modification of the properties of quantum materials. Strontium titanate (SrTi⁢O 3 , STO) and potassium tantalate (KTa⁢O 3 , KTO) are incipient ferroelectrics that show metallization and superconductivity at extremely low charge-carrier concentrations and have been the subject of resurgent interest. These materials also exhibit remarkable ambient-temperature ductility, and thus represent exceptional platforms for studies of the effects of deformation-induced dislocation structures on electronic properties. Recent work on plastically deformed STO revealed an enhancement of the superconducting transition temperature and the emergence of local ferroelectricity and magnetism near self-organized dislocation walls. Here, in this work, we present a comprehensive structural analysis of plastically deformed STO and KTO, employing specially designed strain cells, diffuse neutron and x-ray scattering, Raman scattering, and nuclear magnetic resonance (NMR). Diffuse scattering and NMR provide insight into the dislocation configurations and densities and their dependence on strain. As in the prior work on STO, Raman scattering reveals evidence for local ferroelectric order near dislocation walls in plastically deformed KTO. Our findings provide valuable information about the self-organized defect structures in both materials, and they position KTO as a second model system in which to explore the associated emergent physics.

36 MATERIALS SCIENCE↗

NASA NTRS1989

Subharmonic and fundamental high amplitude excitation of an axisymmetric jet

The effect of simultaneous excitation at the fundamental and subharmonic frequencies on the behavior of a circular jet shear layer is studied. Attention is given to the effect of the initial phase difference, the Strouhal number pair, and amplitudes of the fundamental and subharmonic tones. High-amplitude excitation devices which can provide a wide range of forcing conditions when used in conjunction with equipment that produces complex waveforms are used.

Raman, Ganesh↗

NASA NTRS2003

Preparation and Characterization of Space Durable Polymer Nanocomposite Films from Functionalized Carbon Nanotubes

Low color, flexible, space durable polyimide films with inherent, robust electrical conductivity have been under investigation as part of a continuing materials development activity for future NASA space missions involving Gossamer structures. Electrical conductivity is needed in these films to dissipate electrostatic charge build-up that occurs due to the orbital environment. One method of imparting conductivity is through the use of single walled carbon nanotubes (SWNTs). However, the incompatibility and insolubility of the SWNTs severely hampers their dispersion in polymeric matrices. In an attempt to improve their dispersability, SWNTs were functionalized by the reaction with an alkyl hydrazone. After this functionalization, the SWNTs were soluble in select solvents and dispersed more readily in the polymer matrix. The functionalized SWNTs were characterized by Raman spectroscopy and thermogravimetric analysis (TGA). The functionalized nanotubes were dispersed in the bulk of the films using a solution technique. The functionalized nanotubes were also applied to the surface of polyimide films using a spray coating technique. The resultant polyimide nanocomposite films were evaluated for nanotube dispersion, electrical conductivity, mechanical, and optical properties and compared with previously prepared polyimide-SWNT samples to assess the effects of SWNT functionalization.

Delozier, D. M.↗

NASA NTRS1975

A theoretical/experimental program to develop active optical pollution sensors: Quantitative remote Raman lidar measurements of pollutants from stationary sources

Typical pollutant gas concentrations at the stack exits of stationary sources can be estimated to be about 500 ppm under the present emission standards. Raman lidar has a number of advantages which makes it a valuable tool for remote measurements of these stack emissions. Tests of the Langley Research Center Raman lidar at a calibration tank indicate that night measurements of SO2 concentrations and stack opacity are possible. Accuracies of 10 percent are shown to be achievable from a distance of 300 m within 30 min integration times for 500 ppm SO2 at the stack exits. All possible interferences were examined quantitatively (except for the fluorescence of aerosols in actual stack emissions) and found to have negligible effect on the measurements. An early test at an instrumented stack is strongly recommended.

Poultney, S. K.↗

NASA NTRS1976

The Raman spectra of N-14O2 and N-15O2 solids at 20 K

The Raman spectra of N-14O2 and N-15O2 have been studied at 20 K. The far infrared of N-14O2 at 20 K was also measured. The data were assigned on the basis of a C-sub 2 nu molecular model. Normal coordinate calculations were performed for a variety of assignments. The assignment that yielded the best fit is presented. The solid state effects are discussed.

Durig, J. R.↗

NASA NTRS2016

OH PLIF Visualization of a Premixed Ethylene-fueled Dual-Mode Scramjet Combustor

Hydroxyl radical (OH) planar induced laser fluorescence (PLIF) measurements have been performed in a small-scale scramjet combustor at the University of Virginia Aerospace Research Laboratory at nominal simulated Mach 5 enthalpy. OH lines were carefully chosen to have fluorescent signal that is independent of pressure and temperature but linear with mole fraction. The OH PLIF signal was imaged in planes orthogonal to and parallel to the freestream flow at different equivalence ratios. Flameout limits were tested and identified. Instantaneous planar images were recorded and analyzed to compare the results with width increased dual-pump enhanced coherent anti-Stokes Raman spectroscopy (WIDECARS) measurements in the same facility and large eddy simulation/Reynolds average Navier-Stokes (LES/RANS) numerical simulation. The flame angle was found to be approximately 10 degrees for several different conditions, which is in agreement with numerical predictions and measurements using WIDECARS. Finally, a comparison between NO PLIF non-combustion cases and OH PLIF combustion cases is provided: the comparison reveals that the dominant effect of flame propagation is freestream turbulence rather than heat release and concentration gradients.

Cantu, Luca M. L.↗