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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 361 records · Page 20

Mechanistic aspects of plasma-enhanced catalytic methane decomposition by time-resolved operando diffuse reflectance infrared Fourier transform spectroscopy

To study mechanistic aspects of plasma-enhanced catalysis, methane is decomposed by a supported Ni catalyst assisted by an Ar/O 2 atmospheric pressure plasma jet (APPJ). Here, the time-resolved surface response of the Ni catalyst is investigated by operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) using various experimental settings. Catalyst temperatures of room temperature (RT) and 500 °C and nozzle-catalyst surface distances of 3, 5 and 8 mm were examined, and the amount of O 2 of the Ar/O 2 gas mixture flowing through the APPJ was either 0 or 0.5%. A synergistic effect of surface bonded C-O was observed during the exposure of the Ni catalyst to the APPJ for low oxygen operating conditions (pure Ar jet). Surface bonded C-O formed only when there was plasma present and the C-O signal was enhanced for higher catalyst temperature. When the supported Ni catalyst was subjected to the plasma-generated particle fluxes using highly oxidizing conditions, the presence of surface bonded C-O was suppressed. The plasma-catalytic CO and CO 2 production in the gas phase measured downstream mirrored the surface behavior of C-O bonds when the plasma source operating condition was changed from a low oxygen portion to a high oxygen portion at high catalyst temperature (500 °C). CH n (n =1, 2, ) species on the catalyst surface were also studied by DRIFTS, and CHn destruction was found to correlate with C-O formation. In particular, the time-resolved CH n response showed a possible conversion process of CH n to C-O when the Ni catalyst was exposed to the plasma source. This finding may indicate a plasma-mediated regeneration of the catalyst by plasma-catalyst surface interactions.

42 ENGINEERING↗

Investigation of the Effect of Injected CO 2 on the Morrow B Sandstone through Laboratory Batch Reaction Experiments: Implications for CO 2 Sequestration in the Farnsworth Unit, Northern Texas, USA

About one million tons of CO 2 have been injected into the Farnsworth unit to date. The target reservoir for CO 2 injection is the Morrow B Sandstone, which is primarily made of quartz with lesser amounts of albite, calcite, chlorite, and clay minerals. The impact of CO 2 injection on the mineralogy, porosity, and pore water composition of the Morrow B Sandstone is a major concern. Although numerical modeling studies suggest that porosity changes will be minimal, significant alterations to mineralogy and pore water composition are expected. Given the implications for CO 2 storage effectiveness and risk assessment, it is crucial to verify the accuracy of theoretical model predictions through laboratory experiments. To this end, batch reaction experiments were conducted to model conditions near an injection well in the Morrow B Sandstone and at locations further away, where the CO 2 has been diluted by formation water. The laboratory experiments involved submerging thin sections of both coarse- and fine-grained facies of the Morrow B Sandstone in formation water samples with varying levels of CO 2 . The experiments were conducted at the reservoir temperature of 75 °C. Two experimental runs were conducted, one lasting for 61 days and the other for 72 days. The initial fluid composition used in the second run was the same as in the first. The mineralogy changes in the thin sections were analyzed using SEM and the Tescan Integrated Mineral Analyzer (TIMA), while changes in the composition of the formation water were determined using ICP-AES. During each experiment, a thin layer of white fine-grained particles consisting mainly of dolomite and silica formed on the surface of the thin sections, leading to significant reductions in Ca, Mg, and Sr in the formation water. This outcome is consistent with numerical model predictions that dolomite would be the primary mineral that would react with injected CO 2 and that silica would be oversaturated in the formation water. Changes in mineral abundance in the thin sections themselves were much less systematic than in the theoretical modeling experiments, perhaps reflecting heterogeneities in the mineral grain size surface area to volume ratios and mineral distributions in the thin sections not considered in the numerical models.

58 GEOSCIENCES↗

Snow ALbedo eVOlution (SALVO) Campaign Broadband Albedo from April - June, 2024 in Utqiagivk, AK level a1

A field-portable broadband (285 – 2800 nm) albedometer was used to make spatially distributed albedo measurements on tundra and sea ice surfaces. The albedometer consists of paired upward-looking and downward-looking pyranometers, which were both connected to a data logger. The instrument was mounted approximately 1 m above the surface using a tripod and was placed on a 1.4 m-long boom to minimize the impacts of shading from the operator and to observe surfaces undisturbed by footprints (see Appendix for photos of measurement setup and uncertainty assessment). Albedo measurements were taken parallel to the 200-m albedo lines at 5-m increments (41 measurements) ~1.2 m south of the line. On the operator’s end of the boom, there was a bubble level that was aligned with the bubble level on the upward-looking pyranometer. To take a measurement, the operator first relocated the tripod to the measurement location, then leveled the instrument and held it level for at least twice the pyranometers’ response time (5 or 15 seconds, see below), and finally depressed a trigger on the data logger. The data logger recorded the instantaneous voltage on both pyranometers, the measurement number, and the time. The data logger also converted the voltages to irradiances, and from these computed the ratio (outgoing/incoming) for albedo, which could be checked in the field. The operator recorded in a field notebook the measurement number that corresponded with the locations on the line and any pertinent notes (e.g., invalid measurements). With this setup, a trained operator could measure a 200-m albedo line (41 measurements) in approximately 30 minutes. Measurements were made within 3 hours of solar noon. The data logger had sufficient storage capacity to record all measurements from the campaign, but data were downloaded to a computer after each measurement day.

54 ENVIRONMENTAL SCIENCES↗

Investigation of coverage dependence of the stretching frequency of CO adsorbed on Pd surfaces at low coverage limits

The stretching frequency of the C—O bond is a sensitive probe of the local environment of a surface-bound CO molecule, including the adorption site and density, i.e. surface coverage. In this work, we extend our analysis beyond the frequency shift due to differences in adsorption configurations. Using density functional theory (DFT) calculations, we directly explore the correlations between surface coverage and the stretching frequency of adsorbed CO on Pd surfaces. Here we also perform constant pressure infrared reflection absorption measurements of CO on Pd(111) and use existing relations between pressure and coverage to derive coverage dependency. Both results are compared to previously reported experimental data. Our derived correlations of peak frequency and area with surface coverage can help interpret experimental IR spectra in real time and extract time-dependent concentration data from transient kinetic experiments.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Elucidating Trivalent Ion Adsorption at Floating Carboxylic Acid Monolayers: Charge Reversal or Water Reorganization?

Here we study the adsorption of trivalent neodymium on floating arachidic acid films at the air–water interface by two complementary surface specific probes, sum frequency generation spectroscopy and X-ray fluorescence near total reflection. In the absence of background ions, neodymium ions compensate for the surface charge of the arachidic acid film at a bulk concentration of 50 μM without any charge reversal. Increasing the bulk concentration to 1 mM does not change the neodymium surface coverage but affects the interfacial water structure significantly. In the presence of a high concentration of NaCl, there is overcharging at 1 mM Nd 3+ , i.e., 30% more Nd 3+ than needed to compensate for the surface charge. These results show that the total coverage of neodymium ions is not enough to describe the complete picture at the interface, and interfacial water and ion coverage needs to be considered together to understand more complex ion adsorption and transport processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Effect of Cholesterol on Membrane Binding and Self-Assembly of Collagen Fibrils

Collagen is a skeleton of native extracellular matrix (ECM) that is known to provide mechanical and structural stability. In an attempt to develop a new connective cellular model with the surrounding ECM without further experimental complications, such as the reconstitution of ECM receptors, we designed the experiments and discovered that the fibrillogenesis of membrane-bound collagen is not spontaneous as it is in the form of free collagen in bulk solution. Furthermore, the confocal microscopic results suggest that cholesterol is a crucial component that facilitates the fibril formation on the membrane surface. In situ X-ray and neutron reflectivity on Langmuir monolayer and solid-supported lipid bilayer models, respectively, reveal two features of cholesterol effects on the collagen fibril formation. Mainly, cholesterol increases the lateral lipid headgroup separation on the membrane surface, which promotes the association degree of collagen monomers. It also enhances the elastic modulus of the membrane to impede membrane filtration by the collagen assemblies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Multispectral and thermal surface imagery and surface elevation mosaics - Pendleton Feb 2023

This data set contains high-resolution image products (orthomosaics) acquired from midsized uncrewed aerial systems that have been processed for value-added quality. The instrument Altum multispectral imager by Micasense, captures in six bands (blue - 475nm, green - 560nm, red - 668nm, red edge - 717nm, near-infrared - 840 and LWIR/thermal - 11000nm. The optical bands are converted to reflectance via custom code using the instantaneous band horizontal irradiance ratio to the radiance of the pixel. The code used to develop these images first uses tools from the Micasense Python library to apply dark level corrections, row gradient corrections, and radiometric corrections. Next, it uses the processing API from Agisoft Metashape software to align and mosaic the processed imagery, following the processes developed by the USGS' structure from motion workflow documentation. Captures from different altitudes are used to produce an orthomosaic at each height. A tif image containing information related to the six spectral bands, and a digital elevation model (DEM), a tif image containing information related to the elevation of the surveyed terrain. 1 https://www.arm.gov/publications/tech_reports/handbooks/doe-sc-arm-tr-281.pdf 2 https://micasense.github.io/imageprocessing/MicaSense%20Image%20Processing%20Setup.html 3 https://pubs.usgs.gov/of/2021/1039/ofr20211039.pdf

54 ENVIRONMENTAL SCIENCES↗

Custom NEON AOP reflectance mosaics and maps of shade masks, canopy water content

This mosaic of visible to shortwave infrared (VSWIR) data was derived from the assignable asset NEON AOP radiance data that was collected by LBNL’s Watershed Function SFA during the summer of 2018 (DOI: 10.15485/1617204). This atmospheric correction was completed to take into account site-specific terrain variability in the 334 km2 survey area centered around Crested Butte, CO. The atmospheric correction was completed using ACORN atmospheric correction software executed on 200 x 200 pixel kernels rather than line by line in order to capture local flight altitude conditions. Manual cloud delineation removed any small shaded areas that occurred within the data collection areas. Mosaics were developed based on preference for days that were in close timing proximity to the coincident ground campaign and with mosaicing criteria that minimized the angle between the sun and the sensor to retrieve the most consistent reflectance (min_phase_refl_tiled). Finally, we generated shade masks based on the geometry between the sun angle at time of flight, the ground surface, and the sensor. Here we provide the orthomosaiced estimated reflectance data (min_phase_refl_tiled.tif), canopy water content (wtrl), estimated atmospheric water vapor (wtrv), the observational data (obs) for this particular mosaic, the estimated visibility (vis), shade masks derived from the digital surface elevation model (shade) and the digital terrain model (shade_tch) added to the canopy height model (DOI: 10.15485/1617203), and a wavelength metadata file. Each image file is provided as a GeoTiff with internal tiling and LZW compression. These data can also be found on Google Earth Engine for extraction, download, and analysis of smaller extents (Google Earth Engine data is linked in external link table).

2018 NEON and 2025 CHESS Campaigns↗

Radiological Monitoring Plan for the Oak Ridge Y-12 National Security Complex: Surface Water

DOE Order 458.1 requires that dose estimates consider contributions from all facilities. In the Y-12 Radiological Monitoring Plan (RMP), surface water is monitored at points that reflect individual facilities, as well as at points that reflect the combined contributions of all facilities. This monitoring plan does not consider other potential routes (i.e., airborne releases and food chains). Thus, a complete determination of total effective dose (TED) cannot be made based on this plan alone. The other routes from Y-12, and all routes from other DOE facilities on the Oak Ridge Reservation (e.g., Oak Ridge National Laboratory (ORNL) and The Heritage Center), must be considered in order to satisfy DOE Order 458.1 requirements. Determination of TED from all sites and pathways is done through the use of dose-assessment models and is documented in the Annual Site Environmental Report. This monitoring plan provides adequate monitoring goals for Y-12 surface water releases to provide input of sufficient sensitivity and accuracy to reliably determine the Y-12 surface water component of the TED. The routine radiological monitoring program is designed to monitor effluents at four types of locations: (1) treatment facilities, (2) other point and area source discharges, (3) instream locations, and (4) production building roof run-off. With this sampling and analysis program, data will be obtained on primary point sources as well as on locations that represent the composite of other potential sources. This plan will be reviewed periodically to determine necessary modifications to the sampling frequencies, parameters, and locations. Modifications, if any, will be based on the analysis of the previous data and its effectiveness in satisfying the objectives of this plan. Appendix A contains graphs of the sum of the DCS fractions for locations and frequencies contained in a previous version of this plan. The data was collected from January 2009 through December 2019. Each sample was analyzed, and each result was divided by the appropriate DCS to compute a DCS fraction. These fractions were summed for all isotopes. According to DOE –STD-1196-2011, the annual average of these sums should be below 1.

54 ENVIRONMENTAL SCIENCES↗

Reflectance of Silicon Photomultipliers at Vacuum Ultraviolet Wavelengths

Characterization of the vacuum ultraviolet (VUV) reflectance of silicon photomultipliers (SiPMs) is important for large-scale SiPM-based photodetector systems. In this work, we report the angular dependence of the specular reflectance in vacuum of SiPMs manufactured by Fondazionc Bruno Kessler (FBK) and Hamamatsu Photonics K.K. (HPK) over wavelengths ranging from 120 to 280 nm. Refractive index and extinction coefficient of the thin silicon-dioxide film deposited on the surface of the FBK SiPMs are derived from reflectance data of an FBK silicon wafer with the same deposited oxide film as SiPMs. The diffuse reflectance of SiPMs is also measured at 193 nm. We use the VUV spectral dependence of the optical constants to predict the reflectance of the FBK silicon wafer and FBK SiPMs in liquid xenon.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Patterned dielectric back contact design for GaAs thermophotovoltaic devices

-Patterned-dielectric back contact structures in optoelectronic devices are designed to boost the reflectance of light from the device back surface while retaining a low-resistance pathway for electrical conductance. Their reduced light absorption at near- and sub-bandgap photon energies leads to improved luminescence in light-emitting diodes, greater photon recycling, voltage, and efficiency in photovoltaic cells, and greater recuperation of unabsorbed sub-bandgap light in thermophotovoltaic (TPV) systems. However, diffraction from the patterned features can deflect incident light in propagation directions that lead to light trapping and parasitic absorption in the cell. Here, in this article, we use rigorous coupled-wave analysis (RCWA) to study three-dimensional diffractive scattering of electromagnetic waves by periodic metal point-contact gratings on 1.42-eV GaAs TPV cells, to analyze their effect on unwanted sub-bandgap absorption in order to achieve higher TPV system efficiency. Solutions of Maxwell's equations calculated using RCWA are compared to measured sub-bandgap reflectance in experimental GaAs TPV devices with varying metal point-contact diameters and spacing. Modeling and experiments indicate decreased total reflectance due to these diffractive effects for a small point contact diameter of 1 μm, and this effect is much stronger at higher contact coverage fractions.

14 SOLAR ENERGY↗

Effects of size of an oxide layer on the surface properties of lithium irradiated by deuterium plasma

We investigate how growth of an oxide film will influence the deuterium recycling properties of Li on plasma facing surfaces. Lithium films on the walls or plasma-facing material surfaces of a fusion vacuum vessel improves plasma performance in part by removing residual impurity atoms from the plasma. Oxygen atoms, from residual water vapor or eroded oxide surfaces, are a prominent ubiquitous impurity that can create a layer of oxide on lithium films. The results of the work herein also indicate a possibility for determining the thickness of the oxide layer on such Li films by measuring the reflection probability of incident deuterium particles from the surface.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Elucidating the assembly of Nanoparticle Organic Hybrid Materials (NOHMs) near an electrode interface with varying potential using Neutron Reflectivity

A critical concern regarding electrolyte formulation in an electrochemical environment is the impact of the interaction of the multiple components (i.e., supporting electrolyte or additive) with the electrode surface. Recently, liquid-like neat Nanoparticle Organic Hybrid Materials (NOHMs) have been considered as an electrolyte component to improve the transport of redox-active species to the electrode surface. However, the structure and assembly of the NOHMs near the electrode surface is unknown and could significantly impact the electrode-electrolyte interface. Hence, we have investigated the depth profile of polyetheramine (HPE) polymer and NOHM-I-HPE (nanoparticles with ionically bonded HPE polymer) in deuterated water (D2O) in the presence of two different salts (KHCO3 and ZnCl2) near two different electrode surfaces using neutron reflectometry. Moreover, the depth profile of the NOHM-I-HPE near the electrode surface in a potential has also been studied with in-situ reflectivity experiments. Our results indicate that a change in the chemical structure/hydrophilicity of the electrode surface does not significantly impact the ordering of HPE polymer or NOHM-I-HPE near the surface. Here, this study also indicates that the NOHM-I-HPE particles form a clear layer near the electrode surface immediately above an adsorbed layer of free polymer on the electrode surface. The addition of salt does not impact the layering of NOHM-I-HPE, though it does alter the conformation of the polymer grafted to the nanoparticle surface and free polymer sequestered near the surface. Finally, the application of negative potential results in an increased amount of free polymer near the electrode surface. Correlating the depth profile of free polymer and NOHM-I-HPE particles with the electrochemical performance indicates that this assembly of free polymer near the electrode surface in NOHM-I-HPE solutions contributes to the higher current density of the system. Therefore, this holistic study offers insight into the importance of the assembly of NOHM-I-HPE electrolyte and free polymer near the electrode surface in an electrochemical milieu on its performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing Surface Hydration and Isotope Exchange Kinetics in Proton-Conducting Ceramics Using DRIFTS and EIS

This internship project investigates how water vapor partial pressure (pH2O) affects surface hydration and H/D isotope-exchange kinetics in BaZr0.4Ce0.4Y0.1Yb0.1O3?d (4411) proton-conducting ceramic electrolytes. Diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) is used to monitor surface hydroxyl and deuteroxyl species under controlled humidified atmospheres during gas-switching experiments. These surface kinetic trends are to be correlated with bulk, grain-boundary, and total electrolyte resistance measured by electrochemical impedance spectroscopy (EIS) under matching conditions. The future goals of this study are to clarify the relationship between surface hydration dynamics and proton conduction behavior, improving interpretation of EIS data and guiding the optimization of ceramic electrolytes for energy applications.

08 - HYDROGEN↗

Surface intermediates identified using IR spectroscopy during the catalytic oxidation of C 2 H 6 on IrO 2 (1 1 0) at near-ambient pressures

Characterizing surface intermediates during catalysis is essential for developing mechanistic models of catalytic reactions and for identifying rate-controlling steps. Here, in this work, we used polarization-dependent reflection absorption infrared spectroscopy (PD-RAIRS) to investigate surface intermediates that form on IrO 2 (1 1 0) during the catalytic oxidation of C 2 H 6 at pressures near 0.5 Torr. Our results show that adsorbed CO and HCO 2 are the only intermediates detectable with PD-RAIRS across a wide range of temperatures and reactant compositions during complete C 2 H 6 oxidation, giving rise to dominant peaks at about 2093 and 1310 cm −1 , respectively. These assignments were corroborated by RAIRS measurements following CO and HCOOH adsorption in ultrahigh vacuum, RAIRS with C 2 H 6 – 18 O 2 mixtures during catalysis and vibrational frequencies and IR intensities computed using density functional theory. We find that increasing the C 2 H 6 mole fraction in the reaction mixture raises the CO surface coverage relative to HCO 2 , correlating with increasing catalytic oxidation rates. The formation of CO and HCO 2 surface species at temperatures well below catalytic ignition indicates that the overall rate of C 2 H 6 oxidation on IrO 2 (1 1 0) is governed by steps late in the reaction sequence, such as H 2 O formation, CO oxidation and HCO 2 dehydrogenation. These findings provide key insight into the mechanism of alkane oxidation on IrO 2 (1 1 0) and valuable input for first-principles microkinetic modeling.

Pope, Connor [Univ. of Florida, Gainesville, FL (U↗

Seismic Characterization of the Blue Mountain Geothermal Field

Subsurface characterization is crucial for geothermal energy exploration and production. Yet hydrothermal reservoirs usually reside in highly fractured and faulted zones where accurate characterization is very challenging because of low signal-to-noise ratios of land seismic data and lack of coherent reflection signals. We perform an active-source seismic characterization for the Blue Mountain geothermal field in Nevada using active seismic data to reveal the elastic medium property complexity and fault distribution at this field. We first employ an unsupervised machine learning method to attenuate groundroll and near-surface guided-wave noise and enhance coherent reflection and scattering signals from noisy seismic data. We then build a smooth initial P-wave velocity model based on an existing magnetotellurics survey result, and use 3D first-arrival traveltime tomography to refine the initial velocity model. We then derive a set of elastic wave velocities and anisotropic parameters using elastic full-waveform inversion, and obtain PP and PS images using elastic reverse-time migration. We identify major faults by analyzing the variations of seismic velocities and anisotropy parameters, and reveal mid- to small-scale faults by applying a supervised machine learning method to the seismic migration images. Our characterization reveals complex velocity heterogeneities and anisotropies, as well as faults, with a high spatial resolution. These results can provide valuable information for optimal placement of future injection and production wells to increase geothermal energy production at the Blue Mountain geothermal power plant.

58 GEOSCIENCES↗

Discriminating the Role of Surface Hydride and Hydroxyl for Acetylene Semihydrogenation over Ceria through In Situ Neutron and Infrared Spectroscopy

Ceria has been used as a hydrogenation catalyst especially in selective alkyne hydrogenation, but the reaction mechanism regarding the role of different surface hydrogen species remains unclear. Here, we utilized in situ neutron and infrared vibration spectroscopy to show the catalytic role of cerium hydride (Ce–H) and hydroxyl (OH) groups in acetylene hydrogenation over ceria surfaces with different degree of reduction. In situ inelastic neutron scattering spectroscopy (INS) proved that not only Ce–H but also surface atomic hydrogen species on the reduced ceria surface can participate in acetylene semihydrogenation. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results implied that bridging OH groups both on the oxidized and reduced ceria are active in the selective hydrogenation of acetylene. It appears that surface Ce–H is more reactive than the coexisting OH species on the reduced ceria surface, but over-reduction of ceria also results in strongly bound species that may lead to catalyst deactivation. These spectroscopic results clearly explain the reaction mechanism including not only the surface chemistry but also the nature of the active hydrogen species for selective hydrogenation over ceria, providing insights into the design of more active and stable ceria-based catalysts for hydrogenation reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molecular Dynamics Simulation and Cryo-Electron Microscopy Investigation of AOT Surfactant Structure at the Hydrated Mica Surface

Structural properties of the anionic surfactant dioctyl sodium sulfosuccinate (AOT or Aerosol-OT) adsorbed on the mica surface were investigated by molecular dynamics simulation, including the effect of surface loading in the presence of monovalent and divalent cations. The simulations confirmed recent neutron reflectivity experiments that revealed the binding of anionic surfactant to the negatively charged surface via adsorbed cations. At low loading, cylindrical micelles formed on the surface, with sulfate head groups bound to the surface by water molecules or adsorbed cations. Cation bridging was observed in the presence of weakly hydrating monovalent cations, while sulfate groups interacted with strongly hydrating divalent cations through water bridges. The adsorbed micelle structure was confirmed experimentally with cryogenic electronic microscopy, which revealed micelles approximately 2 nm in diameter at the basal surface. At higher AOT loading, the simulations reveal adsorbed bilayers with similar surface binding mechanisms. Adsorbed micelles were slightly thicker (2.2–3.0 nm) than the corresponding bilayers (2.0–2.4 nm). Upon heating the low loading systems from 300 K to 350 K, the adsorbed micelles transformed to a more planar configuration resembling bilayers. The driving force for this transition is an increase in the number of sulfate head groups interacting directly with adsorbed cations.

58 GEOSCIENCES↗