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DOE OSTI2025

Oxygen Evolution on Mechanically Strained TiO2/NiTi: Implications of Compositional Heterogeneity at (Photo)Electrocatalytic Interfaces

The adsorption and activation energetics underpinning small molecule conversion on heterogeneous (photo)electrocatalysts are intrinsically tied to catalyst surface properties. Absent compositional characterization techniques with sufficient interface sensitivity, however, (photo)electrochemical performance can be misinterpreted in the context of bulk or near-surface material properties. Here we provide a fundamental investigation of the convoluting role of near-surface compositional heterogeneity in the interpretation of (photo)electrochemical alkaline oxygen evolution reaction (OER) activity, highlighting challenges in correlating composition measured by surface- and near-surface-sensitive probes. TiO2 thin films grown by air-annealing the superelastic alloy Nitinol (TiO2/NiTi) crack under tensile mechanical strain, increasing the number of electrochemically active Ni sites (Ni site density) that are probed via voltammetric features corresponding to Ni3+/Ni2+ redox events. (Photo)electrochemical OER kinetics trend with Ni site density, with overpotentials and Tafel slopes decreasing for Ni site densities < 1013 Ni/cm2geo and asymptotically approaching the performance of the base NiTi substrate for Ni site densities > 1013 Ni/cm2geo. Photoelectrochemical fill factors follow similar Ni site density dependent trends. When probing unstrained TiO2/NiTi, Ni site densities are two orders of magnitude higher when comparing near-surface-sensitive techniques (e.g., X-ray photoelectron spectroscopy (XPS), time of flight secondary ion mass spectrometry (TOF-SIMS), and scanning transmission electron microscopy-energy dispersive X-ray spectroscopy (STEM-EDS)) to surface-sensitive electrochemical measurements. This result highlights the challenge of correlating kinetic performance with intrinsic surface properties of electrochemical interfaces in the presence of near-surface compositional heterogeneity. Further, it reinforces the importance of fundamental investigations of surfaces with well-controlled composition and structure and the need for physically grounded and self-consistent interpretation of multiple near-surface characterization techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1986

A computer aided thermodynamic approach for predicting the formation of Z-DNA in naturally occurring sequences

The ease with which a particular DNA segment adopts the left-handed Z-conformation depends largely on the sequence and on the degree of negative supercoiling to which it is subjected. We describe a computer program (Z-hunt) that is designed to search long sequences of naturally occurring DNA and retrieve those nucleotide combinations of up to 24 bp in length which show a strong propensity for Z-DNA formation. Incorporated into Z-hunt is a statistical mechanical model based on empirically determined energetic parameters for the B to Z transition accumulated to date. The Z-forming potential of a sequence is assessed by ranking its behavior as a function of negative superhelicity relative to the behavior of similar sized randomly generated nucleotide sequences assembled from over 80,000 combinations. The program makes it possible to compare directly the Z-forming potential of sequences with different base compositions and different sequence lengths. Using Z-hunt, we have analyzed the DNA sequences of the bacteriophage phi X174, plasmid pBR322, the animal virus SV40 and the replicative form of the eukaryotic adenovirus-2. The results are compared with those previously obtained by others from experiments designed to locate Z-DNA forming regions in these sequences using probes which show specificity for the left-handed DNA conformation.

Non-NASA Center↗

NASA NTRS2019

Common Probe Design Study and Follow-On Activities

The Common Probe Study was funded by the NASA's Planetary Science Division in the Science Mission Directorate in 2018 to investigate the feasibility of a common aeroshell design for atmospheric probe missions at Venus, Jupiter, Saturn, Uranus, and Neptune. The study involved 4 NASA Centers: Ames Research Center, Goddard Space Flight Center, Langley Research Center, and the Jet Propulsion Laboratory. The common aeroshell design that was studied was a 400 kg, 1.5 m diameter, 45-degree sphere cone shape with a high density heatshield material (Heatshield for Extreme Entry Environments Technology, or HEEET) and a parachute system to extract the descent vehicle. This size of aeroshell could accommodate a descent vehicle of 0.75 m diameter, which could encompass both Tier 1 and Tier 2 science instruments at each of the 5 destinations. Study methodology: First, a notional payload of instruments for each destination was defined based on the top priority measurements indicated by the Planetary Science Decadal Survey. Steep and shallow entry flight path angles (EFPA) were defined for each planet based on qualification and operational g-load limits for current, state-of-the-art instruments. Interplanetary trajectories were then identified that bounded the EFPA range.Next, 3-DoF simulations for entry trajectories were run using the entry state vectors from the interplanetary trajectories. Conical ribbon parachutes were sized based on heatshield separation dynamics. Aero-heating correlations were used to generate stagnation point convective and radiative heat flux profiles. High fidelity thermal response models for various TPS materials were used to size stagnation point thicknesses, with margins based on previous studies. Backshell TPS masses were assumed based on scaled heat fluxes from the heatshield and also from previous mission concepts.Based on these analyses, we have found that the common design is applicable for atmospheric probe missions for 4 out of the 5 destinations. Because of the unique gravity well for Jupiter, the entry environments are more severe resulting in heat loads an order of magnitude higher than for the other destinations.The next step is to determine what follow-on activities NASA should engage in. A questionnaire for the atmospheric probe community has been developed, with a focus on what size of aeroshell should be further analyzed (smaller or same diameter), and what incentives would make using such an aeroshell, if assembled and available, desirable to mission proposers.Preliminary results from this questionnaire will be presented.

Hwang, Helen H.↗

DOE OSTI2025

Molten Salt Synthesis of Increased (100)-Facet and Polycrystalline Nickel Oxide Nanoparticles for the Oxygen Evolution Reaction: Impact of Facet and Crystallinity on Electrocatalysis

Nickel oxide nanocubes with increased (100) surface facet presence (NiO(100)) were synthesized through a molten salt synthesis procedure to probe their oxygen evolution reaction (OER) activity in order to investigate the relationship between the surface facet and OER performance. While altering the synthesis parameters to decrease NiO(100) particle sizes and agglomeration, a polycrystalline NiO nanoparticle system formed from using Li2O as a Lux-Flood base (labelled Li2O-MSS NiO, where MSS stands for molten salt synthesis). This novel synthesis was further elaborated and the obtained materials were also tested for OER activity. After thorough structural characterization to determine crystallinity, lattice spacings, and elemental distribution, their OER activity was compared versus high surface area NiO(111) nanosheets in a three-electrode rotating disk electrode (RDE) system. The activity trend of (111) > Li2O-MSS > (100) was observed. This decrease in activity of the nanocube and polycrystalline samples was explained by differences between theoretical and experimental conditions, differences in ink rheology and resulting catalyst layer properties, and significant agglomeration seen in the imaging of the sample. Methods for improving the OER activity of these samples are discussed in the conclusion of this study.

08 HYDROGEN↗

DOE OSTI2025

Operation of Argonne's Liquid Salt-Liquid Metal Separation Testbed for U/TRU Product Processing

Argonne National Laboratory has constructed a liquid salt-liquid metal separation testbed for use in the development and advancement of cathode processing of U/TRU co‑deposits generated by pyroprocessing of used nuclear fuel. The U/TRU product recovered from the electrorefiner contains adhered and entrained salt that must be removed prior to consolidation of the U/TRU alloy for use in advanced reactor fuel fabrication. The bottom pour operation utilizes the low melting points of U/TRU co‑deposits and higher densities of molten metals compared to molten salts to separate and consolidate the U/TRU product. Argonne’s testbed is designed to support the development and optimization of bottom-pouring configurations for batch and semi-continuous operations, integration of process monitoring and control technologies, and determination of operational requirements for implementing in an industrial setting. Scoping tests were performed to demonstrate operational aspects of the testbed, including operation using single-pour spout and dual-pour spout configurations, effectiveness of salt containment and extent of salt vaporization, and the use of sensor probes to detect the location of the interface between the metal and salt phases during pouring. Recommendations for process optimization testing for further development of bottom pour processing to separate U/TRU alloys from adhered salt were made based on the results of scoping tests. Completing the recommended activities will increase the technical readiness level (TRL) of the liquid salt-liquid metal separation operation and consolidation of U/TRU alloys to support industrialization of pyroprocessing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1991

The Combined Release and Radiation Effects Satellite program (CRRES): A unique series of scientific experiments

CRRES is a program to study the space environment which surrounds Earth and the effects of space radiation on modern satellite electronic systems. The satellite will carry an array of active experiments including chemical releases and a complement of sophisticated scientific instruments to accomplish these objectives. Other chemical release active experiments will be performed with suborbital rocket probes. These chemical releases will paint the magnetic and electric fields in Earthspace with clouds of glowing ions. Earthspace will be a laboratory, and the releases will be studied with an extensive network of ground-, aircraft-, and satellite-based diagnostic instruments.

Source record↗

NASA NTRS2013

Functional Near-Infrared Spectroscopy Signals Measure Neuronal Activity in the Cortex

Functional near infrared spectroscopy (fNIRS) is an emerging optical neuroimaging technology that indirectly measures neuronal activity in the cortex via neurovascular coupling. It quantifies hemoglobin concentration ([Hb]) and thus measures the same hemodynamic response as functional magnetic resonance imaging (fMRI), but is portable, non-confining, relatively inexpensive, and is appropriate for long-duration monitoring and use at the bedside. Like fMRI, it is noninvasive and safe for repeated measurements. Patterns of [Hb] changes are used to classify cognitive state. Thus, fNIRS technology offers much potential for application in operational contexts. For instance, the use of fNIRS to detect the mental state of commercial aircraft operators in near real time could allow intelligent flight decks of the future to optimally support human performance in the interest of safety by responding to hazardous mental states of the operator. However, many opportunities remain for improving robustness and reliability. It is desirable to reduce the impact of motion and poor optical coupling of probes to the skin. Such artifacts degrade signal quality and thus cognitive state classification accuracy. Field application calls for further development of algorithms and filters for the automation of bad channel detection and dynamic artifact removal. This work introduces a novel adaptive filter method for automated real-time fNIRS signal quality detection and improvement. The output signal (after filtering) will have had contributions from motion and poor coupling reduced or removed, thus leaving a signal more indicative of changes due to hemodynamic brain activations of interest. Cognitive state classifications based on these signals reflect brain activity more reliably. The filter has been tested successfully with both synthetic and real human subject data, and requires no auxiliary measurement. This method could be implemented as a real-time filtering option or bad channel rejection feature of software used with frequency domain fNIRS instruments for signal acquisition and processing. Use of this method could improve the reliability of any operational or real-world application of fNIRS in which motion is an inherent part of the functional task of interest. Other optical diagnostic techniques (e.g., for NIR medical diagnosis) also may benefit from the reduction of probe motion artifact during any use in which motion avoidance would be impractical or limit usability.

Harrivel, Angela↗

NASA NTRS2013

Functional Near-Infrared Spectroscopy Signals Measure Neuronal Activity in the Cortex

Harrivel, Angela↗

NASA NTRS1986

Microwave remote sensing: Active and passive. Volume 3 - From theory to applications

Aspects of volume scattering and emission theory are discussed, taking into account a weakly scattering medium, the Born approximation, first-order renormalization, the radiative transfer method, and the matrix-doubling method. Other topics explored are related to scatterometers and probing systems, the passive microwave sensing of the atmosphere, the passive microwave sensing of the ocean, the passive microwave sensing of land, the active microwave sensing of land, and radar remote sensing applications. Attention is given to inversion techniques, atmospheric attenuation and emission, a temperature profile retrieval from ground-based observations, mapping rainfall rates, the apparent temperature of the sea, the emission behavior of bare soil surfaces, the emission behavior of vegetation canopies, the emission behavior of snow, wind-vector radar scatterometry, radar measurements of sea ice, and the back-scattering behavior of cultural vegetation canopies.

Ulaby, F. T.↗

NASA NTRS1986

Plasma structures in Comet Halley

Large-scale plasma phenomena based on results of spacecraft probing of comets Halley and Giacobini-Zinner and on International Halley Watch are discussed. The data show that: the basic mechanism for the comets' interaction with the solar wind (Alfven, 1957) is correct; that the turn-on and turn-off of plasma activity follows the description of Mendis and Flammer (1984); and that disconnection events are associated with sector boundary crossings and an essential element in the morphology of developed plasma tails (Niedner and Brandt, 1978).

Brandt, John C.↗

NASA NTRS1988

Finite element simulation of thunderstorm electrodynamics in the proximity of the storm

Observations of electric fields, Maxwell current density, and air conductivity over thunderstorms were presented. The measurements were obtained using electric field mils and conductivity probes installed on a U2 aircraft as the aircraft passed approximately directly over an active thunderstorm at an altitude of 18 to 20 km. Accurate electrical observations of this type are rare and provide important information to those involved in numerically modeling a thunderstorm. A preliminary set of computer simulations based on this data were conducted and are described. The simulations show good agreement with measurements and are used to infer the thundercloud's charging current and amount of charge exchanged per flash.

Baginski, Michael Edward↗

NASA NTRS2003

Science with the Space Infrared Telescope Facility

The Space Infrared Telescope Facility (SIRTF), the fourth and final member of NASA's series of Great Observatories, is scheduled to launch on April 15,2003. Together with the Hubbie Space Telescope, the Compton Gamma ray Telescope, and the Chandra X-Ray Telescope this series of observatories offers observational capabilities across the electromagnetic spectrum from the infrared to high-energy gamma rays. SIRTF is based on three focal plane instruments - an infrared spectrograph and two infrared imagers - coupled to a superfluid-helium cooled telescope to achieve unprecedented sensitivity from 3 to 180 microns. Although SIRTF is a powerful general-purpose infrared observatory, its design was based on the capability to address four broad science themes: (1) understanding the structure and composition of the early universe, (2) understanding the nature of brown dwarfs and super-planets, (3) probing protostellar, protoplanetary, and planetary debris disk systems, and (4) understanding the origin and structure of ultraluminous infrared galaxies and active galactic nuclei. This talk will address the design and capabilities of the SIRTF observatory, provide an overview of some of the initial science investigations planned by the SIRTF Guaranteed Time Observers, and give a brief overview of the General Observer proposal process.

Roellig, Thomas L.↗

DOE OSTI2025

Topological magnons and topological electronic properties in metallic Kagome magnets

The primary goal of this project is to study metallic Kagome magnets that potentially host topological electronic properties and topological magnetic excitations, aiming to understand the effect of lattice geometry on topological character of magnons and electronic bands and to study the interplay between magnetism and topological electronic properties. Through this DOE-funded research program, we have unraveled novel electronic and thermoelectric properties of RMn 6 Sn 6 (R = Y, Tb, and Er) and Fe 3 Ge Kagome magnets, including anomalous Hall effect and anomalous Nernst effect, which are associated with the Berry curvature contribution from the massive Dirac gaps in the 3D momentum space. In addition, we have also revealed topological Hall effect and topological Nernst effect, and we ascribed these phenomena to the Berry curvature associated with the magnetic field-induced non-zero scalar spin chirality. These features highlight the synergic effects of the Berry phases in both momentum space and real space of Kagome magnets, which render them excellent candidates for room-temperature electronic and thermoelectric applications based on transverse transport. In addition, through this program we have also study novel thermal transport properties of quantum materials by probing the thermal Hall effect, which can provide crucial insights into nontrivial topological character and chirality of quasiparticles like magnons and magnon-polarons. This report provides an overview of some project activities related to these accomplishments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2014

Let's Exploit Available Knowledge on Vegetation Fluorescence

The potential to measure vegetation fluorescence from space (1) and to derive from it direct information on the gross primary productivity (GPP) of terrestrial ecosystems is probably the most thrilling development in remote sensing and global ecology of recent years, as it moves Earth observation techniques from the detection of canopy biophysics (e.g., fraction of absorbed radiation) and biochemistry (chlorophyll and nitrogen content) to the realm of ecosystem function. The existence of a functional relationship between fluorescence and photosynthesis has been elucidated over the last decade by several laboratories, notably as part of the preliminary studies of the European Space Agency Fluorescence Explorer (FLEX) Earth Explorer Mission. The empirical observation presented by Guanter et al. (2) of a linear relationship between fluorescence radiance and GPP, however, provides the first experimental confirmation of the feasibility of the approach— already thoroughly tested at leaf level—at the desired scale, despite the confounding effects associated with the satellite detection of such a faint signal. A word of clarification is needed here. The use of fluorescence as a probe of leaf photochemistry has been a staple of plant ecophysiology for decades, rooted in a sound understanding of photosynthetic energy dissipation. However, most past studies had to rely for the interpretation of results on active (pulse-saturated) techniques, making them unsuitable for remote-sensing applications. Over recent years, however, novel process based models have been developed for the interpretation of steady-state, solar-induced fluorescence at the leaf to canopy scale (3). We are therefore in a position to move beyond the mere empirical observation of an association between GPP and fluorescence radiance. In particular, Guanter et al. (2) base their analysis on the assumption of a constant ratio between photosynthetic and fluorescence light use efficiencies (equation 3 in ref. 2).We know, however, that the ratio is not constant, but changes widely in response to light, CO2, stomatal limitations, and extreme stress (4, 5). What’s more, we can make sense of such changes, thus extracting valuable information from the very scatter that is apparent in their data. However, this process will require the availability of more tailored instruments, such as the one planned for the FLEX mission. As already stressed by Guanter et al. (2), the spatial resolution of the Global Ozone Monitoring Experiment-2 sensor (40 × 80 km) makes it difficult to compare meaningfully the fluorescence signal with ground measurements, when only 60–70% of the footprint consists of the desired land-cover type (table S1 in ref. 2), suggesting that this could be largely responsible for the low signals observed in European grasslands. Moreover, the overpass time of the MetOp-A satellite (9:30 AM) implies that fluorescence is generally measured under light-limiting conditions, when fluorescence is only marginally affected by stomatal closure even under stress conditions. This result could explain the seasonal mismatch with daily GPP observed in natural ecosystems in the absence of irrigation (figure 4 in ref. 2). We hope, therefore, that this welcome contribution to this fast-advancing field will help demonstrate the potential of the new technique, and pave the way for more refined studies under both a technological and scientific point of view.

Space↗

DOE OSTI2025

Proton, Electron, and Hydrogen-Atom Transfer Thermodynamics of the Metal–Organic Framework, Ti-MIL-125, Are Intrinsically Correlated to the Structural Disorder

Interfacial charge transfer reactions involving protons and/or electrons are fundamental to heterogeneous catalysis and many other reactions relevant to energy, chemical, and biological sectors. Metal–organic frameworks (MOFs) with redox-active metal-oxo nodes have emerged as candidate materials to examine these reactions with near-atomic-level precision, given their crystalline nature. Here, we employed a colloidally stable, Ti-based MOF, Ti-MIL-125, with different crystal sizes to examine catalytically relevant charge transfer thermodynamics. The Ti 8 (μ 2 -O) 8 (μ 2 -OH) 4 nodes structurally mimic TiO 2 , which has shown some PCET reactivity toward reactions of H 2 , O 2 , and others. In this report, we have demonstrated that a change in crystal size induces different amounts of structural disorder to the Ti-oxo node, further changing the thermodynamics of proton/electron/hydrogen-atom transfer reactions. Using electrochemical open-circuit potential (E OCP ) measurements, we have determined that all crystallites undergo a 1H + /1e – redox reaction, which, given the stoichiometry, can be considered as a net H atom transfer (HAT) reaction. The thermodynamics of this HAT reaction, the Ti 3+ O–H bond dissociation free energy (BDFE), was dependent on the crystal size of the MOF, as the decrease in crystal size induced more structural disorder. Our computational calculations have indicated that this difference in BDFE is due to a local change in the geometry of Ti cations, rather than the commonly invoked defects, such as the “missing-linker” defect sites. Individual proton/electron transfer (PT/ET) thermodynamics were also highly dependent on the crystal sizes. These were probed using pK a or band gaps (E g ), respectively. These findings suggest that, particularly when MOFs are nanosized with a large amount of structural disorder, they should no longer be considered “true” single-site catalysts; this is an implicit, but widespread assumption within the MOF-based catalysis field. Implications of these findings will be contrasted with structurally similar metal oxides like TiO 2 and other redox-active MOFs.

Bond dissociation free energy↗

DOE OSTI2025

Probing the proton exchange kinetics of BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3− δ ceramic electrolyte by operando diffuse reflectance infrared Fourier transform spectroscopy

Proton exchange kinetics plays an important role in governing the performance of intermediate-temperature protonic ceramic electrolysis cells (PCECs) for hydrogen production. Our understanding of the nature of the surface hydration reaction at the single-cell level, however, remains very limited, hampering further efficiency improvements. Here, in this study, we developed a custom operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) platform that operates under high temperature and steam conditions with applied bias. Quantitative investigations of surface H 2 O/D 2 O isotope exchange in a BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3−δ (BZCYYb1711) protonic electrolyte-based single cell were conducted under different applied voltages using this DRIFTS platform, to gain molecular-level insight into hydration kinetics. The findings show that the application of an external voltage significantly enhances the surface proton exchange rate, decreasing the apparent activation energy from 29.1 kJ mol −1 at open-circuit voltage (OCV) to 6.8 kJ mol −1 at 1.3 V. In addition, distinct voltage-induced spectral shifts in O–D vibrations point to dynamic changes in surface hydration. These findings demonstrate a sensitive spectroscopic platform for probing interfacial proton processes and reveal strong electrochemical control over surface proton kinetics, offering new opportunities for probing electrolyte hydration behavior in PCECs.

36 - MATERIALS SCIENCE↗

NASA NTRS2002

Overview of the National Aeronautics and Space Administration's Nondestructive Evaluation (NDE) Program

NASA's Office of Safety and Mission Assurance sponsors an Agency-wide NDE Program that supports Aeronautics and Space Transportation Technology, Human Exploration and Development of Space, Earth Science, and Space Science Enterprises. For each of these Enterprises, safety is the number one priority. Development of the next generation aero-space launch and transportation vehicles, satellites, and deep space probes have highlighted the enabling role that NDE plays in these advanced technology systems. Specific areas of advanced component development, component integrity, and structural heath management are critically supported by NDE technologies. The simultaneous goals of assuring safety, maintaining overall operational efficiency, and developing and utilizing revolutionary technologies to expand human activity and space-based commerce in the frontiers of air and space places increasing demands on the Agencies NDE infrastructure and resources. In this presentation, an overview of NASA's NDE Program will be presented, that includes a background and status of current Enterprise NDE issues, and the NDE investment areas being developed to meet Enterprise safety and mission assurance needs through the year 2009 and beyond.

Generazio, Edward R.↗

NASA NTRS2003

Formation Flying and the Stellar Imager Mission Concept

The Stellar Imager (SI) is envisioned as a space-based, W-optical interferometer composed of 10 or more one-meter class elements distributed with a maximum baseline of 0.5 km. image stars and binaries with sufficient resolution to enable long-term studies of stellar magnetic activity patterns, for comparison with those on the sun. It will also support asteroseismology (acoustic imaging) to probe stellar internal structure, differential rotation, and large-scale circulations. SI will enable us to understand the various effects of the magnetic fields of stars, the dynamos that generate these fields, and the internal structure and dynamics of the stars. The ultimate goal of the mission is to achieve the best-possible forecasting of solar activity as a driver of climate and space weather on time scales ranging from months up to decades, and an understanding of the impact of stellar magnetic activity on life in the Universe. In this paper we briefly describe the scientific goals of the mission, the performance requirements needed to address these goals, and the "enabling technology" development efforts required, with specific attention for this meeting to the formation-flying aspects. It is designed to

Carpenter, Kenneth G.↗