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DOE OSTI2019

Deviations from Vegard's law and evolution of the electrocatalytic activity and stability of Pt-based nanoalloys inside fuel cells by in operando X-ray spectroscopy and total scattering

Catalysts for energy related applications, in particular metallic nanoalloys, readily undergo atomic-level changes during electrochemical reactions. The origin, dynamics and implications of the changes for the catalysts’ activity inside fuel cells though are not well understood. This is largely because they are studied on model nanoalloy structures under controlled laboratory conditions. Here we use combined synchrotron X-ray spectroscopy and total scattering to study the dynamic behaviour of nanoalloys of Pt with 3d-transition metals as they function at the cathode of an operating proton exchange membrane fuel cell. Results show that the composition and atomic structure of the nanoalloys change profoundly, from the initial state to the active form and further along the cell operation. The electrocatalytic activity of the nanoalloys also changes. The rate and magnitude of the changes may be rationalized when the limits of traditional relationships used to connect the composition and structure of nanoalloys with their electrocatalytic activity and stability, such as Vegard's law, are recognized. In particular, deviations from the law inherent for Pt-3d metal nanoalloys can well explain their behaviour under operating conditions. Moreover, it appears that factors behind the remarkable electrocatalytic activity of Pt-3d metal nanoalloys, such as the large surface to unit volume ratio and “size misfit” of the constituent Pt and 3d-transition metal atoms, also contribute to their instability inside fuel cells. The new insight into the atomic-level evolution of nanoalloy electrocatalysts during their lifetime is likely to inspire new efforts to stabilize transient structure states beneficial to their activity and stability under operating conditions, if not synthesize them directly.

25 ENERGY STORAGE↗

DOE OSTI2022

Oxygen–coordinated low–nucleus cluster catalysts for enhanced electrocatalytic water oxidation

The oxygen evolution reaction (OER) activity of single-atom catalysts (SACs) is closely related to the coordination environment of the active site. Oxygen-coordinated atomic metal species bring about unique features beyond nitrogen-coordinated atomic metal species due to the fact that the M–O bond is weaker than the M–N bond. Herein, a series of metal–oxygen–carbon structured low-nucleus clusters (LNCs) are successfully anchored on the surface of multiwalled carbon nanotubes (M-MWCNTs, M = Ni, Co, or Fe) through a foolproof low-temperature gas transfer (300°C) method without any further treatment. The morphology and coordination configuration of the LNCs at the atomic level were confirmed by comprehensive characterizations. The synthetic Ni-MWCNTs electrocatalyst features excellent OER activity and stability under alkaline conditions, transcending the performances of Co-MWCNTs, Fe-MWCNTs and RuO 2 . Density functional theory calculations reveal that the moderate oxidation of low-nucleus Ni clusters changes the unoccupied orbital of Ni atoms, thereby lowering the energy barrier of the OER rate-limiting step and making the OER process more energy-efficient. This study demonstrates a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts.

36 MATERIALS SCIENCE↗

DOE OSTI2015

A Discontinuous Petrov-Galerkin Methodology for Adaptive Solutions to the Incompressible Navier-Stokes Equations

The discontinuous Petrov-Galerkin methodology with optimal test functions (DPG) of Demkowicz and Gopalakrishnan [18, 20] guarantees the optimality of the solution in an energy norm, and provides several features facilitating adaptive schemes. Whereas Bubnov-Galerkin methods use identical trial and test spaces, Petrov-Galerkin methods allow these function spaces to differ. In DPG, test functions are computed on the fly and are chosen to realize the supremum in the inf-sup condition; the method is equivalent to a minimum residual method. For well-posed problems with sufficiently regular solutions, DPG can be shown to converge at optimal rates—the inf-sup constants governing the convergence are mesh-independent, and of the same order as those governing the continuous problem [48]. DPG also provides an accurate mechanism for measuring the error, and this can be used to drive adaptive mesh refinements. We employ DPG to solve the steady incompressible Navier-Stokes equations in two dimensions, building on previous work on the Stokes equations, and focusing particularly on the usefulness of the approach for automatic adaptivity starting from a coarse mesh. We apply our approach to a manufactured solution due to Kovasznay as well as the lid-driven cavity flow, backward-facing step, and flow past a cylinder problems.

adaptive finite elements↗

DOE OSTI2026

Spatiotemporal and Statistical Mapping of Transition Metal Equilibria in Alkaline Media

Transition metal dissolution and redeposition (D/R) kinetics in alkaline media play a critical role in various chemical and electrochemical processes. Competitive reaction kinetics between different transition metals can modulate individual metal behavior in these processes. To date, these phenomena have remained largely unmeasured, and even when captured, they are difficult to statistically characterize due to their dynamic nature, simultaneous occurrence, and spatially heterogeneous nature. Here, in this study, we develop a statistical analysis framework based on in situ and operando X-ray fluorescence microscopy (XFM) to investigate the relative D/R kinetics of multiple transition metals in alkaline media. By employing statistical analysis, we quantify the spatial distribution of D/R species and assess the rate at which the system reaches equilibrium under varying reaction conditions. We show that pH does not simply change the rate of dissolution and redeposition, but reorganizes the cross-element kinetic correlations among Ni, Fe, and Mn and accelerates the spatial equilibration of D/R events, as quantified through correlation analysis, reaction-rate estimation, probability function distributions, and texture-based monitoring statistics. Additionally, we demonstrate how modifying the solvent environment can influence D/R kinetics, providing a pathway for tuning materials synthesis and process optimization. Our study offers valuable insights into the complex interplay between different transition metals and provides a reliable statistical framework for spatial analysis of diverse imaging data sets, enabling deeper extraction of latent information across multiple modalities.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Task Sharing of Proton Incorporation in Vertically Aligned Nanocomposite Triple Conductors: Growth, Structure, and Surface Exchange Kinetics

As protonic ceramic electrolysis cells emerge for efficient H 2 production, there is a need to develop air electrode materials enabling fast, durable steam splitting and proton incorporation. Single-phase triple conductors may fail to satisfy the myriad performance/stability requirements, and their critical charge-carriers (holes, oxygen vacancies, and protons) are in competition, limiting their concentrations. Instead, we propose task-sharing, vertically aligned nanocomposites (VANs), comprising a proton conductor (BaZr 0.9 Y 0.1 O 3-δ ) and a redox-active mixed ionic electronic conductor (Ce 0.9 Pr 0.1 O 2-δ ), that may enable rapid proton surface exchange at the solid–gas interface and transport along the solid–solid heterointerfaces. We grew VANs by pulsed laser deposition and investigated the interplay between their processing conditions, structure, and proton and oxygen surface exchange kinetics. We varied the substrate temperature, laser repetition rate, laser fluence, and processing oxygen pressure. The crystallinity and phases were characterized by grazing-incidence X-ray diffraction, and the strain and structural order as a function of depth were evaluated by angle-dependent synchrotron X-ray pair distribution function analysis. To evaluate the potential for interdiffusion, the formation energies of substitutional defects were simulated with density functional theory. Corresponding structural analysis and elemental mapping were performed by scanning/transmission electron microscopy, energy-dispersive X-ray spectroscopy, and electron energy-loss spectroscopy, indicating distinct nanoscale compositional regions with a hierarchical structure embedded in individual VANs columns and minimal interdiffusion across a bilayer film. Proton and oxygen surface exchange coefficients (k H , k O ) and polarization resistances were evaluated by electrical and optical relaxations and impedance spectroscopy of VAN-incorporated protonic ceramic electrochemical cells, respectively, at 400–500 °C, demonstrating values comparable to some of the best-known triple and mixed conductors.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Experimental Evaluation of Dual-Opposed Jet Mixer Pump Performance for Slurry Mixing

Million-gallon double-shell tanks at Hanford are used to store transuranic, high-level, and low-level radioactive wastes. These wastes consist of a large volume of salt-laden solution covering a smaller volume of settled sludge primarily containing metal hydroxides. These wastes will be retrieved and processed into immobile waste forms suitable for permanent disposal. Retrieval is an important step in implementing these disposal scenarios. The retrieval concept evaluated is to use submerged dual-nozzle jet mixer pumps with horizontally oriented nozzles located near the tank floor that produce horizontal jets of fluid to mobilize the settled solids. The mixer pumps are oscillated through 180 about a vertical axis so the high velocity fluid jets sweep across the floor of the tank. After the solids are mobilized, the pumps will continue to operate at a reduced flow rate producing lower velocity jets sufficient to maintain the particles in a uniform suspension (concentration uniformity). Several types of waste and tank configurations exist at Hanford. The jet mixer pump systems and operating conditions required to mobilize sludge and maintain slurry uniformity will be a function of the waste type and tank configuration. The focus of this work was to conduct a 1/12-scale experiment to develop an analytical model to relate slurry uniformity to tank and mixer pump configurations, operating conditions, and sludge properties. This experimental study evaluated concentration uniformity in a 1/12-scale experiment varying the Reynolds number (Re), Froude number (Fr), and gravitational settling parameter (Gs) space. Simulant physical properties were chosen to obtain the required Re and Gs where Re and Gs were varied by adjusting the kinematic viscosity and mean particle diameter, respectively. Test conditions were achieved by scaling the jet nozzle exit velocity in a 75-in. diameter tank using a mock-up of a centrally located dual-opposed jet mixer pump located just above the tank floor. Concentration measurements at sampling locations throughout the tank were used to assess the degree of uniformity achieved during each test. Concentration data was obtained using a real time in-situ ultrasonic attenuation probe and post-test analysis of discrete batch samples. The undissolved solids concentration at these locations was analyzed to determine whether the tank contents were uniform (≤ ±10% variation about mean) or nonuniform (> ±10% variation about mean) in concentration. Concentration inhomogeneity was modeled as a function of dimensionless parameters. The parameters that best describe the maximum solids volume fraction that can be suspended were found to be 1) the Fr based on nozzle average discharge velocity and tank contents level and 2) the dimensionless particle size based on nozzle diameter. The dependence on the jet Re does not appear to be statistically significant.

correlation↗

DOE OSTI2020

Hanford Site-wide Natural Recharge Boundary Condition for Groundwater Models

The purpose of this environmental calculation file (ECF) is to document the development of a tool that generates temporally and spatially variable representations of natural recharge for the Hanford Site. A key feature of the recharge evolution tool (RET) is that it applies sanctioned natural re-charge rates varying as a function of the condition/cover of the ground surface and soil type at different points in time. No hydrologic calculations are performed by the RET, this script works as a lookup data base between spatial and temporal datasets to assign research-based recharge rates to corresponding regions throughout the Hanford Site. This work will support vadose zone and groundwater models for the Hanford Site. Although efforts will focus on generating recharge estimates for the entirety of the Hanford Site, the focus scope of this work will be the Central Plateau Area to support the Composite Analysis Vadose Zone facet. In other words, the reliability of this calculation will be greatest within the Central Plateau Area and decrease with departures from that geographic region.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics (ROCKE-3D) 1.0: A General Circulation Model for Simulating the Climates of Rocky Planets

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics (ROCKE-3D) is a three-dimensional General Circulation Model (GCM) developed at the NASA Goddard Institute for Space Studies for the modeling of atmospheres of solar system and exoplanetary terrestrial planets. Its parent model, known as ModelE2, is used to simulate modern Earth and near-term paleo-Earth climates. ROCKE-3D is an ongoing effort to expand the capabilities of ModelE2 to handle a broader range of atmospheric conditions, including higher and lower atmospheric pressures, more diverse chemistries and compositions, larger and smaller planet radii and gravity, different rotation rates (from slower to more rapid than modern Earth’s, including synchronous rotation), diverse ocean and land distributions and topographies, and potential basic biosphere functions. The first aim of ROCKE-3D is to model planetary atmospheres on terrestrial worlds within the solar system such as paleo-Earth, modern and paleo-Mars, paleo-Venus, and Saturn’s moon Titan. By validating the model for a broad range of temperatures, pressures, and atmospheric constituents, we can then further expand its capabilities to those exoplanetary rocky worlds that have been discovered in the past, as well as those to be discovered in the future. We also discuss the current and near-future capabilities of ROCKE-3D as a community model for studying planetary and exoplanetary atmospheres.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1974

Acoustic properties of organic acid mixtures in water

The variation of the rate of propagation of ultrasounds in organic acid mixtures in water points to structural changes caused by interactions that take place under conditions of thermal agitation, at different acid concentrations. At the same time, a difference is found in the changes in velocity as a function of the length of the carbon chain of the acids in the mixture as a result of their effect on the groups of water molecules associated by hydrogen bonds.

Macavei, I.↗

NASA NTRS1979

Performance, physiological, and oculometer evaluation of VTOL landing displays

A methodological approach to measuring workload was investigated for evaluation of new concepts in VTOL aircraft displays. Physiological, visual response, and conventional flight performance measures were recorded for landing approaches performed in the NASA Visual Motion Simulator (VMS). Three displays (two computer graphic and a conventional flight director), three crosswind amplitudes, and two motion base conditions (fixed vs. moving base) were tested in a factorial design. Multivariate discriminant functions were formed from flight performance and/or visual response variables. The flight performance variable discriminant showed maximum differentation between crosswind conditions. The visual response measure discriminant maximized differences between fixed vs. motion base conditions and experimental displays. Physiological variables were used to attempt to predict the discriminant function values for each subject/condition trial. The weights of the physiological variables in these equations showed agreement with previous studies. High muscle tension, light but irregular breathing patterns, and higher heart rate with low amplitude all produced higher scores on this scale and thus represent higher workload levels.

North, R. A.↗

NASA NTRS1983

Effect of suction and blowing on boundary-layer transition

The effects of wall blowing and suction on boundary-layer stability and transition are studied on a flat plate. Titanium panels, in which 0.063 mm diameter holes were drilled on 0.635 mm centers, are inserted on the plate. Suction level and distribution are variable. Disturbances are introduced by means of a vibrating ribbon and measurements of both mean-flow and disturbance-flow velocities are made with a hot wire. Disturbance amplitudes are measured as a function of Reynolds number, frequency, and suction characteristics and compared with the previous Dynapore results of Reynolds and Saric. Transition measurements under natural and forced conditions are also made. The stabilizing effects of suction are documented. It is also shown that very high local flow rates through the suction holes (which approach a hole Reynolds number of 300) do not destabilize the flow. On the other hand, weak blowing lowers the transition Reynolds number but is found not to cause serious problems.

Saric, W. S.↗

NASA NTRS1997

Nickel-Hydrogen Battery Fault Clearing at Low State of Charge

Fault clearing currents were achieved and maintained at discharge rates from C/2 to C/3 at high and low states of charge. The fault clearing plateau voltage is strong function of: discharge current, and voltage-prior-to-the-fault-clearing-event and a weak function of state of charge. Voltage performance, for the range of conditions reported, is summarized.

Lurie, C.↗

NASA NTRS1998

Predicting lettuce canopy photosynthesis with statistical and neural network models

An artificial neural network (NN) and a statistical regression model were developed to predict canopy photosynthetic rates (Pn) for 'Waldman's Green' leaf lettuce (Latuca sativa L.). All data used to develop and test the models were collected for crop stands grown hydroponically and under controlled-environment conditions. In the NN and regression models, canopy Pn was predicted as a function of three independent variables: shootzone CO2 concentration (600 to 1500 micromoles mol-1), photosynthetic photon flux (PPF) (600 to 1100 micromoles m-2 s-1), and canopy age (10 to 20 days after planting). The models were used to determine the combinations of CO2 and PPF setpoints required each day to maintain maximum canopy Pn. The statistical model (a third-order polynomial) predicted Pn more accurately than the simple NN (a three-layer, fully connected net). Over an 11-day validation period, average percent difference between predicted and actual Pn was 12.3% and 24.6% for the statistical and NN models, respectively. Both models lost considerable accuracy when used to determine relatively long-range Pn predictions (> or = 6 days into the future).

Non-NASA Center↗

NASA NTRS2004

Autonomous and Autonomic Systems: A Paradigm for Future Space Exploration Missions

NASA increasingly will rely on autonomous systems concepts, not only in the mission control centers on the ground, but also on spacecraft and on rovers and other assets on extraterrestrial bodies. Automomy enables not only reduced operations costs, But also adaptable goal-driven functionality of mission systems. Space missions lacking autonomy will be unable to achieve the full range of advanced mission objectives, given that human control under dynamic environmental conditions will not be feasible due, in part, to the unavoidably high signal propagation latency and constrained data rates of mission communications links. While autonomy cost-effectively supports accomplishment of mission goals, autonomicity supports survivability of remote mission assets, especially when human tending is not feasible. Autonomic system properties (which ensure self-configuring, self-optimizing self-healing, and self-protecting behavior) conceptually may enable space missions of a higher order into any previously flown. Analysis of two NASA agent-based systems previously prototyped, and of a proposed future mission involving numerous cooperating spacecraft, illustrates how autonomous and autonomic system concepts may be brought to bear on future space missions.

Truszkowski, Walter F.↗

NASA NTRS2017

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics (ROCKE-3D) 1.0: A General Circulation Model for Simulating the Climates of Rocky Planets

Resolving Orbital and Climate Keys of Earth and Extraterrestrial Environments with Dynamics (ROCKE-3D) is a three-dimensional General Circulation Model (GCM) developed at the NASA Goddard Institute for Space Studies for the modeling of atmospheres of solar system and exoplanetary terrestrial planets. Its parent model, known as ModelE2, is used to simulate modern Earth and near-term paleo-Earth climates. ROCKE-3D is an ongoing effort to expand the capabilities of ModelE2 to handle a broader range of atmospheric conditions, including higher and lower atmospheric pressures, more diverse chemistries and compositions, larger and smaller planet radii and gravity, different rotation rates (from slower to more rapid than modern Earth's, including synchronous rotation), diverse ocean and land distributions and topographies, and potential basic biosphere functions. The first aim of ROCKE-3D is to model planetary atmospheres on terrestrial worlds within the solar system such as paleo-Earth, modern and paleo-Mars, paleo-Venus, and Saturn's moon Titan. By validating the model for a broad range of temperatures, pressures, and atmospheric constituents, we can then further expand its capabilities to those exoplanetary rocky worlds that have been discovered in the past, as well as those to be discovered in the future. We also discuss the current and near-future capabilities of ROCKE-3D as a community model for studying planetary and exoplanetary atmospheres.

Astrobiology↗

NASA NTRSDate not supplied

Investigation of Liquid Fuel Injection Processes in a Rotating Detonation Combustor using Megahertz Planar Laser-Induced Fluorescence Imaging

Direct imaging of liquid fuel injection is performed within an optically accessible rotating detonation combustor (RDC) using planar laser-induced fluorescence (PLIF) to spatio-temporally resolve the highly dynamic spray characteristics at rates up to 1 MHz. The RDC is operated on air and hydrogen to sustain a stable, cyclically propagating detonation wave with cycle periods of up to ∼250 μs. One of the hydrogen fuel injection sites is replaced with a liquid jet to introduce a diesel spray as a fuel surrogate to enable tracer-free fluorescence excitation using the 355 nm third-harmonic output of a burst-mode Nd:YAG laser. The time-resolved PLIF measurements reveal the evolution of the highly unsteady spray, including the dwell period after the arrival of the detonation wave, the jet recovery, breakup and entrainment into the supersonic crossflow of air, propagation into the detonation chamber, and interaction with the detonation wave. Following passage of the detonation wave, the spray characteristics reveal significant changes in the momentum flux ratio between the liquid and air streams, altering the jet trajectory and temporarily halting fuel delivery to the detonation channel. This temporary cessation of fuel spray injection into the combustor is quantified, along with the fill rate as a function of time. As the injection system recovers, the fuel spray eventually returns to a quasi-steady position prior to the arrival of the detonation wave, allowing qualitative comparisons with theoretical jet trajectories for a range of air mass-flux conditions. These data, enabled by ultra-high-speed PLIF imaging, represent some of the first detailed measurements for characterizing and quantifying the interactions of liquid jets and detonations in an operating RDC.

Propulsion↗

NASA NTRSDate not supplied

Investigation of Liquid Fuel Refill Dynamics in a Rotating Detonation Combustor using Megahertz Planar Laser-Induced Fluorescence

Propulsion↗

NASA NTRSDate not supplied

Evaluating a Cognitive Extension for the Licklider Transmission Protocol in a Spacecraft Emulation Testbed

In space communications, particularly when involving regions beyond cislunar space, the development of advanced networking solutions is essential to address the challenges posed by limited connectivity, substantial propagation delays, and radio signal variations. This study explores a data-driven approach to the Licklider Transmission Protocol (LTP), specifically focusing on dynamically adjusting the maximum payload size of segments. Prior research has emphasized the potential benefits of dynamically adjusting this parameter, introducing the concept of Cognitive LTP. This paper presents a software implementation of Cognitive LTP (CLTP) within an open-source Delay Tolerant Networking (DTN) framework, specifically the High-rate Delay Tolerant Networking (HDTN), and experimentally evaluates its performance under realistic space conditions. Leveraging the Cognitive Ground Testbed (CGT), developed by NASA GRC for spacecraft communication emulation, this study effectively bridges the gap between theoretical advancements and practical applications. By thoroughly analyzing CLTP’s functionality within the CGT, this research offers insights into the practical implications of adaptive networking strategies, emphasizing the importance of conducting tests in relevant environments for the maturation of space communication technologies.

Delay Tolerant Networking↗