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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

On the Limited Role of Electronic Support Effects in Selective Alkyne Hydrogenation: A Kinetic Study of Au/MO x Catalysts Prepared from Oleylamine‐Capped Colloidal Nanoparticles

Abstract We report a quantitative kinetic evaluation and study of support effects for partial alkyne hydrogenation using oleylamine‐capped Au colloids as catalyst precursors. The amine capping agents can be removed under reducing conditions, generating supported Au nanoparticles of ∼2.5 nm in diameter. The catalysts showed high alkene selectivity (>90 %) at all conversions during alkyne partial hydrogenation. Catalytic activity, observed rate constants, and apparent activation energies (25–40 kJ/mol) were similar for all Au catalysts, indicating support effects are relatively small. Alkyne adsorption, probed with FTIR and DFT, showed adsorption on the support was associated with hydrogen‐bonding interactions. DFT calculations indicate strong alkyne adsorption on Au sites, with the strongest adsorption sites at the metal‐support interface (MSI). The catalysts had similar hydrogen reaction orders (0.7–0.9), and 1‐octyne reaction orders (∼−0.2), suggesting a common mechanism. The reaction kinetics are most consistent with a mechanism involving the non‐competitive activated adsorption of H 2 on an alkyne‐covered Au surface.

Bruno, James E.↗
DOE OSTI2012

FY2012 Report on Fast Reactor Toolset Work (PROTEUS-Fast)

As part of the NEAMS activity in DOE, a fast reactor simulation program was launched in April 2007, termed SHARP. The initial goal of SHARP was to develop a suite of modern simulation tools specifically for the analysis and design of sodium cooled fast reactors, and this goal has since been extended to consider all reactor types of interest. As part of that work, a high‐fidelity deterministic neutron transport code named UNIC was started, providing a common framework for fast reactor neutronics tools. Focusing on UNIC, spatial de‐homogenization increased the typical neutronics problem with a few hundred million degrees of freedom (DOF) into ones with hundreds of trillions of DOF. Such problems are beyond the capabilities of existing supercomputers. With the advent of future computer hardware, these high‐fidelity problems can be solved but only after a multiyear development program to adapt codes such as UNIC to that technology. UNIC can presently be used on smaller problems (single assembly, multiple assemblies) with today’s hardware, but it is also necessary to provide tools to solve the larger problems of interest, albeit without the aforementioned level of spatial de‐homogenization. To address the desire to demonstrate the coupling capability of NEAMS, part of the FY12 funding was focused on preparing the legacy codes, termed PROTEUS‐Fast, which are fully capable of solving full‐scale fast reactor problems. A bulk of the work this year was focused on preparing and distributing the PROTEUS‐Fast codes for use by all NEAMS users. The demonstration of a full coupling capability will require more follow on work, but significant progress was made this year preparing the interface coupling routines and preparing PROTEUS‐Fast for use. The primary targets of interest in PROTEUS‐Fast are DIF3D, DIF3D‐K (kinetics), and VARI3D (reactivity coefficients), with REBUS (fuel cycle) being an auxiliary component updated for convenience. All codes in PROTEUS‐Fast were verified and added to the BuildBot regression test. Unfortunately, all of the older codes suffered significant problems from the deprecated coding practices used within them and resulting conflicts with modern compilers. After some work, all of these issues were resolved and we feel confident in releasing them for use by others NEAMS members. With regard to specific upgrades, DIF3D‐VARIANT was upgraded with a few months of effort to allow the large scale problems of interest to be executed. After significant study, we choose not to modify VARI3D to include a transport option, but to develop a new code, PERSENT (partially funded by an external project) which uses the DIF3D‐VARIANT transport solution option. The outstanding features missing from MC 2 ‐3 were added, and MC 2 ‐3 has been released to RSICC. All of the remaining PROTEUS‐Fast codes are either finished with the copyright and licensing procedure or are actively going through it. While that process will delay the targeted August 2012 release to RSICC for a few more months, the codes are ready for immediate use and can be connected to the framework either by us or by others as the interface readers and documentation will be released with the PROTEUS‐Fast codes.

Wolters, E. R.↗
DOE OSTI2016

Ionic charging by local imbalance at interfaces in hybrid lead halide perovskites

Identification of specific operating mechanisms becomes particularly challenging when mixed ionic-electronic conductors are used in optoelectronic devices. Ionic effects in perovskite solar cells are believed to distort operation curves and possess serious doubts about their long term stability. Current hysteresis and switchable photovoltaic characteristics have been connected to the kinetics of ion migration. However, the nature of the specific ionic mechanism (or mechanisms) able to explain the operation distortions is still poorly understood. It is observed here that the local rearrangement of ions at the electrode interfaces gives rise to commonly observed capacitive effects. Charging transients in response to step voltage stimuli using thick CH{sub 3}NH{sub 3}PbI{sub 3} samples show two main polarization processes and reveal the structure of the ionic double-layer at the interface with the non-reacting contacts. It is observed that ionic charging, with a typical response time of 10 s, is a local effect confined in the vicinity of the electrode, which entails absence of net mobile ionic concentration (space-charge) in the material bulk.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Using “Tender” x-ray ambient pressure x-Ray photoelectron spectroscopy as a direct probe of solid-liquid interface

We report a new method to probe the solid-liquid interface through the use of a thin liquid layer on a solid surface. An ambient pressure XPS (AP-XPS) endstation that is capable of detecting high kinetic energy photoelectrons (7 keV) at a pressure up to 110 Torr has been constructed and commissioned. Additionally, we have deployed a “dip & pull” method to create a stable nanometers-thick aqueous electrolyte on platinum working electrode surface. Combining the newly constructed AP-XPS system, “dip & pull” approach, with a “tender” X-ray synchrotron source (2 keV–7 keV), we are able to access the interface between liquid and solid dense phases with photoelectrons and directly probe important phenomena occurring at the narrow solid-liquid interface region in an electrochemical system. Using this approach, we have performed electrochemical oxidation of the Pt electrode at an oxygen evolution reaction (OER) potential. Under this potential, we observe the formation of both Pt²⁺ and Pt⁴⁺ interfacial species on the Pt working electrode in situ . We believe this thin-film approach and the use of “tender” AP-XPS highlighted in this study is an innovative new approach to probe this key solid-liquid interface region of electrochemistry.

25 ENERGY STORAGE↗
DOE OSTI2014

Fast and slow crystal growth kinetics in glass-forming melts

Published values of crystal growth rates are compared for supercooled glass-forming liquids undergoing congruent freezing at a planar crystal-liquid interface. For the purposes of comparison pure metals are considered to be glass-forming systems, using data from molecular-dynamics simulations. For each system, the growth rate has a maximum value U{sub max} at a temperature T{sub max} that lies between the glass-transition temperature T{sub g} and the melting temperature T{sub m}. A classification is suggested, based on the lability (specifically, the propensity for fast crystallization), of the liquid. High-lability systems show “fast” growth characterized by a high U{sub max}, a low T{sub max} / T{sub m}, and a very broad peak in U vs. T / T{sub m}. In contrast, systems showing “slow” growth have a low U{sub max}, a high T{sub max} / T{sub m}, and a sharp peak in U vs. T / T{sub m}. Despite the difference of more than 11 orders of magnitude in U{sub max} seen in pure metals and in silica, the range of glass-forming systems surveyed fit into a common pattern in which the lability increases with lower reduced glass-transition temperature (T{sub g} / T{sub m}) and higher fragility of the liquid. A single parameter, a linear combination of T{sub g} / T{sub m} and fragility, can show a good correlation with U{sub max}. For all the systems, growth at U{sub max} is coupled to the atomic/molecular mobility in the liquid. It is found that, across the diversity of glass-forming systems, T{sub max} / T{sub g} = 1.48 ± 0.15.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Crystallization kinetics of amorphous acetonitrile nanoscale films

We measure the isothermal crystallization kinetics of amorphous acetonitrile films using molecular beam dosing and reflection adsorption infrared spectroscopy RAIRS techniques. Experiments on a graphene covered Pt(111) substrate revealed that the crystallization rate slows dramatically at long times and that the overall kinetics cannot be described by a simple application of the Avrami equation. The crystallization kinetics also have a thickness dependence with the thinner films crystallizing much slower than thicker ones. Additional experiments showed that decane layers at both the substrate and vacuum interfaces can also affect the crystallization rates. A comparison of the crystallization rates for CH 3 CN and CD 3 CN films showed only an isotope effect of ~1.09. When amorphous films were deposited on a crystalline film, the crystalline layer did not act as a template for the formation of a crystalline growth front. Finally, these overall results suggest that the crystallization kinetics complicated indicating the possibility of multiple nucleation mechanisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Evolution and Degradation Patterns of Electrochemical Cells Based on the Analysis of Interfacial Phenomena at Li Metal Anode/Electrolyte Interfaces

In this work, we report the results of a theoretical–computational analysis of the solid electrolyte interphase (SEI) growth and degradation dynamics occurring in lithium metal batteries during cycling. We use ab initio-kinetic Monte Carlo simulations to generate a synthetic data set, which is analyzed by machine learning methods. We aim to determine: (i) how modifications in interfacial interaction energies between solid electrolyte interphase (SEI) blocks and between Li ions and SEI facets impact the Coulombic efficiency (CE) of the battery and (ii) what factors, including reactions, microscopic transport, and other interfacial events, may lead to cell performance “failure” during prolonged charge and discharge cycles, signaled as a sharp decay in the CE over cycling. The demonstration of our approach is done on a cell including a Li metal surface interfacing with a previously introduced state-of-the-art electrolyte, and the idea can be applied to any electrochemical system. Outcomes include the identification of the leading chemical, physical, and structural variables causing cell failure and relating them to the electrolyte formulation, thus paving the way to future more refined analysis and electrolyte design.

batteries↗
DOE OSTI2020

Mathematical Modeling of Hydroxide-Exchange-Membrane Water Electrolyzer

Water electrolyzers can transform intermittent renewable energy like solar energy and wind energy into the chemical energy of hydrogen with zero greenhouse-gas emissions. The hydroxide-exchange membrane electrolyzer (HEME) combines the capability to produce pressurized hydrogen with the advantage of being able to use low or non-platinum group metal (PGM) electrocatalysts in the alkaline environment.1 Hydroxide salts, for example, KOH, are added to the HEME water feed on both anode and cathode to improve its performance. However, the specific mechanism of performance improvement still needs to be further understood. In addition, at high current densities, bubble evolution can result in mass-transport limitations, a less well studied phenomena. Mathematical modeling is ideal to explore these issues as it is cost and time efficient and can deconvolute the physics, processes, and observed phenomena and study the applied-voltage breakdown. In this work, we extend our previously developed 1D two-phase continuum model2 to study the varies processes in the HEME and provide insights on performance optimizations. First, the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) kinetics at different hydroxide concentrations have been studied by rotating disk electrodes (RDE) and implemented in the model. Then, the model is calibrated and validated against experimental HEME polarization curves for different KOH concentrations as a liquid electrolyte. The model clearly shows a performance increase with increasing KOH concentrations, which is consistent with the experimental results. The reduced ohmic resistance and increased electrochemical active surface area (ECSA) are the two main reasons for performance increase. The large amount of hydroxide in the liquid electrolyte not only helps to distribute the reactant hydroxide throughout the catalyst layer (CL), which reduces ohmic loss, but also enables reaction at the interface between the liquid electrolyte and electrocatalyst, which increases the ECSA. Applied-voltage breakdown demonstrates that the electrolyzer performance is dominated by anode kinetics and ohmic loss. A comparison with the DI water feed shows a more uniform current distribution in the anode CL when KOH is added, which indicates a higher utilization of the CL. Second, we present modeling on the effects of bubble coverage. As gas evolves, part of the ECSA is minimized due to bubble coverage. To account for this effect, an empirical relationship between the fractional bubble coverage and the current density is implemented in the model.3 The model shows this bubble coverage effect is more pronounced at large current densities with DI water feed. Acknowledgements This work was funded under the HydroGEN Consortium by the Energy Efficiency and Renewable Energy, Hydrogen and Fuel Cell Technologies Office, of the U. S. Department of Energy under contract number DE-AC02-05CH11231. References R. Abbasi, B. P. Setzler, S. Lin, J. Wang, Y. Zhao, H. Xu, B. Pivovar, B. Tian, X. Chen, G. Wu and Y. Yan, 31, 1805876 (2019). L. N. Stanislaw, M. R. Gerhardt and A. Z. Weber, ECS Transactions, 92, 767 (2019). H. Vogt and R. J. Balzer, Electrochimica Acta, 50, 2073 (2005).

Liu, Jiangjin↗
NASA NTRS1978

Oxide morphology and spalling model for NiAl

A scanning electron microscope equipped with an energy dispersive spectrographic unit was used to study in detail the Al2O3 oxide morphology and oxide-metal interface of a nickel-rich NiAl alloy (Ni-42 at% Al) with a view toward providing information relevant to spalling theories in the MCrAlY system. In addition, the kinetics of spalling was studied for critical evaluation of one of the step-process spall models and for collection of pertinent experimental data. Cyclic oxidation tests were run in 1-atm air at about 1100 C, and isothermal specimens were examined from 2 min to 200 hr of exposure. It is shown that oxide spalling occurs primarily at the oxide-metal interface in an intergranular mode, that crystallographic Kirkendall voids arise as a result of oxidation, and that the fractional area of spalled oxide varies widely in cyclic tests but increases with the square of oxide thickness for isothermal tests. A spall model is developed in the form of a summation series.

Smialek, J. L.↗
DOE OSTI2018

High Activity of Au/K/TiO 2 (110) for CO Oxidation: Alkali-Metal-Enhanced Dispersion of Au and Bonding of CO

In this paper, images from scanning tunneling microscopy show high mobility for potassium (K) on an oxidized TiO 2 (110) surface. At low coverages, the alkali metal occupies mainly terrace sites of the o-TiO 2 (110) system. The results of X-ray photoelectron spectroscopy indicate that K is fully ionized. The electron transferred from K to the titania affects the reactivity of this oxide, favoring the dispersion of Au particles on the terraces of the o-TiO 2 (110) surface. When small coverages of K and Au are present on the o-TiO 2 (110) system, only a few K–Au pairs are formed and the alkali metal affects Au chemisorption mainly through the oxide interactions. Addition of K to Au/o-TiO 2 (110) enhances the reactivity of the system, opening new reaction paths for the adsorption and oxidation of carbon monoxide. CO can undergo disproportionation (2CO → C ads + CO 2,ads ) on K/o-TiO 2 (110) and Au/K/o-TiO 2 (110) surfaces. The Au–KO x interface binds CO much better than plain Au–TiO 2 , increasing the surface coverage of CO and facilitating its oxidation. Kinetic tests show that K promotes CO oxidation on Au/TiO 2 . Finally, turnover frequencies of 2.1 and 10.8 molecules (Au site) -1 s –1 were calculated for oxidation of CO on Au/o-TiO 2 (110) and Au/K/o-TiO 2 (110) catalysts, respectively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Design principles of heterointerfacial redox chemistry for highly reversible lithium metal anode

High electrochemical reversibility is required for the application of high-energy-density lithium (Li) metal batteries; however, inactive Li formation and SEI (solid electrolyte interface)-instability-induced electrolyte consumption cause low Coulombic efficiency (CE). The prior interfacial chemical designs in terms of alloying kinetics have been used to enhance the CE of Li metal anode; however, the role of its redox chemistry at heterointerfaces remains a mystery. Herein, the relationship between heterointerfacial redox chemistry and electrochemical transformation reversibility is investigated. It is demonstrated that the lower redox potential at heterointerface contributes to higher CE, and this enhancement in CE is primarily due to the regulation of redox chemistry to Li deposition behavior rather than the formation of SEI films. Low oxidation potential facilitates the formation of the surface with the highly electrochemical binding feature after Li stripping, and low reduction potential can maintain binding ability well during subsequent Li plating, both of which homogenize Li deposition and thus optimize CE. In particular, Mg hetero-metal with ultra-low redox potential enables Li metal anode with significantly improved CE (99.6%) and stable cycle life for 700 cycles at 3.0 mA cm -2 . This work provides insight into the heterointerfacial design principle of next-generation negative electrodes for highly reversible metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2021

High-Entropy Ceramic Coatings: Transformative New Materials for Environmentally-Compatible Thin-Film Insulators against High-T Molten Salts

An emerging new class of promising materials, High-Entropy Ceramics (HECs) or Compositionally-Complex Ceramics (CCCs), have been successfully fabricated in the last three years. This project evaluates HECs/CCCs in the concentrated solar power (CSP) context. In this project, we have identified a couple of simple, and key descriptors governing thermal conductivity in HECs. Size disorder among the cations was found to have a strong influence on the thermal conductivity across multiple systems and throughout a vast compositional space. Since identifying this, we have optimized previous compositions to achieve low thermal conductivities of $k$~$1-1.4Wm{-1}K{-1}$. We have further reduced our selection of promising compositions based on project guidelines and applied a theory that can potentially predict reactivity with molten salts to identify a small set of HECs that are suitable for further molten salt heat transfer media (HTM) stability testing. Many compositions reveal poor resistance to molten chloride salt after being exposed for 24 h compared to the reference structural alloy, Haynes 230. However, after 100 h, a few HECs/CCCs show strong parabolic rate constant effects and provide greater resistance to chloride salt compared to Haynes 230 alloy, which shows more linear kinetics. Postmortem characterization of the microstructure reveals the parabolic rate constant originates from a dense reaction layer form at the interface. This feature is absent in Haynes 230, which only shows grain boundary infiltration. The HECs/CCCs were also put in contact with the metal alloy under Ar for 800 h at 800°C and show negligible interaction. Lastly, parabolic rate constant HECs/CCCs also have low thermal conductivity $(<2 Wm^{-1} K^{-1})$ at 800°C. These specimens satisfy all project requirements and demonstrate their promising application in next-generation CSP.

14 SOLAR ENERGY↗
NASA NTRS2019

A Multi-Physics Study on High-Specific Power Li-O2 Batteries for Electric Aircraft

Commercialization of lithium-air batteries faces many challenges, such as electrolyte decomposition, short cycle life, low energy and power density, etc. However, commercialization of Li-O2 batteries for aeronautics is much more challenging due to additional safety constraints on cyclability and performance (high specific power and specific energy). For this presentation, we will discuss inter-related aspects of physics-based modeling of a pack: cell and battery model calibration. In addition, we will evaluate and present optimal battery designs for high discharge current density, high discharge time, and low battery mass using simulation-based optimization.The Finite Element Model (FEM) used to simulate a Li-O2 cell is based on the work of Bevara [1]. The different aspects of the model are based on: porous electrode theory and concentrated electrolyte theory; quantum tunneling model for the resistance of conformal layer of discharge product (Li2O2) [1]; Butler-Volmer kinetics for electrochemical reaction; Fick's diffusion for oxygen transport; and an oxygen dissolution model is applied at the air/electrolyte interface [2]. The electrolyte properties such as ion conductivity, ion diffusion, oxygen diffusion, and mass density of the electrolyte were taken from Molecular Dynamics (MD) simulations [3]; while the other model parameters, which includes mass of cell components, were calibrated to match experiments at high discharge current densities. The cell mass includes the anode, cathode, separator, electrolyte, and other components (such as current collector). This calibrated model is used to perform parametric studies on cathode thickness, porosity, tortuosity, carbon particle size, electrolyte transport and material properties, partial pressure of oxygen, discharge time, and discharge current density to study optimal designs for high specific power and energy. References:1. Bevara, V. & Andrei, P. (2014), J. Electrochem. Soc. 161 (14), A2068-A2079.2.Mehta, M. & Andrei, P. (2015), J. Power Sources. 286, 299-308.3.Liyana-Arachchi, T.; Haskins, J.; Burke, C.; Diederichsen, K.; McCloskey, B.; & Lawson, J. (2018), J. Phys. Chem. B. 122 (36), 8548 - 8559.4.Choi, W.; Kikumoto, H.; Choudhary, R. & Ooka, R. (2018), Applied Energy, 209, 306-321.

Mehta, Mohit↗
NASA NTRS2022

The Polstar High Resolution Spectropolarimetry MIDEX Mission

The Polstar mission will provide a space-borne 60 cm spectropolarimeter operating at ultraviolet (UV) wavelengths, capturing all four Stokes parameters (intensity, two linear polarization components, and circular polarization). Polstar’s capabilities are designed to meet its goal of determining how circumstellar gas flows alter and inform massive star evolution, affect the stellar remnant population, and stir and enrich the interstellar medium (ISM). These will be achieved by investigating the dynamical geometries in the winds and disks of hot stars, the composition and magnetic alignment of interstellar dust, and the star-forming accretion disks of UV-bright stars at an important transition boundary. Together these areas map out a kind of two-way interface between massive stars and their effect on our galaxy, wherein the stellar winds enrich the ISM with metals and kinetic energy, preconditioning their environment and the stellar endpoints prior to undergoing supernova. The ISM dust in turn reveals the composition and magnetic environment leading to new star formation, and the accretion disks of Herbig Ae/Be stars reveal how the ISM gas returns to make new massive stars. Polstar will combine high-resolution spectroscopy in the time domain with high-precision UV polarimetry. Doppler-shifted UV resonance line opacity will provide information about circumstellar kinematics, while polarization gives complementary geometric information about unseen structures. The composition and magnetic alignment of the smallest interstellar dust grains provides a probe of the ISM utilizing radiative alignment theory (RAT). Polstar will operate in the far-UV (FUV) at 122–200 nm at high spectral resolution of around R ∼ 30k, and at FUV and near-UV (NUV) wavelengths of 122–320 nm at lower spectral resolutions of 0.1 - 1k. Detection of polarization levels as weak as 0.1% are expected, with a temporal cadence ranging from 5–10 minutes for most wind variability studies, to hours or days for sampling rotation, to days or weeks for sampling binary orbits, to months to a year for sampling substructure in the inner regions of protoplanetary disks. Sub-meter-class aperture is well suited to access this wide array of time domain science, made possible by restricting to a few hundred bright, massive stars, necessarily extincted by a small to moderate column of interstellar dust, informing both the attributes of the stars and the ISM through which they are seen. As such, the focus is on our own galaxy and its evolutionary drivers, but a few targets in the Magellanic clouds offer the potential to extend this understanding to low-metallicity environments.

Paul A Scowen↗
DOE OSTI2018

Does Marine Surface Tension Have Global Biogeography? Addition for the OCEANFILMS Package

We apply principles of Gibbs phase plane chemistry across the entire ocean-atmosphere interface to investigate aerosol generation and geophysical transfer issues. Marine surface tension differences comprise a tangential pressure field controlling trace gas fluxes, primary organic inputs, and sea spray salt injections, in addition to heat and momentum fluxes. Mapping follows from the organic microlayer composition, now represented in ocean system models. Organic functional variations drive the microforcing, leading to (1) reduced turbulence and (by extension) laminar gas-energy diffusion; plus (2) altered bubble film mass emission into the boundary layer. Interfacial chemical behaviors are, therefore, closely reviewed as the background. We focus on phase transitions among two dimensional “solid, liquid, and gaseous” states serving as elasticity indicators. From the pool of dissolved organic carbon (DOC) only proteins and lipids appear to occupy significant atmospheric interfacial areas. The literature suggests albumin and stearic acid as the best proxies, and we distribute them through ecodynamic simulation. Consensus bulk distributions are obtained to control their adsorptive equilibria. We devise parameterizations for both the planar free energy and equation of state, relating excess coverage to the surface pressure and its modulus. Constant settings for the molecular surrogates are drawn from laboratory study and successfully reproduce surfactant solid-to-gas occurrence in compression experiments. Since DOC functionality measurements are rare, we group them into super-ecological province tables to verify aqueous concentration estimates. Outputs are then fed into a coverage, tension, elasticity code. The resulting two dimensional pressure contours cross a critical range for the regulation of precursor piston velocity, bubble breakage, and primary aerosol sources plus ripple damping. Concepts extend the water-air adsorption theory currently embodied in our OCEANFILMS aerosol emissions package, and the two approaches could be inserted into Earth System Models together. Uncertainties in the logic include kinetic and thermochemical factors operating at multiple scales.

54 ENVIRONMENTAL SCIENCES↗