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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 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Sequential Capacitive Deposition of Ionic Liquids for Conformal Thin Film Coatings on Oxygen Reduction Reaction Electrocatalysts

Ionic liquid (IL)-modified carbon-supported catalysts have demonstrated significant improvements in oxygen reduction reaction (ORR) activity. However, transition of this result from the half-cell to the proton exchange membrane fuel cell (PEMFC) has been challenging. Presented here is a processing methodology that yields the formation of a thin (<2 nm) conformal IL coating on the surface of both three-dimensional electrocatalysts and bulk single crystals through the sequential capacitive deposition (SCD) of anionic and cationic components and their subsequent condensation into a hydrophobic, protic IL. In conclusion, SCD shows promise for IL incorporation into preformed PEMFC catalyst layers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

The liquid surface of chiral ionic liquids as seen from molecular dynamics simulations combined with intrinsic analysis

We present molecular-level insight into the liquid/gas interface of two chiral room-temperature ionic liquids (RTILs) derived from 1-n-butyl-3-methylimidazolium bromide ([bmim][Br]); namely, (R)-1-butyl-3-(3-hydroxy-2-methylpropyl)imidazolium bromide (hydroxypropyl) and 1-butyl-3-[(1R)-nopyl]imidazolium bromide (nopyl). We use our currently developed force field which was validated against the experimental bulk density, heat of vaporization, and surface tension of [bmim][Br]. The force field for the RTILs adopts the Chemistry at Harvard Molecular Mechanics (CHARMM) parameters for the intramolecular and repulsion-dispersion interactions along with the reduced partial atomic charges based on ab initio calculations. The net charges of the ions are around ±0.8e, which mimic the anion to cation charge transfer and many-body effects. Molecular dynamics simulations in the slab geometry combined with the intrinsic interface analysis are employed to provide a detailed description of the RTIL/gas interface in terms of the structural and dynamic properties of the interfacial, sub-interfacial, and central layers at a temperature of 300 K. The focus is on the comparison of the liquid/gas interface for the chiral RTILs with the interface for parent [bmim][Br]. The structure of the interface is elucidated by evaluating the surface roughness, intrinsic atomic density profiles, and orientation ordering of the cations. The dynamics of the ions at the interfacial region is characterized by computing the survival probability, and normal and lateral self-diffusion coefficients in the layers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Order-parameter-aided temperature-accelerated sampling for the exploration of crystal polymorphism and solid-liquid phase transitions

The problem of predicting polymorphism in atomic and molecular crystals constitutes a significant challenge both experimentally and theoretically. From the theoretical viewpoint, polymorphism prediction falls into the general class of problems characterized by an underlying rough energy landscape, and consequently, free energy based enhanced sampling approaches can be brought to bear on the problem. In this paper, we build on a scheme previously introduced by two of the authors in which the lengths and angles of the supercell are targeted for enhanced sampling via temperature accelerated adiabatic free energy dynamics [T. Q. Yu and M. E. Tuckerman, Phys. Rev. Lett. 107, 015701 (2011)]. Here, that framework is expanded to include general order parameters that distinguish different crystalline arrangements as target collective variables for enhanced sampling. The resulting free energy surface, being of quite high dimension, is nontrivial to reconstruct, and we discuss one particular strategy for performing the free energy analysis. The method is applied to the study of polymorphism in xenon crystals at high pressure and temperature using the Steinhardt order parameters without and with the supercell included in the set of collective variables. The expected fcc and bcc structures are obtained, and when the supercell parameters are included as collective variables, we also find several new structures, including fcc states with hcp stacking faults. We also apply the new method to the solid-liquid phase transition in copper at 1300 K using the same Steinhardt order parameters. Our method is able to melt and refreeze the system repeatedly, and the free energy profile can be obtained with high efficiency.

36 MATERIALS SCIENCE↗
DOE OSTI2015

IR and SFG vibrational spectroscopy of the water bend in the bulk liquid and at the liquid-vapor interface, respectively

Vibrational spectroscopy of the water bending mode has been investigated experimentally to study the structure of water in condensed phases. In the present work, we calculate the theoretical infrared (IR) and sum-frequency generation (SFG) spectra of the HOH bend in liquid water and at the water liquid/vapor interface using a mixed quantum/classical approach. Classical molecular dynamics simulation is performed by using a recently developed water model that explicitly includes three-body interactions and yields a better description of the water surface. Ab-initio-based transition frequency, dipole, polarizability, and intermolecular coupling maps are developed for the spectral calculations. The calculated IR and SFG spectra show good agreement with the experimental measurements. In the theoretical imaginary part of the SFG susceptibility for the water liquid/vapor interface, we find two features: a negative band centered at 1615 cm{sup −1} and a positive band centered at 1670 cm{sup −1}. We analyze this spectrum in terms of the contributions from molecules in different hydrogen-bond classes to the SFG spectral density and also compare to SFG results for the OH stretch. SFG of the water bending mode provides a complementary picture of the heterogeneous hydrogen-bond configurations at the water surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Tunable meta-atom using liquid metal embedded in stretchable polymer

Reconfigurable metamaterials have great potential to alleviate complications involved in using passive metamaterials to realize emerging electromagnetic functions, such as dynamical filtering, sensing, and cloaking. This paper presents a new type of tunable meta-atoms in the X-band frequency range (8–12 GHz) toward reconfigurable metamaterials. The meta-atom is made of all flexible materials compliant to the surface of an interaction object. It uses a liquid metal-based split-ring resonator as its core constituent embedded in a highly flexible elastomer. We demonstrate that simple mechanical stretching of the meta-atom can lead to the great flexibility in reconfiguring its resonance frequency continuously over more than 70% of the X-band frequency range. The presented meta-atom technique provides a simple approach to dynamically tune response characteristics of metamaterials over a broad frequency range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Site-Specific Structure at Multiple Length Scales in Kagome Quantum Spin Liquid Candidates

Realizing a quantum spin liquid (QSL) ground state in a real material is a leading issue in condensed matter physics research. In this pursuit, it is crucial to fully characterize the structure and influence of defects, as these can significantly affect the fragile QSL physics. In this work, we perform a variety of cutting-edge synchrotron x-ray scattering and spectroscopy techniques, and we advance new methodologies for site-specific diffraction and L-edge Zn absorption spectroscopy. The experimental results along with our first-principles calculations address outstanding questions about the local and long-range structures of the two leading kagome QSL candidates, Zn-substituted barlowite Cu 3 Zn x Cu 1-x (OH) 6 FBr and herbertsmithite Cu 3 Zn(OH) 6 Cl 2 . On all length scales probed, there is no evidence that Zn substitutes onto the kagome layers, thereby preserving the QSL physics of the kagome lattice. Our calculations show that antisite disorder is not energetically favorable and is even less favorable in Zn-barlowite compared to herbertsmithite. Site-specific x-ray diffraction measurements of Zn-barlowite reveal that Cu 2+ and Zn 2+ selectively occupy distinct interlayer sites, in contrast to herbertsmithite. Using the first measured Zn L-edge inelastic x-ray absorption spectra combined with calculations, we discover a systematic correlation between the loss of inversion symmetry from pseudo-octahedral (herbertsmithite) to trigonal prismatic coordination (Zn-barlowite) with the emergence of a new peak. Overall, our measurements suggest that Zn-barlowite has structural advantages over herbertsmithite that make its magnetic properties closer to an ideal QSL candidate: its kagome layers are highly resistant to nonmagnetic defects while the interlayers can accommodate a higher amount of Zn substitution.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Statistical characteristics of cloud variability. Part 1: Retrieved cloud liquid water path at three ARM sites: Observed cloud variability at ARM sites

Statistical characteristics of cloud variability are examined for their dependence on averaging scales and best representation of probability density function with the decade-long retrieval products of cloud liquid water path (LWP) from the tropical western Pacific (TWP), Southern Great Plains (SGP), and North Slope of Alaska (NSA) sites of the Department of Energy’s Atmospheric Radiation Measurement Program. The statistical moments of LWP show some seasonal variation at the SGP and NSA sites but not much at the TWP site. It is found that the standard deviation, relative dispersion (the ratio of the standard deviation to the mean), and skewness all quickly increase with the averaging window size when the window size is small and become more or less flat when the window size exceeds 12 h. On average, the cloud LWP at the TWP site has the largest values of standard deviation, relative dispersion, and skewness, whereas the NSA site exhibits the least. Correlation analysis shows that there is a positive correlation between the mean LWP and the standard deviation. The skewness is found to be closely related to the relative dispersion with a correlation coefficient of 0.6. The comparison further shows that the log normal, Weibull, and gamma distributions reasonably explain the observed relationship between skewness and relative dispersion over a wide range of scales.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

A Rechargeable Al/S Battery with an Ionic‐Liquid Electrolyte

Abstract Aluminum metal is a promising anode material for next generation rechargeable batteries owing to its abundance, potentially dendrite‐free deposition, and high capacity. The rechargeable aluminum/sulfur (Al/S) battery is of great interest owing to its high energy density (1340 Wh kg −1 ) and low cost. However, Al/S chemistry suffers poor reversibility owing to the difficulty of oxidizing AlS x . Herein, we demonstrate the first reversible Al/S battery in ionic‐liquid electrolyte with an activated carbon cloth/sulfur composite cathode. Electrochemical, spectroscopic, and microscopic results suggest that sulfur undergoes a solid‐state conversion reaction in the electrolyte. Kinetics analysis identifies that the slow solid‐state sulfur conversion reaction causes large voltage hysteresis and limits the energy efficiency of the system.

Gao, Tao↗
DOE OSTI2015

Glucose- and Cellulose-Derived Ni/C-SO3H Catalysts for Liquid Phase Phenol Hydrodeoxygenation

Sulfonated carbons were explored as functionalized supports for Ni nanoparticles to hydrodeoxygenate (HDO) phenol. Both hexadecane and water were used as solvents. The dual-functional Ni catalysts supported on sulfonated carbon (Ni/C-SO3H) showed high rates for phenol hydrodeoxygenation in liquid hexadecane, but not in water. Glucose and cellulose were precursors to the carbon supports. Changes in the carbons resulting from sulfonation of the carbons resulted in variations of carbon sheet structures, morphologies and the surface concentrations of acid sites. While the C-SO3H supports were active for cyclohexanol dehydration in hexadecane and water, Ni/C-SO3H only catalyzed the reduction of phenol to cyclohexanol in water. The state of 3 – 5 nm grafted Ni particles was analyzed by in situ X-ray absorption spectroscopy. The results show that the metallic Ni was rapidly formed in situ without detectable leaching to the aqueous phase, suggesting that just the acid functions on Ni/C-SO3H are inhibited in presence of water. Using in situ IR spectroscopy, it was shown that even in hexadecane, phenol HDO is limited by the dehydration step. Thus, phenol HDO catalysis was further improved by physically admixing C-SO3H with the Ni/C-SO3H catalyst to balance the two catalytic functions. The minimum addition of 7 wt.% C-SO3H to the most active of the Ni/C-SO3H catalysts enabled nearly quantitative conversion of phenol and the highest selectivity (90%) towards cyclohexane in 6 h, at temperatures as low as 473 K, suggesting that the proximity to Ni limits the acid properties of the support.

Carbon Support↗
DOE OSTI2018

Time reversal, SU(N) Yang–Mills and cobordisms: Interacting topological superconductors/insulators and quantum spin liquids in 3+1D

We introduce a web of strongly correlated interacting 3+1D topological superconductors/insulators of 10 particular global symmetry groups of Cartan classes, realizable in electronic condensed matter systems, and their new SU(N) generalizations. The symmetries include SU(N), SU(2), U(1), fermion parity, time reversal and relate to each other through symmetry embeddings. We overview the lattice Hamiltonian formalism. We complete the list of field theories of bulk symmetry-protected topological invariants (SPT invariants/partition functions that exhibit boundary ’t Hooft anomalies) via cobordism calculations, matching their full classification. We also present explicit 4-manifolds that detect these SPTs. On the other hand, once we dynamically gauge part of their global symmetries, we arrive in various new phases of SU(N) Yang–Mills (YM) gauge theories, analogous to quantum spin liquids with emergent gauge fields. We discuss how coupling YM theories to time reversal-SPTs affects the strongly coupled theories at low energy. For example, we point out a possibility of having two deconfined gapless time-reversal symmetric SU(2) YM theories at θ=π as two distinct conformal field theories, which although are secretly indistinguishable by correlators of local operators on orientable spacetimes nor by gapped SPT states, can be distinguished on non-orientable spacetimes or potentially by correlators of extended operators.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗