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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Vacancy Mediated Electrooxidation of 5‐Hydroxymethyl Furfuryl Using Defect Engineered Layered Double Hydroxide Electrocatalysts

Abstract Electrochemical biomass oxidation coupled with hydrogen evolution offers a promising route to generate value‐added chemicals and clean energy. The complex adsorption behavior of 5‐hydroxymethyl furfural (HMF) and hydroxyl ions (OH − ) on the electrocatalyst surface during HMF electrooxidation reaction (HMFOR) necessitates an in‐depth understanding of active sites available for adsorption. Herein, oxygen vacancy (V O ) defects are introduced in NiFe layered double hydroxide (LDH) using Ce dopants to manipulate electronic structure. Synchrotron‐based HE‐XRD and XAS indicate negligible V O in La‐doped NiFe while Ce doping leads to V O defects due to flexible Ce redox (Ce 3+ ↔ Ce 4+ ). The V O ‐rich Ce‐NiFe exhibits higher Faradic efficiency of ≈90% to produce 2,5‐furan dicarboxylic acid (FDCA), far greater than ≈60% for NiFe V O in Ce‐NiFe act as alternative active sites for OH − adsorption, hence reducing adsorption competition for the same metal sites. DFT calculation results corroborate experimental findings by showcasing that the presence of V O in Ce‐NiFe manipulates the adsorption energies and facilitates the chemical adsorption OH − in V O to improve HMFOR. In situ HE‐XRD derived pair distribution function coupled to RMC simulations confirm OH − trapping in V O and HMF adsorption on metal centers as evident by interlayer distance evolution. Taken together, this work showcases routes for dual‐site electrocatalyst design for improved biomass electrooxidation.

Chemistry↗
NASA NTRS1976

The Skylab barium plasma injection experiments. II - Evidence for a double layer

Television observations of a barium-plasma flux tube extending from near 4500 km to near 10,000 km during a magnetic substorm and dawn-sector auroral display indicated several interesting anomalous events. Beyond 5500 km, there was a rapid increase in brightness accompanied by flux-tube splitting and diffusion, leaving behind a truncated single flux tube. From the orientation of the flux tube compared with theoretical field models, the presence of a substantial field-aligned current sheet is deduced. A suggested explanation of these phenomena is given in terms of a plasma potential double layer.

Wescott, E. M.↗
NASA NTRS2000

Concentration of simple aldehydes by sulfite-containing double-layer hydroxide minerals: implications for biopoesis

Environmental conditions play an important role in conceptual studies of prebiotically relevant chemical reactions that could have led to functional biomolecules. The necessary source compounds are likely to have been present in dilute solution, raising the question of how to achieve selective concentration and to reach activation. With the assumption of an initial 'RNA World', the questions of production, concentration, and interaction of aldehydes and aldehyde phosphates, potential precursors of sugar phosphates, come into the foreground. As a possible concentration process for simple, uncharged aldehydes, we investigated their adduct formation with sulfite ion bound in the interlayer of positively charged expanding-sheet-structure double-layer hydroxide minerals. Minerals of this type, initially with chloride as interlayer counter anion, have previously been shown to induce concentration and subsequent aldolization of aldehyde phosphates to form tetrose, pentose, and hexose phosphates. The reversible uptake of the simple aldehydes formaldehyde, glycolaldehyde, and glyceraldehyde by adduct formation with the immobilized sulfite ions is characterized by equilibrium constants of K=1.5, 9, and 11, respectively. This translates into an observable uptake at concentrations exceeding 50 mM.

NASA Discipline Exobiology↗
NASA NTRS1990

Double layers in contactor plasmas

The concept of using a hollow cathode to establish a low impedance contact between a spacecraft and the ambient plasma continues to gain in popularity, and is often then referred to as a plasma contactor. A growing number of studies indicate that large contact currents can be supported with small potential difference between the contactor and the ambient plasma. Results will be presented from a simple one-dimensional spherical model that obtains potentials from the solution of Poisson's equation, and particle densities from a turning point formalism that includes particle angular momentum. The neglect of collisions and magnetic field limits the realism. However, the results illustrate the effect of double layers that can form at the interface between contactor and ambient plasmas, when there is any voltage differential between the contactor and the ambient. The I-V characteristic of this model shows the usual space charge depends upon collection when the contactor flux is lower than some threshold; independence of I from variation in V when the flux is slightly greater than that threshold, and (numerical ?) instability for excessive flux suggesting the possibility of negative resistance. Even if a real I-V characteristic does not exhibit negative resistance, flat spots or high resistance regions may still be troublesome (or useful) to the total circuit.

Cooke, David L.↗
NASA NTRS1987

Some aspects of double layer formation in a plasma constrained by a magnetic mirror

The shift from wave-generated anomalous resistivity toward the more large-scale effects of magnetic confinement of current carrying plasmas was inspired by the more extensive data on auroral particle distribution functions that were made available, data that may often seem consistent with a dissipation-free acceleration of auroral electrons over an extended altitude range. Efforts to interpret these data have brought new vigor to the concept that a smooth and static electric field can be self-consistently generated by suitable pitch angle anisotropies among the high altitude particle populations, different for electrons and ions, and that such an electric field is both necessary and sufficient to maintain the plasma in a quasi-neutral steady state. Certain aspects of this concept are reviewed and criticized, both from a general theoretical standpoint and from the standpoint of what is known about the magnetospheric environment. It is argued that this concept has flaws and that the actual physical problem is considerably more complicated, requiring a more complex electric field, possibly including double layer structures.

Lennartsson, W.↗
DOE OSTI2023

Toggling Stereochemical Activity through Interstitial Positioning of Cations between 2D V 2 O 5 Double Layers

The 5/6s 2 lone-pair electrons of p-block cations in their lower oxidation states are a versatile electronic and geometric structure motif that can underpin lattice anharmonicity and often engender electronic and structural instabilities that underpin the function of active elements in nonlinear optics, thermochromics, thermoelectrics, neuromorphic computing, and photocatalysis. In contrast to periodic solids where lone-pair-bearing cations are part of the structural framework, installing lone-pair-bearing cations in the interstitial sites of intercalation hosts provides a means of a systematically modulating electronic structure through the choice of the group and the period of the inserted cation while preserving the overall framework connectivity. The extent of stereochemical activity and the energy positioning of lone-pair-derived mid-gap states depend on the cation identity, stoichiometry, and strength of anion hybridization. V 2 O 5 polymorphs are versatile insertion hosts that can accommodate a broad range of s-, p-, and d-block cations. However, the insertion of lone-pair-bearing cations remains largely underexplored. In this article, we examine the implications of varying the 6s 2 cations situated in interlayer sites between condensed [V 4 O 10 ] n double layers. Systematic modulations of lattice distortions, electronic structure, and magnetic ordering are observed with increasing strength of stereochemical activity from group 12 to group 14 cations. We compare and contrast p-block-layered M x V 2 O 5 (M = Hg, Tl, and Pb) compounds and map the significance of local off-centering arising from the stereochemical activity of lone-pair cations to the emergence of filled antibonding lone-pair 6s 2 –O 2p-hybridized mid-gap states mediated by second-order Jahn–Teller distortions. Crystallographic studies of cation coordination environments and the resulting modulation of V–V interactions have been used in conjunction with variable-energy hard X-ray photoelectron spectroscopy measurements, first-principles electronic structure calculations, and crystal orbital Hamilton population analyses to decipher the origins of stereochemical activity. Magnetic susceptibility measurements reveal antiferromagnetic signatures for all the three compounds. However, the differences in V–V interactions significantly affect the energy balance of the superexchange interactions, resulting in an ordering temperature of 160 and 260 K for Hg 0.5 V 2 O 5 and δ-Tl 0.5 V 2 O 5 , respectively, as compared to 7 K for δ-Pb 0.5 V 2 O 5 . In δ-Pb 0.5 V 2 O 5 , the strong stereochemical activity of electron lone pairs and the resulting electrostatic repulsions enforce superlattice ordering, which strongly modifies the electronic localization patterns along the [V 4 O 10 ] slabs, resulting in disrupted magnetic ordering and an anomalously low ordering temperature. The results demonstrate a versatile strategy for toggling the stereochemical activity of electron lone pairs to modify the electronic structure near the Fermi level and to mediate superexchange interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1981

Ion-cyclotron turbulence and diagonal double layers in a magnetospheric plasma

A survey of current concepts regarding electrostatic ion-cyclotron turbulence (theory and experiment), and regarding inclined double potential layers in the magnetospheric plasma is presented. Anomalous resistance governed by electrostatic ion-cyclotron turbulence, and one-dimensional and two-dimensional models of double electrostatic layers in the magnetospheric plasma are examined.

Liperovskiy, V. A.↗
DOE OSTI2021

Hollow nanoparticles with hybrid double layers

The present invention discloses the morphology of hollow, double-shelled submicrometer particles generated through a rapid aerosol-based process. The inner shell is an essentially hydrophobic carbon layer of nanoscale dimension (5-20 nm), and the outer shell is a hydrophilic silica layer of approximately 5-40 nm, with the shell thickness being a function of the particle size. The particles are synthesized by exploiting concepts of salt bridging to lock in a surfactant (CTAB) and carbon precursors together with iron species in the interior of a droplet. This deliberate negation of surfactant templating allows a silica shell to form extremely rapidly, sealing in the organic species in the particle interior. Subsequent pyrolysis results in a buildup of internal pressure, forcing carbonaceous species against the silica wall to form an inner shell of carbon. The incorporation of magnetic iron oxide into the shells opens up applications in external stimuli-responsive nanomaterials.

John, Vijay T.↗
NASA NTRS1994

Double layer hydroxide minerals as host structures for bioorganic molecules

A central problem in molecular evolution concerns the selective concentration from dilute, multicomponent solution of source molecules into a reactive environment, where formation of larger molecular assemblages can take place. Minerals consisting of positively charged, separable metal hydroxide sheets have proven capable of these functions. This common structural type is represented by minerals such as pyroaurite (Mg-Fe(3+) hydroxide), hydrotalcite (Mg-Al), green rust Fe(2+)-Fe(3+) and others. Effective interlayer sorption is demonstrated for orthophosphate and condensed phosphates, anionic alkyl compounds, polypeptides, nucleic acids, cyanide complexes and glycolaldehyde phosphate, the latter shown to readily oligomerize to form and selectively retain racemic hexose -2, 4, 6-phosphates, preferentially of altrose (Pitsch, et al, 1993). The selective aldomerization and retention effects correlate with the charge distribution in the host mineral structure and the stereochemistry of the substrate molecules. Interaction between nucleic acid bases, and between the cyanide groups of glycolaldehyde phosphate nitrile at the low water activity in the mineral interlayer is indicated by doubling of the monomeric separation of the hydroxide mineral sheets.

Lee, Ton↗
DOE OSTI2020

Tensor network investigation of the double layer Kagome compound Ca 10 Cr 7 O 28

Quantum spin liquids are exotic quantum phases of matter that do not order even at zero temperature. While there are several toy models and simple Hamiltonians that could host a quantum spin liquid as their ground state, it is very rare to find actual, realistic materials that exhibit their properties. At the same time, the classical simulation of such instances of strongly correlated systems is intricate and reliable methods are scarce. Here, in this work, we investigate the quantum magnet Ca 10 Cr 7 O 28 that has recently been discovered to exhibit properties of a quantum spin liquid in inelastic neutron scattering experiments. This compound has a distorted bilayer Kagome lattice crystal structure consisting of Cr 5+ ions with spin- moments. Coincidentally, the lattice structure renders a tensor network algorithm in 2D applicable that can be seen as a new variant of a projected entangled simplex state algorithm in the thermodynamic limit. In this first numerical investigation of this material that takes into account genuine quantum correlations, good agreement with the experimental findings is found. Our study contributes to uplifting tensor networks from conceptual tools to methods to describe real two-dimensional quantum materials.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗