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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 847 records · Page 47
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Calculations of the pH-Dependent Onset Potential for CO Electrooxidation on Au(111)

CO electrooxidation on the Au(111) surface exhibits an onset potential that depends strongly on the pH of the electrolyte. In alkaline solution, the onset potential for CO electrooxidation is found, experimentally, to be 0.5 V lower than in acidic media on the reversible hydrogen electrode scale. This phenomenon is explained here with density functional theory which is used to calculate adsorbate binding energies including the electric double layer of the Au(111)/aqueous interface. Our model consists of a charged Au(111) slab and implicit solvation for the electrolyte. The double reference method is used to determine the potential-dependent CO electrooxidation reaction energetics. A microkinetic model, based upon the calculated reaction energetics, confi rms the lower onset potential in alkaline media. Our results show that there are three factors contributing to the lower onset potential in base: (1) stronger CO adsorption, (2) attraction between adsorbed CO and OH - , and (3) the high concentration of OH - in base.

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

Preparation of a membrane-sealed cell for studying catalyst nanoparticles in flowing gas with high vacuum x-ray photoelectron spectrometer

Here a sealing-style x-ray photoelectron spectroscopy study of the surface of a 1.0 wt. %Ni/TiO2 nanoparticle catalyst in a flowing mixture of CO and O2 at 1 bar was performed with a graphene membrane-sealed Si3N4 window-based miniature cell. We report the details on how a commercial Si3N4 window is modified before assembling a graphene membrane, how single-layer graphene membranes are transferred from their metal supports to the modified Si3N4 window, how a modified Si3N4 window covered with a double-layer graphene membrane is assembled onto a blank cell cap, how a nanoparticle catalyst is introduced to the cell cap and then the cell cap is installed onto a cell body to form a complete reaction cell, and how a complete cell is interfaced with a high vacuum chamber of an XPS system before an XPS study of 1.0 wt. %Ni/TiO2 catalyst surface in a flowing mixture for 0.2 bar CO and 0.8 bar O2 is performed. How the characterization of a catalyst using this type of graphene membrane-sealed Si3N4 window-based miniature cell is relevant to the finding of the actual surface chemistry of a catalyst during catalysis is discussed.

Instruments & Instrumentation↗
DOE OSTI2025

Cleavable quaternary oxychlorides with high magnetic ordering temperatures

Quaternary oxychlorides derived from Ruddlesden–Popper 3d transition metal oxides offer a route to cleavable crystals with bulk antiferromagnetic ordering temperatures reaching at least 550 K. Here, we study the magnetic, optical, and mechanical behavior of Sr 2 FeO 3 Cl, Ca 2 FeO 3 Cl, Ca 3 Fe 2 O 5 Cl 2 , and Sr 3 Fe 2 O 5 Cl 2 . Through optical absorption measurements, we show that these antiferromagnetic semiconductors have optical band gaps of ≈2.1(1) eV. The magnetic ordering symmetries and temperatures were probed by neutron powder diffraction and Mössbauer spectroscopy on polycrystalline samples, demonstrating Néel temperatures (T N ) near room temperature in the single layer Sr 2 FeO 3 Cl (T N ≈ 311 K) and Ca 2 FeO 3 Cl (T N ≈ 360 K), and the double-layer compound Sr 3 Fe 2 O 5 Cl 2 has T N ≈ 545 K. The high-spin moments of Fe 3+ lie within the basal plane and the magnetic structures are compensated within each magnetic layer and characterized by magnetic propagation vectors k = ($\frac{1}{2}$ $\frac{1}{2}$ 0). Magnetization results demonstrate the quasi-2D nature of the magnetism, with a broad maximum in the susceptibility near 2T N for Sr 2 FeO 3 Cl. Scotch tape tests and mechanical exfoliation onto SiO 2 confirm the micaceous nature of these crystals with cleavage down to a single unit cell (two magnetic layers) achieved for Sr 3 Fe 2 O 5 Cl 2 . In conclusion, this paper highlights strong antiferromagnetic interactions, semiconducting band gaps, and cleavability of quaternary Fe-based oxychlorides and motivates future work on crystals and exfoliated flakes of these and related oxyhalide systems.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Superplasticizer to layered calcium aluminate hydrate interface characterized using model organic molecules

Ten organic molecule models simulating the chemical functions of commercial superplasticizers used in the cement/concrete industry were intercalated into lamellar calcium aluminate hydrates to synthesize hybrid AFm phases. AFm phases, encountered in cement hydration chemistry, belong to the large Layered Double Hydroxide (LDH) family. The intercalation process was performed using the anion exchange method. The affinities of the model molecules toward the AFm mineral layers, [Ca{sub 2}Al(OH){sub 6}]{sup +}, were compared using several complementary techniques. They display the following tendencies: –PO{sub 3}{sup 2-} > –SO{sub 3}{sup -} > –CO{sub 2}{sup -} for the hydrophilic parts and heptyl-R > phenyl-R > pentyl-R > ethyl-R for the hydrophobic parts. The organic-inorganic interface of the hybrid AFm phases was achieved. The organic molecule arrangement is either perpendicular or parallel to the inorganic main layer, resulting in various connection modes, from intercalation to grafting. The results enable a better understanding of the chemical reactivity of the utilized superplasticizers during the concrete setting process.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Fluidized bed coupled rotary reactor for nanoparticles coating via atomic layer deposition

A fluidized bed coupled rotary reactor has been designed for coating on nanoparticles (NPs) via atomic layer deposition. It consists of five major parts: reaction chamber, dosing and fluidizing section, pumping section, rotary manipulator components, as well as a double-layer cartridge for the storage of particles. In the deposition procedure, continuous fluidization of particles enlarges and homogenizes the void fraction in the particle bed, while rotation enhances the gas-solid interactions to stabilize fluidization. The particle cartridge presented here enables both the fluidization and rotation acting on the particle bed, demonstrated by the analysis of pressure drop. Moreover, enlarged interstitials and intense gas–solid contact under sufficient fluidizing velocity and proper rotation speed facilitate the precursor delivery throughout the particle bed and consequently provide a fast coating process. The cartridge can ensure precursors flowing through the particle bed exclusively to achieve high utilization without static exposure operation. By optimizing superficial gas velocities and rotation speeds, minimum pulse time for complete coating has been shortened in experiment, and in situ mass spectrometry showed the precursor usage can reach 90%. Inductively coupled plasma-optical emission spectroscopy results suggested a saturated growth of nanoscale Al{sub 2}O{sub 3} films on spherical SiO{sub 2} NPs. Finally, the uniformity and composition of the shells were characterized by high angle annular dark field-transmission electron microscopy and energy dispersive X-ray spectroscopy.

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

The Origin of Improved Performance in Boron‐Alloyed Silicon Nanoparticle‐Based Anodes for Lithium‐Ion Batteries

Stabilizing the solid electrolyte interphase (SEI) remains a key challenge for silicon‐based lithium‐ion battery anodes. Alloying silicon with secondary elements like boron has emerged as a promising strategy to improve the cycle life of silicon anodes, yet the underlying mechanism remains unclear. To address this knowledge gap, how boron concentration influences battery performance is systematically investigated. These results show a near‐monotonic increase in cycle lifetime with higher boron content, with boron‐rich electrodes significantly outperforming pure silicon. Additionally, silicon‐boron alloy anodes exhibit nearly three times longer calendar life than pure silicon. Through detailed mechanistic analysis, alternative contributing factors are systematically ruled out, and it is proposed that improved passivation arises from a strong permanent dipole at the nanoparticle surface. This dipole, formed by undercoordinated and highly Lewis acidic boron, creates a static, ion‐dense layer that stabilizes the electrochemical interface, reducing parasitic electrolyte decomposition and enhancing long‐term stability. These findings suggest that, within the SEI framework, the electric double layer is an important consideration in surface passivation. This insight provides an underexplored parameter space for optimizing silicon anodes in next‐generation lithium‐ion batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Macroscale and Nanoscale Photoelectrochemical Behavior of p-Type Si(111) Covered by a Single Layer of Graphene or Hexagonal Boron Nitride

Two-dimensional (2D) materials may enable a general approach to the introduction of a dipole at a semiconductor surface as well as control over other properties of the double layer at a semiconductor/liquid interface. Vastly different properties can be found in the 2D materials currently studied due in part to the range of the distribution of density-of-states. In this work, the open-circuit voltage (V oc ) of p-Si–H, p-Si/Gr (graphene), and p-Si/h-BN (hexagonal boron nitride) in contact with a series of one-electron outer-sphere redox couples was investigated by macroscale measurements as well as by scanning electrochemical cell microscopy (SECCM). The band gaps of Gr and h-BN (0–5.97 eV) encompass the wide range of band gaps for 2D materials, so these interfaces (p-Si/Gr and p-Si/h-BN) serve as useful references to understand the behavior of 2D materials more generally. The value of Voc shifted with respect to the effective potential of the contacting solution, with slopes (ΔV oc /ΔE Eff ) of -0.27 and -0.38 for p-Si/Gr and p-Si/h-BN, respectively, indicating that band bending at the p-Si/h-BN and p-Si/Gr interfaces responds at least partially to changes in the electrochemical potential of the contacting liquid electrolyte. Additionally, SECCM is shown to be an effective method to interrogate the nanoscale photoelectrochemical behavior of an interface, showing little spatial variance over scales exceeding the grain size of the CVD-grown 2D materials in this work. The measurements demonstrated that the polycrystalline nature of the 2D materials had little effect on the results and confirmed that the macroscale measurements reflected the junction behavior at the nanoscale.

2D material↗
NASA NTRS1990

Development of a unique laboratory standard indium gallium arsenide detector for the 500 to 1700 micron spectral region, phase 2

In the course of this work, 5 mm diameter InGaAs pin detectors were produced which met or exceeded all of the goals of the program. The best results achieved were: shunt resistance of over 300 K ohms; rise time of less than 300 ns; contact resistance of less than 20 ohms; quantum efficiency of over 50 percent in the 0.5 to 1.7 micron range; and devices were maintained and operated at 125 C without deterioration for over 100 hours. In order to achieve the goals of this program, several major technological advances were realized, among them: successful design, construction and operation of a hydride VPE reactor capable of growing epitaxial layers on 2 inch diameter InP substrates with a capacity of over 8 wafers per day; wafer processing was upgraded to handle 2 inch wafers; a double layer Si3N4/SiO2 antireflection coating which enhances response over the 0.5 to 1.7 micron range was developed; a method for anisotropic, precisely controlled CH4/H2 plasma etching for enhancement of response at short wavelengths was developed; and electronic and optical testing methods were developed to allow full characterization of detectors with size and spectral response characteristics. On the basis of the work and results achieved in this program, it is concluded that large size, high shunt resistance, high quantum efficiency InGaAs pin detectors are not only feasible but also manufacturable on industrial scale. This device spans a significant portion of visible and near infrared spectral range and it will allow a single detector to be used for the 0.5 to 1.7 micron spectral region, rather than the presently used silicon (for 0.5 to 1.1 microns) and germanium (0.8 to 1.7 microns).

Ban, Vladimir S.↗
DOE OSTI2014

The dynamic behavior of thin-film ionic transition metal complex-based light-emitting electrochemical cells

Light-emitting electrochemical cells (LECs) have received increasing attention during recent years due to their simple architecture, based on solely air-stabile materials, and ease of manufacture in ambient atmosphere, using solution-based technologies. The LEC's active layer offers semiconducting, luminescent as well as ionic functionality resulting in device physical processes fundamentally different as compared with organic light-emitting diodes. During operation, electrical double layers (EDLs) form at the electrode interfaces as a consequence of ion accumulation and electrochemical doping sets in leading to the in situ development of a light-emitting p-i-n junction. In this paper, we comment on the use of impedance spectroscopy in combination with complex nonlinear squares fitting to derive key information about the latter events in thin-film ionic transition metal complex-based light-emitting electrochemical cells based on the model compound bis-2-phenylpyridine 6-phenyl-2,2´-bipyridine iridium(III) hexafluoridophosphate ([Ir(ppy)₂(pbpy)][PF₆]). At operating voltages below the bandgap potential of the ionic complex used, we obtain the dielectric constant of the active layer, the conductivity of mobile ions, the transference numbers of electrons and ions, and the thickness of the EDLs, whereas the transient thickness of the p-i-n junction is determined at voltages above the bandgap potential. Most importantly, we find that charge transport is dominated by the ions when carrier injection from the electrodes is prohibited, that ion movement is limited by the presence of transverse internal interfaces and that the width of the intrinsic region constitutes almost 60% of the total active layer thickness in steady state at a low operating voltage.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Electrical conduction of LiF interlayers in organic diodes

An interlayer of LiF in between a metal and an organic semiconductor is commonly used to improve the electron injection. Here, we investigate the effect of moderate bias voltages on the electrical properties of Al/LiF/poly(spirofluorene)/Ba/Al diodes by systematically varying the thickness of the LiF layer (2-50 nm). Application of forward bias V below the bandgap of LiF (V < E{sub g} ∼ 14 V) results in reversible formation of an electrical double layer at the LiF/poly(spirofluorene) hetero-junction. Electrons are trapped on the poly(spirofluorene) side of the junction, while positively charged defects accumulate in the LiF with number densities as high as 10{sup 25}/m{sup 3}. Optoelectronic measurements confirm the built-up of aggregated, ionized F centres in the LiF as the positive trapped charges. The charged defects result in efficient transport of electrons from the polymer across the LiF, with current densities that are practically independent of the thickness of the LiF layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1984

High Curie temperature drive layer materials for ion-implanted magnetic bubble devices

Ion implantation of bubble garnets can lower the Curie temperature by 70 C or more, thus limiting high temperature operation of devices with ion-implanted propagation patterns. Therefore, double-layer materials were made with a conventional 2-micron bubble storage layer capped by an ion-implantable drive layer of high Curie temperature, high magnetostriction material. Contiguous disk test patterns were implanted with varying doses of a typical triple implant. Quality of propagation was judged by quasistatic tests on 8-micron period major and minor loops. Variations of magnetization, uniaxial anisotropy, implant dose, and magnetostriction were investigated to ensure optimum flux matching, good charged wall coupling, and wide operating margins. The most successful drive layer compositions were in the systems (SmDyLuCa)3(FeSi)5O12 and (BiGdTmCa)3(FeSi)5O12 and had Curie temperatures 25-44 C higher than the storage layers.

Fratello, V. J.↗
DOE OSTI2019

Quinary Defect-Rich Ultrathin Bimetal Hydroxide Nanosheets for Water Oxidation

The electronic structure of layered double hydroxides (LDHs) can be modulated by heteroatom doping and creating vacancies. The number of exposed active sites can be enriched by exfoliating the bulk structure into fewer layers. Herein, we successfully achieved multielement doping and exfoliation for Co 3 Fe LDHs by one SF 6 -plasma etching step at room temperature (named as Co 3 Fe LDHs-SF 6 ). The obtained Co 3 Fe LDHs-SF 6 ultrathin nanosheets display outstanding oxygen evolution reaction (OER) activity, which only needs 268 mV overpotential to reach 10 mA cm –2 . Tafel slope and charge transfer resistance are dramatically decreased indicating a faster reaction kinetic rate. Lastly, the excellent OER activity can be attributed to an increased number of active sites and an optimized electronic structure modulated by the incorporation of electron-withdrawing F, electron-donating S, and abundant vacancies resulting in proper adsorption energy to oxygen species.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Onset of normal and inverse homoclinic bifurcation in a double plasma system near a plasma fireball

Plasma fireballs are generated due to a localized discharge and appear as a luminous glow with a sharp boundary, which suggests the presence of a localized electric field such as electrical sheath or double layer structure. The present work reports the observation of normal and inverse homoclinic bifurcation phenomena in plasma oscillations that are excited in the presence of fireball in a double plasma device. The controlling parameters for these observations are the ratio of target to source chamber (n{sub T}/n{sub S}) densities and applied electrode voltage. Homoclinic bifurcation is noticed in the plasma potential fluctuations as the system evolves from narrow to long time period oscillations and vice versa with the change of control parameter. The dynamical transition in plasma fireball is demonstrated by spectral analysis, recurrence quantification analysis (RQA), and statistical measures, viz., skewness and kurtosis. The increasing trend of normalized variance reflects that enhancing n{sub T}/n{sub S} induces irregularity in plasma dynamics. The exponential growth of the time period is strongly indicative of homoclinic bifurcation in the system. The gradual decrease of skewness and increase of kurtosis with the increase of n{sub T}/n{sub S} also reflect growing complexity in the system. The visual change of recurrence plot and gradual enhancement of RQA variables DET, L{sub max}, and ENT reflects the bifurcation behavior in the dynamics. The combination of RQA and spectral analysis is a clear evidence that homoclinic bifurcation occurs due to the presence of plasma fireball with different density ratios. However, inverse bifurcation takes place due to the change of fireball voltage. Some of the features observed in the experiment are consistent with a model that describes the dynamics of ionization instabilities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Dopant Sensitive Electrolytic Etching of Germanium with High Selectivity

Abstract The enhanced charge carrier mobility and photon absorption compared to silicon make germanium attractive for next-generation photo diodes. However, the complex oxidation behavior of germanium challenges dopant-dependent selective etching that is desired for the fabrication of backside imaging architectures. This report demonstrates electrolytic wet etching of p-doped germanium which proceeds up to 17,500x faster than etching of intrinsic germanium. Homoepitaxially grown layers of germanium were electrolytically etched in potassium hydroxide over a range of biases. Intermittent acquisition of cyclic voltammetry spectra during etching has suppressed the formation of electric double layers, maintained appreciable etch rates, and allowed for in operando process control. The observed etch rates scaled with dopant concentration. An effective etch rate of germanium removal of 2.100±0.044 µm/min was accomplished for a boron dopant concentration of 6E18cm-3. For nominally intrinsic germanium, however, an effective etch rate of only 0.00012±0.00011 µm/min was observed. A series of systematic electrolytic etch experiments have revealed the transfer of 4 electrons per germanium atom removed.

Wood, Joseph G.↗
NASA NTRS1994

Feasibility study of superconducting LSM rocket launcher system

A feasibility study is presented concerning an application of a superconducting linear synchronous motor (LSM) to a large-scale rocket launcher, whose acceleration guide tube of LSM armature windings is constructed 1,500 meters under the ground. The rocket is released from the linear launcher just after it gets to a peak speed of about 900 kilometers per hour, and it flies out of the guide tube to obtain the speed of 700 kilometers per hour at the height of 100 meters above ground. The linear launcher is brought to a stop at the ground surface for a very short time of 5 seconds by a quick control of deceleration. Very large current variations in the single-layer windings of the LSM armature, which are produced at the higher speed region of 600 to 900 kilometers per hour, are controlled successfully by adopting the double-layer windings. The proposed control method makes the rocket launcher ascend stably in the superconducting LSM system, controlling the Coriolis force.

Yoshida, Kinjiro↗
DOE OSTI2026

A nanoporous capacitive electrochemical ratchet for continuous ion separations

Directed ion transport in liquid electrolyte solutions underlies many phenomena in natural and industrial settings. While nature has evolved structures that drive continuous ion flow without Faradaic redox reactions, establishing this process in synthetic systems has been challenging. Here, in this study, we report an ion pump that drives aqueous ions against a force using a capacitive ratchet mechanism independent of redox reactions. Modulation of an electric potential between thin metallic layers on either face of a nanoporous alumina wafer immersed in solution results in persistent voltages and ionic currents. This occurs due to the nonlinear capacitive nature of electric double layers, whose repeated charging and discharging sustains a continuous ion flux. Using this approach, we demonstrate ratchet-driven electrodialysis that reaches a 50% decrease in the conductivity of the solution in a dilution cell. These ratchet-based ion pumps can enable continuous desalination and selective ion separation using an electrically powered device with no moving parts.

Kautz, Rylan [University of California, Irvine, CA↗
DOE OSTI2017

Structural Differentiation between Layered Single (Ni) and Double Metal Hydroxides (Ni–Al LDHs) Using Wavelet Transformation

Layered double hydroxides (LDHs) are anionic clays important in disciplines such as environmental chemistry, geochemistry, and materials science. Developments in signal processing of extended X-ray absorption fine structure (EXAFS) data, such as wavelet transformation (WT), have been used to identify transition metals and Al present in the hydroxide sheets of LDHs. The WT plots of LDHs should be distinct from those of isostructural single metal hydroxides. However, no direct comparison of these minerals appears in the literature using WT. This work systematically analyzes a suite of Ni-rich mineral standards, including Ni–Al LDHs, single metal Ni hydroxides, and Ni-rich silicates using WT. The results illustrate that the WT plots for α-Ni(OH)2 and Ni–Al LDHs are often indistinguishable from each other, with similar two-component plots for the different mineral types. This demonstrates that the WT of the first metal shell often cannot be used to differentiate an LDH from a single metal hydroxide. Interlayer anions adsorbed to the hydroxide sheet of α-Ni(OH)2 affect the EXAFS spectra and are not visible in the FT but are clearly resolved and discrete in the WT.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Purely electronic mechanism of electrolyte gating of indium tin oxide thin films

Epitaxial indium tin oxide films have been grown on both LaAlO 3 and yttria-stabilized zirconia substrates using RF magnetron sputtering. Electrolyte gating causes a large change in the film resistance that occurs immediately after the gate voltage is applied, and shows no hysteresis during the charging/discharging processes. When two devices are patterned next to one another and the first one gated through an electrolyte, the second one shows no changes in conductance, in contrast to what happens in materials (like tungsten oxide) susceptible to ionic electromigration and intercalation. These findings indicate that electrolyte gating in indium tin oxide triggers a pure electronic process (electron depletion or accumulation, depending on the polarity of the gate voltage), with no electrochemical reactions involved. Electron accumulation occurs in a very thin layer near the film surface, which becomes highly conductive. These results contribute to our understanding of the electrolyte gating mechanism in complex oxides and may be relevant for applications of electric double layer transistor devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗