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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Surface photovoltage spectroscopy observes junctions and carrier separation in gallium nitride nanowire arrays for overall water-splitting

Gallium nitride (GaN) nanowire arrays on silicon are able to drive the overall water-splitting reaction with up to 3.3% solar-to-hydrogen efficiency. Photochemical charge separation is key to the operation of these devices, but details are difficult to observe experimentally because of the number of components and interfaces. Here, we use surface photovoltage spectroscopy to study charge transfer in i-, n-, and p-GaN nanowire arrays on n+ -Si wafers in the presence and absence of Rh/Cr 2 O 3 co-catalysts. The effect of the space charge layer and sub-bandgap defects on majority and minority carrier transport can be clearly observed, and estimates of the built-in potential of the junctions can be made. Transient illumination of the p-GaN/n + -Si junction generates up to -1.4 V surface photovoltage by carrier separation along the GaN nanowire axis. This process is central to the overall water-splitting function of the n + -Si/p-GaN/Rh/Cr 2 O 3 nanowire array. Overall, these results improve our understanding of photochemical charge transfer and separation in group III–V semiconductor nanostructures for the conversion of solar energy into fuels.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Sustainable chemistry with plasmonic photocatalysts

There is a pressing global need to increase the use of renewable energy sources and limit greenhouse gas emissions. Towards this goal, highly efficient and molecularly selective chemical processes that operate under mild conditions are critical. Plasmonic photocatalysis uses optically resonant metallic nanoparticles and their resulting plasmonic, electronic, and phononic light-matter interactions to drive chemical reactions. The promise of simultaneous high-efficiency and product-selective reactions with plasmon photocatalysis provides a compelling opportunity to rethink how chemistry is achieved. Plasmonic nanoparticles serve as nanoscale ‘antennas’ that enable strong light–matter interactions, surpassing the light-harvesting capabilities one would expect purely from their size. Complex composite structures, combining engineered light harvesters with more chemically active components, are a focal point of current research endeavors. In this review, we provide an overview of recent advances in plasmonic catalysis. We start with a discussion of the relevant mechanisms in photochemical transformations and explain hot-carrier generation and distributions from several ubiquitous plasmonic antennae. Then we highlight three important types of catalytic processes for sustainable chemistry: ammonia synthesis, hydrogen production and CO 2 reduction. To help elucidate the reaction mechanism, both state-of-art electromagnetic calculations and quantum mechanistic calculations are discussed. This review provides insights to better understand the mechanism of plasmonic photocatalysis with a variety of metallic and composite nanostructures toward designing and controlling improved platforms for green chemistry in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Chemical manipulation of hydrogen induced high p-type and n-type conductivity in Ga 2 O 3

Advancement of optoelectronic and high-power devices is tied to the development of wide band gap materials with excellent transport properties. However, bipolar doping (n-type and p-type doping) and realizing high carrier density while maintaining good mobility have been big challenges in wide band gap materials. Here P-type and n-type conductivity was introduced in β-Ga 2 O 3 , an ultra-wide band gap oxide, by controlling hydrogen incorporation in the lattice without further doping. Hydrogen induced a 9-order of magnitude increase of n-type conductivity with donor ionization energy of 20 meV and resistivity of 10 -4 Ω.cm. The conductivity was switched to p-type with acceptor ionization energy of 42 meV by altering hydrogen incorporation in the lattice. Density functional theory calculations were used to examine hydrogen location in the Ga 2 O 3 lattice and identified a new donor type as the source of this remarkable n-type conductivity. Positron annihilation spectroscopy measurements confirm this finding and the interpretation of the experimental results. This work illustrates a new approach that allows a tunable and reversible way of modifying the conductivity of semiconductors and it is expected to have profound implications on semiconductor field. At the same time, it demonstrates for the first time p-type and remarkable n-type conductivity in Ga 2 O 3 which should usher in the development of Ga 2 O 3 devices and advance optoelectronics and high-power devices.

36 MATERIALS SCIENCE↗
NASA NTRS2011

Messengers from the Early Solar System - Comets as Carriers of Cosmic Information

Viewed from a cosmic perspective, Earth is a dry planet yet its oceans are enriched in deuterium by a large factor relative to nebular hydrogen. Can comets have delivered Earth s water? The question of exogenous delivery of water and organics to Earth and other young planets is of critical importance for understanding the origin of Earth s water, and for assessing the possible existence of exo-planets similar to Earth. Strong gradients in temperature and chemistry in the proto-planetary disk, coupled with dynamical models, imply that comets from the Oort Cloud and Kuiper Disk reservoirs should have diverse composition. The primary volatiles in comets (ices native to the nucleus) provide the preferred metric, and taxonomies based on them are now beginning to emerge [1, 2, 3]. The measurement of cosmic parameters such as the nuclear spin temperatures for H2O, NH3, and CH4, and of enrichment factors for isotopologues (D/H in water and hydrogen cyanide, N-14/N-15 in CN and hydrogen cyanide) provide additional important tests for the origin of cometary material.

Mumma, Michael J.↗
DOE OSTI2022

LaNi x Fe 1–x O 3 as flexible oxygen or carbon carriers for tunable syngas production and CO 2 utilization

The current study reports LaFe 1–x Ni x O 3–δ redox catalysts as flexible oxygen or carbon carriers for CO2 utilization and tunable production of syngas at relatively low temperatures (~700 °C), in the context of a hybrid redox process. Specifically, perovskite-structured LaFe 1–x Ni x O 3–δ with seven different compositions (x = 0.4–1) were prepared and investigated. Cyclic experiments under alternating methane and CO 2 flows indicated that all the samples exhibited favorable reactive performance: CH 4 and CO 2 conversions varied between 85% and 98% and 70–88%, respectively. While H 2 /CO ratio from Fe-rich redox catalysts was ~2.3:1 in the methane conversion step, Ni-rich catalysts produced a concentrated (~ 93.7 vol%) hydrogen stream via methane cracking. The flexibility of LaFe 1–x Ni x O 3–δ to produce syngas (or hydrogen) with tunable compositions was found to be governed by the iron/nickel (Fe/Ni) ratio. Redox catalysts with higher Fe contents act as a lattice oxygen carrier via chemical looping partial oxidation (CLPOx) of methane whereas those with higher Ni contents function as a carbon carrier via chemical looping methane cracking (CLMC) scheme. XRD analysis and temperature-programmed reactions revealed that both types of catalysts involve the formation of La 2 O 3 and Ni 0 /Ni-Fe phases under the methane environment. The ability to re-incorporate La 2 O 3 and Ni/Fe into a perovskite structure gives rise to oxygen-carrying capacity whereas stable Ni 0 or Ni/Fe phases would catalyze methane cracking without lattice oxygen exchange in the reaction cycles. Here, temperature programmed oxidation and Raman spectroscopy indicated the presence of graphitic and amorphous carbon species, which were effectively gasified by CO 2 to produce concentrated CO. Stability tests over LaFe 0.5 Ni 0.5 O 3 and LaNiO 3 revealed that the redox performance was stable over a span of 50 cycles.

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

Enhancement to the conductivity of surface transfer-doped (111) diamond through thermochemical surface etching

The use of a transition metal catalyzed thermochemical etching method for improving the carrier transport properties of the near-surface two-dimensional (2D) hole gas in surface transfer-doped hydrogen-terminated (111) diamond is demonstrated. Using Ni 0.8 Cr 0.2 films deposited and annealed to a temperature of 900 °C, with up to three etch cycles, preferential (111) surface etching produces large terraces exceeding 10 μm in size with a surface microroughness, σ 2 RMS λ, that is two orders of magnitude lower than for the pre-etched (111) surface. Magnetotransport measurements on hydrogen-terminated Hall bars engineered on the pre- and post-etched surfaces and rendered conductive by the adsorbed water layer formed on exposure to ambient conditions demonstrate that this etching causes an improvement in the hole mobility by an order of magnitude, resulting in a measured sheet resistivity of 1.04 kΩ/sq at a temperature of 4.2 K without gating.

42 ENGINEERING↗
NASA NTRS1994

The physics of grain-grain collisions and gas-grain sputtering in interstellar shocks

Grain-grain collisions and ion sputtering destroy dust grains in interstellar shocks. An analytical theory is developed for the propagation of shock waves in solids driven by grain-grain collisions, which compares very favorably with detailed numerical calculations. This theory is used to determine the fraction of grain vaporized by a grain-grain collision. Our results predict much less vaporization of colliding grains in interstellar shocks than previous estimates. This theory can also be used to determine the fraction of a colliding grain that melts, shatter, or undergoes a phase transformation to a higher density phase. In particular, the latter two processes can be much more important in interstellar shocks than vaporization. The sputtering of grains by impacting gas ions is reanalyzed based upon extensive laboratory studies and a theoretically derived 'universal'sputtering relation. The analytical results are compared to available experimental studies of sputtering of graphite/amorphous carbon, SiO2, SiC, Fe, and H2O. Sputtering yields for astrophysically relevant materials as a function of impact energy and ion mass are derived. These yields are also averaged over thermal impact spectrum and simple polynomial fits to the resulting yields as a function of temperature are presented. The derived sputtering yields are similar to those adopted in previous studies, except for graphite near threshold where the new yields are much larger due to a lower adopted binding energy. The ion bombardment will amorphitize the surface layers of interstellar grains. It will also convert graphite into hydrogenated amorphous carbon (HAC) to a depth of 10-20 A. It is suggested that these HAC surfaces are the carriers of the 3.4 micrometer absorption feature in the interstellar medium.

Tielens, A. G. G. M.↗
NASA NTRS1993

Diagnostics development for the Electric Propulsion Orbital Platform

We describe the development of the diagnostics systems for the first flight of the Electric Propulsion Orbital Platform (EPOP), which will center around the in-flight characterization of a 1.8 kW hydrogen arcjet system. In particular, we discuss a spacecraft communications experiment involving ground-to-spacecraft communications of the EPOP carrier; electrical probe measurements in the arcjet plume; and spectrally resolved plume imaging measurements of the same plume. The communications experiment is designed to measure small noise on the communications link which results from arcjet operation. The other two measurements primarily serve the purpose of characterization of the plume plasma. These measurements will be compared to similar measurements performed in a ground chamber to establish whether systematic differences exist between ground-based and in-flight performance of the arcjet system.

Ruyten, Wilhelmus M.↗
DOE OSTI2021

Literature Review on the Impact of Thermolytic Hydrogen Generation Rate from the Next Generation Solvent

A literature review was undertaken to assess the thermolytic hydrogen generation potential of the Next Generation Solvent (NGS) system, which is planned to replace the Original Caustic-Side Solvent Extraction (CSSX) Solvent at the Salt Waste Processing Facility. NGS uses a new extractant and suppressor and the same modifier and organic carrier solvent as the Original CSSX Solvent at different concentrations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Effects of frequency and pulse width on electron density, hydrogen peroxide generation, and perfluorooctanoic acid mineralization in a nanosecond pulsed discharge gas-liquid plasma reactor

Plasma electron density and temperature were characterized in a continuous flowing gas-liquid film reactor with argon carrier gas by time-resolved optical emission spectroscopy. The plasma parameters were studied as a function of time for varying pulse widths and frequencies. Pulse frequency was varied between 1 and 10 kHz at 16 kV (input voltage) and 40 ns (pulse width) using an Eagle Harbor Technologies, Inc. (EHT) power supply and 5–100 kHz using an Airity Technologies, LLC (AT) power supply. The pulse width was varied between 40 and 200 ns at 16 kV, 2 kHz with the EHT power supply. Optimal frequencies of 5 and 20 kHz were observed for peak electron density with EHT and AT power supplies, respectively. The peak electron density increased with increasing pulse width between 40 and 200 ns using the EHT power supply. Hydrogen peroxide exiting the reactor in the liquid phase increased with discharge power irrespective of the power supply or pulse parameters. Mineralization of 12.5, 50, and 200 ppm perfluorooctanoic acid (PFOA) dissolved in DI water to fluoride (F - ) correlated to the peak electron density. Glycerol, a liquid-phase hydroxyl radical scavenger, depleted hydrogen peroxide but did not affect PFOA mineralization. CO, a gas-phase hydroxyl radical scavenger, led to a reduction in the formation of F - production, suggesting hydroxyl radicals in the gas-liquid film play a necessary, but not singular, role in mineralization of PFOA.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Photodepositing CdS on the Active Cyano Groups Decorated g‐C 3 N 4 in Z‐Scheme Manner Promotes Visible‐Light‐Driven Hydrogen Evolution

Abstract g‐C 3 N 4 /CdS heterojunctions are potential photocatalysts for hydrogen production but their traditional type‐II configuration generally leads to weak oxidative and reductive activity. How to construct the novel Z‐scheme g‐C 3 N 4 /CdS counterparts to address this issue remains a great challenge in this field. In this work, a new direct Z‐scheme heterojunction of defective g‐C 3 N 4 /CdS is designed by introducing cyano groups (NC‐) as the active bridge sites. Experimental observations in combination with density functional theory (DFT) calculations reveal that the unique electron‐withdrawing feature of cyano groups in the defective g‐C 3 N 4 /CdS heterostructure can endow this photocatalyst with numerous advantageous properties including high light absorption ability, strong redox performance, satisfactory charge separation efficiency, and long lifetime of charge carriers. Consequently, the resultant photocatalytic system exhibits more active performance than CdS and g‐C 3 N 4 under visible light and reaches an excellent hydrogen evolution rate of 1809.07 µmol h −1 g −1 , which is 6.09 times higher than pristine g‐C 3 N 4 . Moreover, the defective g‐C 3 N 4 /CdS photocatalyst maintains good stability after 40 h continuous test. This work provides new insights into design and construction of Z‐scheme heterojunctions for regulating the visible‐light‐induced photocatalytic activity for H 2 evolution.

Wang, Zhipeng↗
NASA NTRS1986

Photo Hall-effect characterization of closely compensated Ge:Be

The temperature dependence of the free-carrier concentration in germanium doped with the double acceptor Be has been investigated using the photo Hall-effect technique and found to be strongly temperature dependent when the residual shallow impurities are closely compensated. Close compensation of shallow levels was achieved by controlling the concentration of a beryllium-hydrogen acceptor complex A(Be,H) which is present in crystals grown under a H2 atmosphere. This complex can be removed with high-temperature annealing. An increase of up to two orders of magnitude in free-carrier lifetime as a function of temperature is found to occur between 5 and 11 K in closely compensated material due to the population inversion of ionized centers created by optical pumping.

Germer, T. A.↗
DOE OSTI2023

Silver nanoparticle enhanced metal-organic matrix with interface-engineering for efficient photocatalytic hydrogen evolution

Integrating plasmonic nanoparticles into the photoactive metal-organic matrix is highly desirable due to the plasmonic near field enhancement, complementary light absorption, and accelerated separation of photogenerated charge carriers at the junction interface. The construction of a well-defined, intimate interface is vital for efficient charge carrier separation, however, it remains a challenge in synthesis. Here we synthesize a junction bearing intimate interface, composed of plasmonic Ag nanoparticles and matrix with silver node via a facile one-step approach. The plasmonic effect of Ag nanoparticles on the matrix is visualized through electron energy loss mapping. Moreover, charge carrier transfer from the plasmonic nanoparticles to the matrix is verified through ultrafast transient absorption spectroscopy and in-situ photoelectron spectroscopy. The system delivers highly efficient visible-light photocatalytic H 2 generation, surpassing most reported metal-organic framework-based photocatalytic systems. This work sheds light on effective electronic and energy bridging between plasmonic nanoparticles and organic semiconductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Observation of attosecond electron dynamics in the photoelectron momentum distribution of atoms using few-cycle laser pulses

The method of time-resolved measurement with ultrashort laser pulses is vital to the development of attosecond science. Pump-probe measurements using a train of attosecond pulses in combination with a near-infrared (NIR) multicycle driving laser have been successful in capturing the intercycle electron dynamics which repeats every optical cycle and leads to above-threshold ionization (ATI) spectra in the frequency domain. Here in this work, we study the effect of a carrier-envelope phase (CEP) in a few-cycle (< 6 fs) NIR laser pulse on the photoelectron momentum distribution (PMD) of a hydrogen atom and show that interference patterns in a PMD change dramatically with CEPs in the few-cycle regime. When the few-cycle driving laser pulse has a sine shape, the double-slit interference with characteristic modulation of ATI peaks dominates the PMD. On the other hand, when the driving pulse has a cosine shape, the holographical interference featured by a spider-like pattern is isolated. Our results suggest that the CEP-stable few-cycle laser pulses can be used to identify different types of intracycle interference structures in a PMD which reveal the underlying subcycle electron dynamics on an attosecond timescale.

74 ATOMIC AND MOLECULAR PHYSICS↗
NASA NTRS1994

Electrochemical Characterization of InP and GaAs Based Structures for Space Solar Cell Applications.

In this paper the emphasis is on accurate majority carrier concentration EC-V profiling of structures based on Indium Phosphide and Gallium Arsenide, using a newly developed electrolyte based on Hydrogen Flouride, Acetic Acid, Phosphoric Acid, 1-phenyl-2-propanamine and Ammonia Diflouride. Some preliminary data on the use of this electrolyte for determining the energy distribution of surface and deep states of these structures, applicable to fabrication process optimization and radiation induced defects studies of solar cells, are also provided.

Faur, Maria↗
NASA NTRS1997

A laboratory analog for the carrier of the 3 micron emission of the protoplanetary nebula IRAS 05341+0852

A mixture of the polycyclic aromatic hydrocarbons (PAHs), acenaphthylene and acenaphthene, when subjected to the energetic environment of a hydrogen plasma, is transformed into a material that exhibits an infrared absorption profile in the 3 micron region that is an excellent match of the protoplanetary nebula IRAS 05341+0852 emission profile in the same wavelength region. Acenaphthylene and acenaphthene were chosen as precursors in the experiment because these molecules have a structure that can be described as a keystone in a process in which carbon atoms in a stellar wind condense into PAH species. The spectral match between experiment and observations appears to validate that scenario.

Non-NASA Center↗
DOE OSTI2021

Integrating computation and experiment to investigate photoelectrodes for solar water splitting at the microscopic scale.

CONSPECTUS: Photoelectrochemical water-splitting is a promising and sustainable way to store the energy of the sun in chemical bonds and use it to produce hydrogen gas, a clean fuel. The key components in photoelectrochemical cells (PECs) are photoelectrodes, including a photocathode that reduces water to hydrogen gas and a photoanode that oxidizes water to oxygen gas. Materials used in photoelectrodes for PECs must effectively absorb sunlight, yield photogenerated carriers, and exhibit electronic properties that enable the efficient shuttling of carriers to the surface to participate in relevant water-splitting reactions. Discovering and understanding the key characteristics of optimal photoelectrode materials is paramount to the realization of PEC technologies. Oxide-based photoelectrodes can satisfy many of these materials requirements, including stability in aqueous environments, band edges with reasonable alignment with the redox potentials for water splitting, and ease of synthesis. However, oxide photoelectrodes generally suffer from poor charge transport properties and considerable bulk electron-hole separation, and they have relatively large band gaps. Numerous strategies have been proposed to improve these aspects and understand how these improvements are reflected in the photoelectrochemical performance. Unfortunately, the structural and compositional complexity of multinary oxides accompanied by the inherent complexity of photoelectrochemical processes makes it challenging to understand the individual effects of composition, structure, and defects in the bulk and on the surface on a material's photoelectrochemical properties. The integration of experiment and theory has great potential to increase our atomic-level understanding of structure-composition-property relationships in oxide photoelectrodes. In this Account, we describe how integrating experiment and theory is beneficial for achieving scientific insights at the microscopic scale. We highlight studies focused on understanding the role of (i) bulk composition via solid-state solutions, intercalation, and comparison with isoelectronic compounds, (ii) dopants for both the anion and cation and their interactions with oxygen vacancies, and (iii) surface/interface structure in the photocurrent generation and photoelectrochemical performance in oxide photoelectrodes. In each instance, we outline strategies and considerations for integrating experiment and theory and describe how this integration led to valuable insights and new directions in uncovering structure-composition-property relationships. Our aim is to demonstrate the unique value of combining experiment and theory in studying photoelectrodes and to encourage the continued effort to bring experiment and theory in closer step with each other.

Wang, Wennie↗
DOE OSTI2021

Effects of HZ-PAN Sorbent Irradiation on Kr Adsorption

Idaho National Laboratory (INL) has developed and studied an engineered form hydrogen mordenite in polyacrylonitrile matrix (HZ-PAN) for krypton (Kr) adsorption. Adsorption studies to date have successfully separated and captured Kr from carrier gas streams, but those studies have used non-radioactive gases for testing. However, if utilized in a used nuclear fuel (UNF) reprocessing facility, this sorbent will be exposed to the potential deleterious effects of radiation. This report explores Kr adsorption behavior on HZ PAN after the sorbent was exposed to gamma radiation. A batch of HZ-PAN was divided into five segments, a control segment that was not exposed to radiation, and the other four segments that were exposed to progressively increased levels of radiation dose, up to 5 MGy. Samples were then analyzed to determine total surface area as well as their capacity to capture Kr. This study reveals HZ PAN retains its initial surface area and Kr-capture capacity after radiation exposure, indicating viability for service in radioactive gases.

42 - ENGINEERING↗