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At least 703 records · Page 39
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Photocatalytic Semi‐Hydrogenation of Acetylene to Polymer‐Grade Ethylene with Molecular and Metal–Organic Framework Cobaloximes

Abstract The semi‐hydrogenation of acetylene in ethylene‐rich gas streams is a high‐priority industrial chemical reaction for producing polymer‐grade ethylene. Traditional thermocatalytic routes for acetylene reduction to ethylene, despite progress, still require high temperatures and high H 2 consumption, possess relatively low selectivity, and use a noble metal catalyst. Light‐powered strategies are starting to emerge, given that they have the potential to use directly the abundant and sustainable solar irradiation, but are ineffective. Here an efficient, >99.9% selective, visible‐light powered, catalytic conversion of acetylene to ethylene is reported. The catalyst is a homogeneous molecular cobaloxime that operates in tandem with a photosensitizer at room temperature and bypasses the use of non‐environmentally friendly and flammable H 2 gas feed. The reaction proceeds through a cobalt‐hydride intermediate with ≈100% conversion of acetylene under competitive (ethylene co‐feed) conditions after only 50 min, and with no evolution of H 2 or over‐hydrogenation to ethane. The cobaloxime is further incorporated as a linker in a metal–organic framework; the result is a heterogeneous catalyst for the conversion of acetylene under competitive (ethylene co‐feed) conditions that can be recycled up to six times and remains catalytically active for 48 h, before significant loss of performance is observed.

Stone, Aaron E. B. S.↗
DOE OSTI2021

Highly Efficient Surface Charge Transfer in Fe 2 TiO 5 Epitaxial Thin Film Photoanodes

Pseudobrookite (Fe 2 TiO 5 ) has attracted significant attention as an emerging photoanode for water oxidation due to reports of enhanced performance in polycrystalline heterostructures with α-Fe 2 O 3 or TiO 2 . However, the specific properties and contribution of Fe 2 TiO 5 remain unknown. Here, we present the first photoelectrochemical characterization of epitaxial thin film Fe 2 TiO 5 , an ideal platform for probing the inherent response of this earth-abundant photoanode for solar water splitting. Moreover, by using an electrolyte containing a hole scavenger, we find highly efficient charge transfer at the Fe 2 TiO 5 –electrolyte interface. This notable surface property is exploited in the form of an Fe 2 TiO 5 /α-Fe 2 O 3 heterostructure photoanode, for which we observe a photocurrent density increase by 1 order of magnitude and an onset potential improvement by ~300 mV. Establishing these fundamental properties elucidates the nature of reaction mechanisms on Fe 2 TiO 5 and informs the design of highly efficient water photo-oxidation devices by incorporating this material with other photoanodes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Photo-DAC: Light-Driven Ambient-Temperature Direct Air Capture by a Photobase

Direct air capture (DAC) may reduce atmospheric CO 2 concentrations to preindustrial levels, yet the high energies and temperatures involved in current DAC technologies hinder large-scale deployment. In the case of aqueous-based CO 2 absorbents, a large energetic penalty is associated with heating and boiling off water, as required for thermally driven solvent regeneration. This could be avoided via photochemically driven pH swings involving photoacids or photobases, and harnessing abundant and renewable solar energy, though efficient solvent regeneration and recycling in a realistic multicycle DAC process remains challenging. Herein, we report a photochemically driven DAC process (photo-DAC) in which atmospheric CO 2 capture by an aqueous glycylglycine (GlyGly) solution is enabled through a pH swing by a pyridine-substituted diiminoguanidine (PyDIG) photobase. Upon irradiation with UV light, the PyDIG photobase undergoes photoisomerization from the E,E to the Z,Z isomer, corresponding to a pK a increase of 2.8 units that activates GlyGly for DAC through deprotonation. After the GlyGly/PyDIG solvent is saturated with atmospheric carbon dioxide, leaving it in the dark under ambient conditions leads to the isomerization of PyDIG from the Z,Z back to the E,E isomer, which is accompanied by a pH drop and CO 2 release. To demonstrate the recyclability of the GlyGly/PyDIG solvent, we have completed six consecutive DAC cycles, with a measured average cyclic capacity in the range of 0.21–0.26 mol CO 2 per mol of GlyGly/PyDIG. These results open the prospect for energy-efficient DAC cycles completed entirely at ambient conditions, thereby avoiding the significant energy penalties associated with heating and boiling aqueous solvents.

Einkauf, Jeffrey D. [Oak Ridge National Laboratory↗
DOE OSTI2021

Effects of Hydrogen on the Phase Relations in Fe-FeS at Pressures of Mars-Sized Bodies

The large radius, and therefore low density, of the Martian core found in the InSight mission data analysis highlights the importance of considering other light elements besides sulfur (S), which has been considered as the main light element for Mars for decades. Hydrogen (H) is abundant in the solar system and becomes siderophile at high pressures. Although Fe-S and Fe-H systems have been studied individually, the Fe-S-H ternary system has only been investigated up to 16 GPa and 1723 K. We have investigated the Fe-S-H system at pressures and temperatures (P-T) relevant to the cores of Mars-sized planets (up to 45 GPa and well above the melting temperature of FeS) in the laser-heated diamond anvil cell combined with in situ synchrotron X-ray diffraction. Here we found that sufficient hydrogen leads to the disappearance of Fe 3 S at high P-T. Instead, separate Fe-H and Fe-S phases appear at 23–35 GPa. At pressures above 35 GPa, we found a new phase appearing while Fe-S phases disappear and Fe-H phases remain. Our analysis indicates that the new phase likely contains both S and H in the crystal structure (tentatively FeS x H y where x ≈ 1 and y ≈ 1). The observed pressure-dependent changes in the phase relation may be important for understanding the structure and dynamics of the Martian core and the cores of Mars-sized exoplanets.

58 GEOSCIENCES↗
NASA NTRS1966

The problem of atomic hydrogen.

Lyman alpha airglow observations indicate diurnal variation of atomic hydrogen in thermosphere and exosphere with abundance change with solar activity

AIRGLOW↗
NASA NTRS1973

Bombardment as a cause of the lunar asymmetry.

The moon is asymmetric in crustal thickness and also in the distribution of maria and gamma radioactivity. Early bombardment of the moon by planetesimals, in both heliocentric and geocentric orbits, is examined as a possible cause of the asymmetries. The presence of a massive companion (earth) causes a spin-orbit coupled moon to be bombarded nonuniformly. The most pronounced local concentration of impacts would have occurred on the west limb of the moon, when it orbited close to the earth, if low-eccentricity heliocentric planetesimals were still abundant in the solar system at that time. A very intense bombardment of this type could have redistributed crustal material on the moon, thinning the west limb crust appreciably. This would have caused a change in position of the principal axes of inertia, and a reorientation of the spin-orbit coupled moon such that the thinnest portion of its crust turned toward one of the poles. Erupting lavas would have preferentially flooded such a thin-crusted, low-lying area. This would have caused another readjustment of principal moments, and a reorientation of the moon such that the mare areas tipped toward the equator.

Wood, J. A.↗
NASA NTRS1981

A balloon measurement of the isotopic composition of galactic cosmic ray boron, carbon and nitrogen

The isotopic compositions of galactic cosmic ray boron, carbon, and nitrogen were measured at energies near 300 MeV amu, using a balloon-borne instrument at an atmospheric depth of approximately 5 g/sq cm. The calibrations of the detectors comprising the instrument are described. The saturation properties of the cesium iodide scintillators used for measurement of particle energy are studied in the context of analyzing the data for mass. The achieved rms mass resolution varies from approximately 0.3 amu at boron to approximately 0.5 amu at nitrogen, consistent with a theoretical analysis of the contributing factors. Corrected for detector interactions and the effects of the residual atmosphere the results are B-10/B=0.33 (+0.17, -0.11), C-13/C=0.06 (+0.13, -0.11), and N-15/N=0.42 (+0.19, -0.17). A model of galactic propagation and solar modulation is described. Assuming a cosmic ray source composition of solar-like isotopic abundances, the model predicts abundances near Earth consistent with the measurements.

Zumberge, J. F.↗
NASA NTRS1985

Propagation and nucleosynthesis of ultraheavy cosmic rays

The observed fluxes of cosmic ray (C.R.) ultraheavy elements depend on their charge and mass spectrum at the sources and on the propagation effects, on the distribution of path lengths traversed by the particles on their way from the sources to the observation point. The effect of different path length distributions (p.l.d.) on the infered source abunances is analyzed. It seems that it is rather difficult to fit a reasonable p.l.d. so that the obtained source spectrum coincides with the Solar System (SS) abundances in more detail. It suggests that the nucleosynthesis conditions for c.r. nuclei may differ from that for SS matter. The nucleosynthesis of ultraheavy elements fitting its parameters to get the c.r. source abundances is calculated. It is shown that it is possible to get a very good agreement between the predicted and the observed source abundance.

Giler, M.↗
NASA NTRS1984

X-ray emission from supernova remnants MSH 14 - 63 and RCW 103

Electron-ion collisions, heavy element enrichment of emissions from reverse-shocked ejecta, abundances in the interstellar medium (ISM), the correspondence between the projected and measured age, ISM particle density, and distance, and classification factors for Type I or II supernovae are examined using a nonequilibrium ionization (NEI) model. The NEI model accounts for the absence of collisional ionization equilibrium and possibly thermal equilibrium between electrons and ions behind the shock fronts, and describes the emission spectra from ejecta and the shocked ISM. When applied to data from the SNR MSH 14 - 63 a non-Coulomb, ion-electron interaction is obtained that is consistent with a shocked ISM. For the SNR RCW 103, however, the processes behind the shock front are not discernable, although the elemental abundances will have solar values if the interactions are non-Coulomb. The age of RCW 103 must be approximated from physical data, as Chinese astronomers would not have been able to see the event from their position on earth two millenia ago.

Nugent, J. J.↗
NASA NTRS1985

Ultraviolet spectral evolution and heavy element abundances in Nova Austrinae 1981

Nova CrA 1981, a moderately fast galactic nova, was systematically observed over a period of seven months with the IUE satellite. The initial evolution of the UV spectrum was similar to that of previously observed novae; however, several months after maximum, weak emission due to very high ionizating forbidden lines of Na, Mg, Al, and Si appeared, eventually decreasing in strength over the next two months. The spectral development of the lines is consistent with the photoionization of an expanding shell; a high-temperature 'coronal' origin is ruled out. Abundances deduced from the spectra show that most of the observed heavy elements in the ejected material are enhanced with respect to helium, with neon the most abundant of these. In addition, there are substantial deviations of the Na/Mg/Al/Si abundance ratios from solar values. This is interpreted as evidence for the mixing of core material with the accreted envelope on a massive O-Ne-Mg (as opposed to a C-O) white dwarf. Furthermore, the proportion of core material in the ejecta implies that the mass of the white dwarf decreased as a consequence of the outburst.

Williams, R. E.↗
NASA NTRS1986

Galactic cosmic ray composition

An assessment is given of the galactic cosmic ray source (GCRS) elemental composition and its correlation with first ionization potential. The isotopic composition of heavy nuclei; spallation cross sections; energy spectra of primary nuclei; electrons; positrons; local galactic reference abundances; comparison of solar energetic particles and solar coronal compositions; the hydrogen; lead; nitrogen; helium; and germanium deficiency problems; and the excess of elements are among the topics covered.

Meyer, J. P.↗
NASA NTRS1988

Infrared spectroscopy of Jupiter and Saturn

High resolution infrared spectoscopy provides unique insights into the chemistry and dynamics of the atmospheres of Jupiter and Saturn. The 5 micrometer spectral region, which is transparent to deep levels, is particularly useful for the identification of molecules that are present at very low (parts per billion) concentrations. These are tracers of convective and strongly non-equilibrium processes in the atmosphere. High resolution ground-based spectroscopy complements Voyager and Galileo measurements. Spectroscopy is sensitive to lower mixing levels for selected molecules, while the on-board mass spectrometers probe molecules that are spectroscopically inaccessible. Analysis and modeling of the 4.7 micrometer carbon monoxide in Jupiter was completed. CO is present at a mole fraction of 1.6 plus or minus 0.3 x 10 to the 9th power and concentrated in the troposphere. At this abundance, it must be convected upward from much deeper levels in Jupiter where the temperature is near 1100 K. Thus CO is a tracer of the deep atmosphere which is otherwise unobservable. The oxygen abundance in Jupiter (as measured by the CO abundance) is near solar. Chemical or physical process must deplete the major oxygen carrier, water. Germane, GeH4, was discovered on Saturn at amole fraction of 4 plus or minus 2 x 10 to the 10th power.

Knacke, Roger↗
NASA NTRS1989

The development of the red giant branch. I - Theoretical evolutionary sequences

A grid of 100 evolutionary sequences extending from the zero-age main sequence to the onset of helium burning has been computed for stellar masses between 1.4 and 3.4 solar masses, helium abundances of 0.20 and 0.30, and heavy-element abundances of 0.004, 0.01, and 0.04. Using these computations the transition in the morphology of the red giant branch (RGB) between low-mass stars, which have an extended and luminous first RGB phase prior to helium ignition, and intermediate-mass stars, which do not, is investigated. Extensive tabulations of the numerical results are provided to aid in applying these sequences. The effects of the first dredge-up on the surface helium and CNO abundances of the sequences is discussed.

Sweigart, Allen V.↗
NASA NTRS1989

The carbon chemistry of meteorites: Relationships to comets

The carbonaceous meteorites exhibiting alteration by liquid water bear a strong relationship to comets. Not only is their elemental composition closer to solar in relative abundances than other meteorites, they are water rich; and they contain isotopic compositions among refractory and volatile elements indicative of presolar components. Some of these isotopic anomalies occur in organic compounds and carbonaceous grains signifying the presence of discrete and identifiable carbon components derived from interstellar and circumstellar matter. Insofar as comets and meteorites are ultimately formed from interstellar gas and dust, and comets have been subjected to considerably less aqueous and thermal evolution than carbonaceous meteorites, the interstellar imprint should be much stronger and better preserved in comets.

Chang, S.↗
NASA NTRS1990

Ultraviolet spectroscopy of planetary nebulae: Cosmological implications

Optical spectrophotometry of PW Vulpeculae (Nova Vul 1984 no. 1) is combined with ultraviolet data to estimate electron temperatures, densities, and abundances in the ejecta of this slow classical nova. The reddening, distance, and evolution of the ultraviolet spectrum are also discussed. Abundances are nearly solar, with the exception of Nitrogen, which is substantially higher. Although Neon has been reported to be enhanced in several novae, it does not seem to be the case for PW Vul. Photoionization model calculations are presented of the ejecta that give a reasonable match of the observed emission spectrum. A strong featureless continuum shows that very hot, presumably shock heated, gas plays a major role in determining the energetics of this nova. Emission from this hot gas is responsible for the ionization of the nebular gas. A calculation of the masses of both the hot coronal gas and the cooler nebular gas shows that the former may account for most of the mass of the ejecta.

Ferland, Gary J.↗