Nonequilibrium gasdynamics
Nonequilibrium gas dynamics of hydrogen dissociation and recombination
Watt, W. S.↗
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Storage and recombination of atomic H in solid H2
A phenomenological rate process theory is developed for the storage and rapid recombination of atomic hydrogen free radicals in a crystalline molecular hydrogen solid at temperatures in the range of about 0.1-4 K. It is shown that such a theory can account quantitatively for the recently observed dependence of the storage time on the storage temperature, for the maximum concentration of trapped H atoms, and for the time duration of the energy release in the tritium decay experiments of Webeler. The theory predicts that maximum atomic hydrogen concentrations of the order 10 to the 20th per cu cm are realizable for storage temperatures in the vicinity of 0.14 K.
Rosen, G.↗
Spectroscopy of the B-gamma line in the Galactic center
Spectra of the B-gamma recombination line of hydrogen in the Galactic center show that the line has central velocities and shapes similar to those reported previously for the Ne II line. Observations are made at 10 positions within the infrared cluster of the Galactic center with a circular diaphragm of diameter 5 arcsec and with a spectral resolution of approximately 85 km/sec. The spectra confirm that the ionized gas in the Galactic center is distributed in discrete clouds.
Nadeau, D.↗
Infrared imaging spectroscopy of the Galactic center - Distribution and motions of the ionized gas
High spatial spectral resolution IR images of the Galactic center in the Br-gamma recombination line of hydrogen were taken. A coherent filament of gas extending from north of IRS 1, curving around IRS 16/Sgr A complex, and continuing to the southwest, is seen. Nine stellar sources have associated Br-gamma emission. The total Br-gamma line flux in the filament is approximately 3 x 10 exp -15 W/sq m. The distribution and kinematics of the northern arm suggest orbital motion; the observations are accordingly fit with elliptical orbits in the field of a central point of mass.
Herbst, T. M.↗
Hubble Space Telescope images of the Seyfert galaxies NGC 5929 and MCG 8-11-11
We present the initial results of a program to obtain high resolution images of Seyfert galaxies with the Planetary Camera aboard the Hubble Space Telescope (HST). In this paper we discuss the images of the type 2 Seyfert NGC 5929 and the type 1.5 Seyfert MCG 8-11-11 (= UGC 3374). The images were obtained in the emission lines of (O III) lambda lambda 4959 and 5007 A and H alpha + (N II) lambda lambda 6548 and 6583 A and their adjacent continua. The high-excitation gas in the narrow line region (NLR) of NGC 5929 is resolved into individual clouds in the central 1 sec .5. Although the (O III) emission is clearly not spherically symmetric with respect to the nucleus, it does not define a distinct 'bicone' morphology, as observed by the HST in a few other Seyfert galaxies. We find no direct evidence for the reddening and/or obscuration effects characteristic of a dusty torus, which, in the context of 'unified models', is expected to obscure the active galactic nucleus (AGN) in type 2 Seyfert galaxies. The correspondence between the emission line gas and the radio morphology suggests that the structure of the NLR in NGC 5929 is governed by matter ejected from the AGN. A comparison of the recombination rate of hydrogen in the brightest emission line cloud with an upper limit on the ionizing luminosity emitted toward Earth provides no evidence that the central ionizing source radiates anisotropically. The images of MCG 8-11-11 show only an unresolved nuclear source. No emission line gas associated with the extended radio source is detected. We estimate upper limits on the intensity of extended line emission in this galaxy and examine their significance.
Bower, Gary A.↗
Evolution of Iron K Alpha Line Emission in the Black Hole Candidate GX 339-4
GX 339-4 was regularly monitored with the Rossi X-Ray Timing Explorer during a period (in 1999) when its X-ray flux decreased significantly (from 4.26 x 10(exp -10) to 7.6 x 10(exp -12) ergs in the 3-20 keV band), as the source settled into the 'off state.' Our spectral analysis revealed the presence of a prominent iron K alpha line in the observed spectrum of the source for all observations. The line shows an interesting evolution: it is centered at approx. 6.4 keV when the measured flux is above 5 x 10(exp -1) ergs per sq cm/s but is shifted to approx. 6.7 keV at lower fluxes. The equivalent width of the line appears to increase significantly toward lower fluxes, although it is likely to be sensitive to calibration uncertainties. While the fluorescent emission of neutral or mildly ionized iron atoms in the accretion disk can perhaps account for the 6.4 keV line, as is often invoked for black hole candidates, it seems difficult to understand the 6.7 keV line with this mechanism because the disk should be less ionized at lower fluxes (unless its density changes drastically). On the other hand, the 6.7 keV line might be due to a recombination cascade of hydrogen- or helium-like iron ions in an optically thin, highly ionized plasma. We discuss the results in the context of proposed accretion models.
Feng, Y. X.↗
Near-infrared spectroscopy of the proto-planetary nebula CRL 618 and the origin of the hydrocarbon dust component in the interstellar medium
A new 2.8-3.8 micrometers spectrum of the carbon-rich protoplanetary nebula CRL 618 confirms the previous detection of a circumstellar 3.4 micrometers absorption feature in this object (Lequeux & Jourdain de Muizon). The high resolution and high signal-to-noise ratio of our spectrum allow us to derive the detailed profile of this absorption feature, which is very similar to that observed in the spectrum of the Galactic center and also resembles the strong 3.4 micrometers emission feature in some post-asymptotic giant branch stars. A weak 3.3 micrometers unidentified infrared band, marginally detected in the CRL 618 spectrum of Lequeux & Jourdain de Muizon, is present in our spectrum. The existence of the 3.4 micrometers feature implies the presence of relatively short-chained, aliphatic hydrocarbon materials (-CH2-/-CH3 approximately = 2-2.5) in the circumstellar environment around CRL 618. It also implies that the carriers of the interstellar 3.4 micrometers feature are produced at least in part in circumstellar material, and it calls into question whether any are produced by the processing of interstellar ices in dense interstellar clouds, as has been previously proposed. Other features in the spectrum are recombination lines of hydrogen, rotational and vibration-rotation lines of molecular hydrogen, and a broad absorption probably due to a blend of HCN and C2H2 bands.
Spectroscopy, Near-Infrared↗
Multiphysics Analysis of a Solid-Core Nuclear Thermal Engine Thrust Chamber
The objective of this effort is to develop an efficient and accurate thermo-fluid computational methodology to predict environments for a hypothetical solid-core, nuclear thermal engine thrust chamber. The computational methodology is based on an unstructured-grid, pressure-based computational fluid dynamics methodology. Formulations for heat transfer in solids and porous media were implemented and anchored. A two-pronged approach was employed in this effort: A detailed thermo-fluid analysis on a multi-channel flow element for mid-section corrosion investigation; and a global modeling of the thrust chamber to understand the effect of hydrogen dissociation and recombination on heat transfer and thrust performance. The formulations and preliminary results on both aspects are presented.
Wang, Ten-See↗
Lyman-Alpha Comes of Age
The Lyman-alpha (Lyα) line is the strongest recombination line of hydrogen, which constitutes the dominant share of normal matter in the Universe. Fifty-one years ago, it was predicted that Lyα emission should appear prominently in the spectra of young primordial galaxies. For the next 30 years, this prediction was tested by many surveys, but none found the predicted galaxies at the predicted luminosities. The blame for these non-detections was squarely cast on the resonant nature of the Lyα line, which requires Lyα photons to scatter off many hydrogen atoms before escaping from a galaxy. This can hugely increase the path that they traverse, and consequently also the probability that they will be absorbed by dust. This remained the dominant explanation of the missing high-redshift lines for decades, despite some dissenting opinions about the effect of dust. The spectra of nearby galaxies from the International Ultraviolet Explorer are inconclusive about what allows galaxies to be Lyα emitters. The ‘missing’ lines were finally detected 20 years ago, at flux levels much below the original predictions - a difference that we understand to be predominantly due to the hierarchical growth of galaxies, such that star-forming objects at high redshift are much less massive than anticipated in the original prediction. The discovery and study of Lyα galaxies has blossomed into an invaluable method for understanding the youngest stages of galaxy formation, the circumgalactic medium, and ultimately the epoch of reionization. The high equivalent widths of Lyα galaxies from the earliest high-redshift surveys show that they are low-mass galaxies dominated by young stellar populations. The Sakura CLAW workshop (which used the Twitter hashtag #SakuraCLAW) gathered more than 110 participants (Fig. 1) who showcased progress that pushed the frontiers of Lyα galaxy science in sample size, sensitivity, redshifts and physical understanding..
Malhotra, Sangeeta↗
A Lunar Farside Low Radio Frequency Array for Dark Ages 21-cm Cosmology
An array of low-frequency dipole antennas on the lunar farside surface will probe a unique, unexplored epoch in the early Universe called the Dark Ages. It begins at Recombination when neutral hydrogen atoms formed, first revealed by the cosmic microwave background. This epoch is free of stars and astrophysics, so it is ideal to investigate high energy particle processes including dark matter, early Dark Energy, neutrinos, and cosmic strings. A NASA-funded study investigated the design of the instrument and the deployment strategy from a lander of 128 pairs of antenna dipoles across a 10 kmx10 km area on the lunar surface. The antenna nodes are tethered to the lander for central data processing, power, and data transmission to a relay satellite. The array, named FARSIDE, would provide the capability to image the entire sky in 1400 channels spanning frequencies from 100 kHz to 40 MHz, extending down two orders of magnitude below bands accessible to ground-based radio astronomy. The lunar farside can simultaneously provide isolation from terrestrial radio frequency interference, the Earth's auroral kilometric radiation, and plasma noise from the solar wind. It is thus the only location within the inner solar system from which sky noise limited observations can be carried out at sub-MHz frequencies. Through precision calibration via an orbiting beacon and exquisite foreground characterization, the farside array would measure the Dark Ages global 21-cm signal at redshifts z~35-200. It will also be a pathfinder for a larger 21-cm power spectrum instrument by carefully measuring the foreground with high dynamic range.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Forecasting ground-based sensitivity to the Rayleigh scattering of the CMB in the presence of astrophysical foregrounds
The Rayleigh scattering of cosmic microwave background (CMB) photons off the neutral hydrogen produced during recombination effectively creates an additional scattering surface after recombination that encodes new cosmological information, including the expansion and ionization history of the universe. A first detection of Rayleigh scattering is a tantalizing target for next-generation CMB experiments. We have developed a Rayleigh scattering forecasting pipeline that includes instrumental effects, atmospheric noise, and astrophysical foregrounds (e.g., Galactic dust, cosmic infrared background, or CIB, and the thermal Sunyaev-Zel'dovich effect). We forecast the Rayleigh scattering detection significance for several upcoming ground-based experiments, including SPT-3G+, Simons Observatory, CCAT-prime, and CMB-S4, and examine the limitations from atmospheric and astrophysical foregrounds as well as potential mitigation strategies. When combined with Planck data, we estimate that the ground-based experiments will detect Rayleigh scattering with a significance between 1.6 and 3.7, primarily limited by atmospheric noise and the CIB.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Role of Metal Cocatalysts in the Photocatalytic Production of Hydrogen from Water Revisited
The use of photocatalysts to promote the production of molecular hydrogen from water, following the so-called water splitting reaction, continues to be a promising route for the green production of fuels. The molecular basis of this photocatalysis is the photoexcitation of electrons from the valence band of semiconductors to their conduction band, from which they can be transferred to chemical reactants, protons in the case of water, to promote a reduction reaction. The mechanism by which such a process takes place has been studied extensively using titanium oxide, a simple material that fulfills most requirements for water splitting. However, photocatalysis with TiO 2 tends to be highly inefficient; a cocatalyst, commonly a late transition metal (Au, Pt) in nanoparticle form, needs to be added to facilitate the production of H 2 . The metal is widely believed to help with the scavenging of the excited electrons from the conduction band of the semiconductor in order to prevent their recombination with the accompanying hole formed in the valence band, a step that cancels the initial photon absorption and competes with the photolytic chemical reduction. Here we review and analyze the molecular basis for that mechanism and argue for an alternative explanation, that the role of the metal is to help with the recombination of the atomic hydrogen atoms produced by proton reduction on the semiconductor surface instead. First, we summarize what is known about the electronic structure of these photocatalysts and how the electronic levels need to line up for the reduction of protons in water to be feasible. Next, we review the current understanding of the dynamics of the steps associated with the absorption of photons, the de-excitation via electron–hole pair recombination and fluorescence decay, and the electronic transitions that lead to proton reduction, and contrast those with the rates of the chemical steps required to produce molecular hydrogen. The following section addresses the changes introduced by the addition of the metal cocatalyst, comparatively evaluating its role as either an electron scavenger or a promoter of the recombination of hydrogen atoms. A discussion of the viable chemical mechanisms for the latter pathway is included. Finally, we briefly mention other associated aspects of this photocatalysis, including the possible promotion of H 2 production with visible light via resonant excitation of the surface plasmon of Au nanoparticles, the use of single-metal (Au, Pt) atom catalysts and of yolk–shell nanostructures, and the reduction of organic molecules. We end with a brief personal perspective on the possible generality of the concepts introduced in this Critical Review.
08 HYDROGEN↗
Entropic Control of HD Exchange Rates over Dilute Pd-in-Au Alloy Nanoparticle Catalysts
Dilute Pd-in-Au alloy catalysts are promising materials for selective hydrogenation catalysis. Extensive surface science studies have contributed mechanistic insight on the energetic aspect of hydrogen dissociation, migration and recombination on dilute alloy systems. Yet, translating these fundamental concepts to the kinetics and free energy of hydrogen dissociation on nanoparticle catalysts operating at ambient pressures and temperatures remains challenging. Here, the effect of the Pd concentration and Pd ensemble size on the catalytic activity, apparent activation energy and rate limiting process is addressed by combining experiment and theory. Experiments in a flow reactor show that a compositional change from 4 to 8 atm% Pd of the Pd-in-Au alloy catalyst leads to strong increase in activity, even exceeding the activity per Pd atom of monometallic Pd under the same conditions, albeit with an increase in apparent activation energy. First-principles calculations show that the rate and apparent activation enthalpy for HD exchange increase when increasing the Pd ensemble size from single Pd atoms to Pd trimers in a Au surface, suggesting that the ensemble size distribution shifts from mainly single Pd atoms on the 4 atm% Pd alloy to larger Pd ensembles of at least three atoms for the 8 atm% Pd/Au catalyst. The DFT studies also indicated that the rate-controlling process is different: H 2 (D 2 ) dissociation determines the rate for single atoms whereas recombination of adsorbed H and D determines the rate on Pd trimers. Both experiment and theory suggest that the increased reaction rate with increasing Pd content and ensemble size stems from an entropic driving force. Lastly, our results support hydrogen migration between Pd sites via Au and indicate that the dilute alloy design prevents the formation of subsurface hydrogen, which is crucial in achieving high selectivity in hydrogenation catalysis.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Dielectronic recombination rates, ionization equilibrium, and radiative energy-loss rates for neon, magnesium, and sulfur ions in low-density plasmas
Results of detailed and systematic calculations are presented for the total dielectronic recombination rate coefficients for the ions of Ne, Mg, and S in a low-density predominantly hydrogen plasma. The new recombination rates are used to calculate solar corona ionization-equilibrium distributions of the ions. The most important effect of dielectronic recombination for ions in corona equilibrium is found to be a shift in the maximum-abundance temperatures toward higher temperatures, which are in some cases reduced from those predicted on the basis of the simple Burgess formula.
Jacobs, V. L.↗
Asymmetrical C–C Coupling for Electroreduction of CO on Bimetallic Cu–Pd Catalysts
Electroreduction of carbon monoxide (CO) possesses great potential for achieving the renewable synthesis of hydrocarbon chemicals from CO 2 . We report here selective reduction of CO to acetate using Cu–Pd bimetallic electrocatalysts. High activity and selectivity are demonstrated for CO-to-acetate conversion with >200 mA/cm 2 in geometric current density and >65% in Faradaic efficiency (FE). An asymmetrical C–C coupling mechanism is proposed to explain the composition-dependent catalytic performance and high selectivity toward acetate. This mechanism is supported by the computationally predicted shift of the *CO adsorption from the top-site configuration on Cu (or Cu-rich) surfaces to the bridge sites of Cu–Pd bimetallic surfaces, which is also associated with the reduction of the CO hydrogenation barrier. Further kinetic analysis of the reaction order with respect to CO and Tafel slope supports a reaction pathway with *CO–*CHO recombination following a CO hydrogenation step, which could account for the electroreduction of CO to acetate on the Cu–Pd bimetallic catalysts. Furthermore, our work highlights how heteroatomic alloy surfaces can be tailored to enable distinct reaction pathways and achieve advanced catalytic performance beyond monometallic catalysts.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Understanding the cold plasma synthesis of ammonia with model metal catalysts through plasma diagnostics (Final Report)
The industrial synthesis of ammonia, which amounts to over 200 million tons annually, is the most energy-intensive chemical process. Therefore, there is a critical need and increased interest in exploring less energetic routes to produce ammonia. Not only does ammonia have a direct impact on the food market, but also it has the potential as a fuel and hydrogen carrier. Recently, plasma catalysis has emerged as a promising alternative for synthesizing ammonia at mild (pressure, temperature and power) conditions. The key to this catalytic process is the synergy between the plasma and the catalyst, where the non-equilibrium plasma allows the generation of excited species, which recombine at the catalyst surface to form ammonia. However, our current understanding of this process is in its infancy. In this respect, model metals are ideal candidates for gaining a basic understanding of this reaction. Moreover, a major roadblock to rationally designing novel effective catalysts for plasma-assisted ammonia production is the need for fundamental aspects of this process. Through a comprehensive plan that integrates model metals as catalysts and world-class diagnostics, the proposed work aims to provide fundamental knowledge about the nature of reactive processes occurring during plasma-assisted catalysis and to demonstrate the selective production of ammonia, catalyzed by employing selected metals under non-thermal plasma conditions. Toward this goal, the central thrust of this proposal was to demonstrate that the synergy between plasma and rationally selected model metals will boost ammonia yields during plasma-assisted ammonia synthesis by delaying hydrogen recombination. Specifically, we aimed to (1) understand the formation and role of gas-phase active species such as NH, N 2 , N 2 + and Ha during the plasma-enhanced synthesis of ammonia through OES and FTIRAS using different reaction configurations: a) only plasma (non-packed DBD reactor) and b) packed DBD reactor with metal nanoparticles. This proposal was awarded/recommended with a run time on the PCRF facility FY20.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Multiple jets from the young star IRAS 21334 + 5039
The source IRAS 21334 + 5039, a young stellar object (YSO) with broad CO outflow velocity profiles, was imaged in the 1-2 micron region with broad-band J, H, and K filters, and with a Fabry-Perot set to the molecular hydorgen v = 1-0 S(1) line, the hydrogen Br-gamma recombination line, and the neighboring continua. At 2 microns the source has an elongated continuum emission structure centered on the star. The structure has very blue tips, with a weak VLA 6 cm continuum source coincident with one of them. Strong molecular hydrogen emission appears as bow-shaped arcs oriented along an axis perpendicular to the continuum emission, and as a weaker structure aligned with it. Both the continuum and the molecular hydrogen emission are most likely produced by jets, possibly emanating in multiple directions from the central source at large angles to each other. While jets are a common feature of young stars, this source provides solid evidence for multiple jet structures.
Smith, Howard A.↗
Metal-free carbocatalyst for room temperature acceptorless dehydrogenation of N-heterocycles
Catalytic dehydrogenation enables reversible hydrogen storage in liquid organics as a critical technology to achieve carbon neutrality. However, oxidant or base-free catalytic dehydrogenation at mild temperatures remains a challenge. Here, we demonstrate a metal-free carbocatalyst, nitrogen-assembly carbons (NCs), for acceptorless dehydrogenation of N-heterocycles even at ambient temperature, showing greater activity than transition metal–based catalysts. Mechanistic studies indicate that the observed catalytic activity of NCs is because of the unique closely placed graphitic nitrogens (CGNs), formed by the assembly of precursors during the carbonization process. The CGN site catalyzes the activation of C–H bonds in N-heterocycles to form labile C–H bonds on catalyst surface. The subsequent facile recombination of this surface hydrogen to desorb H 2 allows the NCs to work without any H-acceptor. With reverse transfer hydrogenation of various N-heterocycles demonstrated in this work, these NC catalysts, without precious metals, exhibit great potential for completing the cycle of hydrogen storage.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗