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Results for “heterogeneous catalysis”

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 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1982

Neutral and charged clusters in the atmosphere - Their importance and potential role in heterogeneous catalysis

An assessment is presented of current knowledge concerning the role and importance of neutral and charged clusters in atmospheric heterogeneous catalysis, with a view to the recommendation of future studies needed for progress in the quantification of aerosol formation and catalytic reactivity. It is established that nucleation from the gaseous to the aerosol state commences via the formation of clusters among molecules participating in the phase-transformation process. Nucleation may proceed in some cases by way of the formation of prenucleation embryos, which then evolve through the energy barrier and undergo phase transformation. In other cases, cluster-cluster interaction among neutral particles or stagewise building of alternate-sign ion clusters may be important in the gas-to-particle conversion process.

Castleman, A. W., Jr.↗
NASA NTRS1983

ECUT: Energy Conversion and Utilization Technologies program. Heterogeneous catalysis modeling program concept

Insufficient theoretical definition of heterogeneous catalysts is the major difficulty confronting industrial suppliers who seek catalyst systems which are more active, selective, and stable than those currently available. In contrast, progress was made in tailoring homogeneous catalysts to specific reactions because more is known about the reaction intermediates promoted and/or stabilized by these catalysts during the course of reaction. However, modeling heterogeneous catalysts on a microscopic scale requires compiling and verifying complex information on reaction intermediates and pathways. This can be achieved by adapting homogeneous catalyzed reaction intermediate species, applying theoretical quantum chemistry and computer technology, and developing a better understanding of heterogeneous catalyst system environments. Research in microscopic reaction modeling is now at a stage where computer modeling, supported by physical experimental verification, could provide information about the dynamics of the reactions that will lead to designing supported catalysts with improved selectivity and stability.

Voecks, G. E.↗
NASA NTRS1994

Stability of the Martian atmosphere: Is heterogeneous catalysis essential?

A comprehensive homogeneous gas phase photochemical model is developed to study the problem of stability of the Martian atmosphere. The one-dimensional model extends from the ground up to 220 km, passing through the homopause at 125 km. The model thus couples the lower (neutral) atmosphere to the ionosphere above which provides significant downward flux of carbon monoxide and oxygen atoms. It is concluded on the basic of currently accepted values for globally and seasonally averaged water vapor abundance, dust opacity and the middle atmospheric eddy mixing coefficient, as well as the relevant laboratory data (particularly the temperature dependence of CO2 absorption cross section and the rate constant for CO+OH reaction), that the rate of re-formation of carbon dioxide exceeds its photolytic destruction rate by about 40%. Furthermore, it is found that this result is virtually independent of the choice of eddy mixing coefficient, unless its value in the middle atmosphere exceeds 10(exp 8) sq cm/sec or is far smaller than 10(exp 5)sq cm/sec, or the dust opacity, unless it exceeds unity, or the water vapor mixing ratio at the surface, unless it is far smaller (less than or = 1 ppm) or far greater (greater than or = 500 ppm) than the average value (approximately 150 ppm). Since none of these extremes represent globally and seasonally averaged conditions on Mars, we propose that the present model requires existence of a mechanism to throttle down the recycling rate of carbon dioxide on Mars. Therefore, it is suggested that a heterogeneous process which provides a sink to the species that participate in the recycling of CO2, i.e., H2O, H2O2, OH, CO or O, in particular, may be necessary to bring about the balance between the CO2 recycling rate and its photolytic destruction rate. Aerosols of dust or ice (pure or doped water or carbon dioxide ice present in the atmosphere of Mars) can provide the appropriate adsorption sites for the above heterogeneous process. Despite our conclusion that some heterogeneous process may be needed, it is important to recognize that one-dimensional models can only provide first-order results which, most likely, represent globally and seasonally averaged conditions. However, it is only after actual temporal, latitudinal and longitudinal variations of relevant atmospheric parameters are included in the model that one can determine fuly whether the problem of atmospheric stabiltiy still continues to persist and whether some heterogeneous process is required to correct it.

Atreya, Sushil K.↗
NASA NTRS1977

Observations of exoelectron emission associated with heterogeneous catalysis

It is suggested that the exoelectron emission from the catalyst may be used to monitor the rate of oxidation of CO and CH4 over palladium catalysts. Indirect heating of the catalyst and atmospheric pressure have no effect upon this monitoring system. Although the mechanism relating catalysis to exoelectron emission is not clear, it is considered possible that electron emission is triggered by the adsorption-desorption cycle.

Hoenig, S. A.↗
NASA NTRS1995

Two-Photon Laser-Induced Fluorescence O and N Atoms for the Study of Heterogeneous Catalysis in a Diffusion Reactor

Advanced laser-based diagnostics have been developed to examine catalytic effects and atom/surface interactions on thermal protection materials. This study establishes the feasibility of using laser-induced fluorescence for detection of O and N atom loss in a diffusion tube to measure surface catalytic activity. The experimental apparatus is versatile in that it allows fluorescence detection to be used for measuring species selective recombination coefficients as well as diffusion tube and microwave discharge diagnostics. Many of the potential sources of error in measuring atom recombination coefficients by this method have been identified and taken into account. These include scattered light, detector saturation, sample surface cleanliness, reactor design, gas pressure and composition, and selectivity of the laser probe. Recombination coefficients and their associated errors are reported for N and O atoms on a quartz surface at room temperature.

Pallix, Joan B.↗
NASA NTRS2009

Method of Heating a Foam-Based Catalyst Bed

A method of heating a foam-based catalyst bed has been developed using silicon carbide as the catalyst support due to its readily accessible, high surface area that is oxidation-resistant and is electrically conductive. The foam support may be resistively heated by passing an electric current through it. This allows the catalyst bed to be heated directly, requiring less power to reach the desired temperature more quickly. Designed for heterogeneous catalysis, the method can be used by the petrochemical, chemical processing, and power-generating industries, as well as automotive catalytic converters. Catalyst beds must be heated to a light-off temperature before they catalyze the desired reactions. This typically is done by heating the assembly that contains the catalyst bed, which results in much of the power being wasted and/or lost to the surrounding environment. The catalyst bed is heated indirectly, thus requiring excessive power. With the electrically heated catalyst bed, virtually all of the power is used to heat the support, and only a small fraction is lost to the surroundings. Although the light-off temperature of most catalysts is only a few hundred degrees Celsius, the electrically heated foam is able to achieve temperatures of 1,200 C. Lower temperatures are achievable by supplying less electrical power to the foam. Furthermore, because of the foam s open-cell structure, the catalyst can be applied either directly to the foam ligaments or in the form of a catalyst- containing washcoat. This innovation would be very useful for heterogeneous catalysis where elevated temperatures are needed to drive the reaction.

Fortini, Arthur J.↗
NASA NTRS1972

Detection techniques for tenuous planetary atmospheres

The research for the development of new types of detectors for analysis of planetary atmospheres is summarized. Topics discussed include: corona discharge humidity detector, surface catalysis and exo-electron emission, and analysis of soil samples by means of exo-electron emission. A report on the exo-electron emission during heterogeneous catalysis is included.

Hoenig, S. A.↗
NASA NTRS2001

Catalysis in the 3rd Dimension: How Organic Molecules May be Formed

Catalysis is often little more than a word to phenomenologically describe the fact that a reaction follows a pat1 that leads to products of an unexpected kind or of unexpected yield. Low activation energy barriers for intermediates are recognized as the most likely cause why a system deviates from the thermodynamic pull towards minimizing its free energy and ends up in a metastable state. Seldom is the mechanism known. This i: particularly true for heterogeneous catalysis under hydrothermal conditions with minerals as catalysts. It is commonly assumed that catalytic action takes place across solid-fluid interfaces and that, on the atomic level, interfaces are just 2-dimensional contacts. This makes it difficult to understand, for instance, the assembly of long-chain carboxylic (fatty) acids. 3y studying single crystals that grew from a melt in the presence of H2O and CO2, we can show: (1) that numerals take up the fluid components into solid solution, (2) that some-thing happens converting them to -educedH and C, (3) that C atoms segregate into dislocations and tie C-C bonds. The products are medium-to-long chain Cn protomolecules, with some C-H attached, pre-assembled in the dislocations. Upon solvent extraction, these proto-molecules turn into carboxylic and dicarboxylic acids. This observation suggests that, in a very elementary step, catalysis under hydrothermal conditions leading to fatty acids involves the pre-assembly of Cn entities in the interface that is not 2-D but extends into the 3rd dimension, with dislocations as synthesis sites.

Freund, Friedemann↗
NASA NTRS1979

Theory of molecular rate processes in the presence of intense laser radiation

The present paper deals with the influence of intense laser radiation on gas-phase molecular rate processes. Representations of the radiation field, the particle system, and the interaction involving these two entities are discussed from a general rather than abstract point of view. The theoretical methods applied are outlined, and the formalism employed is illustrated by application to a variety of specific processes. Quantum mechanical and semiclassical treatments of representative atom-atom and atom-diatom collision processes in the presence of a field are examined, and examples of bound-continuum processes and heterogeneous catalysis are discussed within the framework of both quantum-mechanical and semiclassical theories.

George, T. F.↗
NASA NTRS1981

Effect of particle size on the chemisorption and decomposition of carbon monoxide by palladium and nickel clusters

The chemisorption of gases on well-defined, supported metal particles is a model for basic processes in heterogeneous catalysis. In this study, the chemisorption and decomposition of carbon monoxide on palladium and nickel particles was examined as a function of particle size. Particulate films with average particle sizes ranging from 1 to 10 nm were grown by vapor deposition on UHV-cleaved mica. Successive CO adsorption-desorption cycles resulted in the accumulation of carbon on the particles, which suppressed CO adsorption. The rate of carbon accumulation was strongly dependent on particle size and was higher for Ni than for Pd over the same size range. Carbon was removed from both metals by oxygen treatments at elevated temperatures. However, a mixture of CO and O2 was effective for monitoring the removal of carbon from palladium.

Doering, D. L.↗
NASA NTRS1992

Catalytic oxidation for treatment of ECLSS and PMMS waste streams

Catalytic oxidation was added to the baseline multifiltration technology for use on the Space Station Freedom in order to convert low-molecular weight organic waste components such as alcohols, aldehydes, ketones, amides, and thiocarbamides to CO2 at low temperature (121 C), thereby reducing the total organic carbon (TOC) to below 500 ppb. The rate of reaction for the catalytic oxidation of aqueous organics to CO2 and water depends primarily upon the catalyst, temperature, and concentration of reactants. This paper describes a kinetic study conducted to determine the impact of each of these parameters upon the reaction rate. The results indicate that a classic kinetic model, the Langmuir-Hinshelwood rate equation for heterogeneous catalysis, can accurately represent the functional dependencies of this rate.

Akse, James R.↗
NASA NTRS1995

Molecular dynamics studies of simple membrane-water interfaces: Structure and functions in the beginnings of cellular life

Molecular dynamics computer simulations of the structure and functions of a simple membrane are performed in order to examine whether membranes provide an environment capable of promoting protobiological evolution. Our model membrane is composed of glycerol 1-monooleate. It is found that the bilayer surface fluctuates in time and space, occasionally creating thinning defects in the membrane. These defects are essential for passive transport of simple ions across membranes because they reduce the Born barrier to this process by approximately 40%. Negative ions are transferred across the bilayer more readily than positive ions due to favorable interactions with the electric field at the membrane-water interface. Passive transport of neutral molecules is, in general, more complex than predicted by the solubility-diffusion model. In particular, molecules which exhibit sufficient hydrophilicity and lipophilicity concentrate near membrane surfaces and experience 'interfacial resistance' to transport. The membrane-water interface forms an environment suitable for heterogeneous catalysis. Several possible mechanisms leading to an increase of reaction rates at the interface are discussed. We conclude that vesicles have many properties that make them very good candidates for earliest protocells. Some potentially fruitful directions of experimental and theoretical research on this subject are proposed.

Pohorille, Andrew↗
NASA NTRS2000

The Decomposition of Carbonates and Organics on Mars

The return and analysis of pristine material that is relict of a putative period of chemical evolution is a fumdamental goal of the exobiological exploration of Mars. In order to accomplish this objective, it is desirable to find oxidant-free regions where pristine material can be accessed at the shallowest possible depth (ideally directly from the surface). The objective of our ongoing research is to understand the spatial and temporal distribution of oxidants in the martian regolith and the redox chemistry of the soil; in effect to understand the chemical mechanisms and kinetics relating to the in-situ destruction of organics and the formation of the reactive species responsible for the Viking biology results. In this work, we report on experimental studies of oxidizing processes that may contribute to carbonate and organic degradation on Mars. Organic molecules directly exposed to solar UV may decomposed either directly into CO2, or into more volatile organic fragments. Organic macromolecules not directly exposed to high UV flux are most likely to be affected by atmospheric oxidants which can diffuse to their surfaces. The oxidizing processes examined include: gas-phase oxidants, UV photolysis, and UV-assisted heterogeneous catalysis. For example, assuming a meteroritic infall rate of 4 x 10(exp -4) g/m^2yr (Flynn and McKay 1990) and a flux of organic carbon of 2 x 10(exp -5) g/m^2yr, laboratory measurements of the UV-assisted decomposition of benzenehexacarboxylic acid (mellitic acid, a likely intermediate of kerogen oxidation), indicate its decomposition rate on Mars would exceed the total flux of organic carbon to the planet by over four orders of magnitude. Our measurements indicate that although the decomposition temperature of kerogens in some cases exceeds the temperature limit of the Viking GCMS, it is unlikely kerogens or their decomposition intermediates were present at the Viking landings sites at levels above the GCMS detection limits.

Quinn, Richard C.↗
NASA NTRS1997

Template-directed synthesis using the heterogeneous templates produced by montmorillonite catalysis. A possible bridge between the prebiotic and RNA worlds

The synthesis of oligoguanylates [oligo(G)s] is catalyzed by a template of oligocytidylates [oligo(C)s] containing 2',5'- and 3',5'-linked phosphodiester bonds with and without incorporated C5'ppC groupings. An oligo(C) template containing exclusively 2',5'-phosphodiester bonds also serves as a template for the synthesis of complementary oligo(G)s. The oligo(C) template was prepared by the condensation of the 5'-phosphorimidazolide of cytidine on montmorillonite clay. These studies establish that RNA oligomers prepared by mineral catalysis, or other routes on the primitive earth, did not have to be exclusively 3',5'-linked to catalyze template-directed synthesis, since oligo(C)s containing a variety of linkage isomers serve as templates for the formation of complementary oligo(G)s. These findings support the postulate that origin of the RNA world was initiated by the RNA oligomers produced by polymerization of activated monomers formed by prebiotic processes.

NASA Discipline Exobiology↗
NASA NTRS1982

Heterogeneous atmospheric chemistry

The present conference on heterogeneous atmospheric chemistry considers such topics concerning clusters, particles and microparticles as common problems in nucleation and growth, chemical kinetics, and catalysis, chemical reactions with aerosols, electron beam studies of natural and anthropogenic microparticles, and structural studies employing molecular beam techniques, as well as such gas-solid interaction topics as photoassisted reactions, catalyzed photolysis, and heterogeneous catalysis. Also discussed are sulfur dioxide absorption, oxidation, and oxidation inhibition in falling drops, sulfur dioxide/water equilibria, the evidence for heterogeneous catalysis in the atmosphere, the importance of heterogeneous processes to tropospheric chemistry, soot-catalyzed atmospheric reactions, and the concentrations and mechanisms of formation of sulfate in the atmospheric boundary layer.

Schryer, D. R.↗
NASA NTRS1987

High repetition rate sealed CO2 TEA lasers using heterogeneous catalysts

The significant operational advantages offered by CO2 lasers, operating in the 10.6 micron region of the spectrum, over current solid state lasers, emitting in the near IR region, have prompted increased interest in the development of compact, reliable, rugged CO2 laser sources. Perhaps the most critical aspect associated with achieving a laser compatible with military use is the development of lasers which require no gas replenishment. Sealed, single shot, CO2 TEA lasers have been available for a number of years. Stark et al were first to demonstrate reliable sealed operation in single shot CO2 TEA lasers in 1975 using gas catalysis. GEC Avionics reported the compact, environmentally qualified, MKIII CO2 TEA laser with a pulse life of greater than 10 to the 6th power pulses in 1980. A sealed laser lifetime of greater than 10 to the 6th power pulses is acceptable for single shot cases, such as direct detection rangefinders for tank laser sights. However, in many other applications, such as tracking of fast moving targets, it is essential that a repetition rate of typically 30Hz to 100Hz is employed. In such cases, a pulse lifetime of 10 to the 6th power pulses is no longer sufficient and a minimum pulse lifetime 10 to the 7th power pulses is essential to ensure a useful service life. In 1983 Stark el al described a sealed, 100Hz CO2 TEA laser, with a life of greater than 2.6 x 10 to the 6th power, which employed heterogeneous catalysis. Following this pioneering work, GEC Avionics has been engaged in the development of sealed high repetition rate lasers with a pulse lifetime of 20 million pulses.

Price, H. T.↗
NASA NTRS1990

Radiolysis of aqueous solutions of acetic acid in the presence of Na-montmorillonite

The gamma-irradiation of 0.8 mol dm-3 aqueous, oxygen-free acetic acid solutions was investigated in the presence or absence of Na-montmorillonite. H2, CH4, CO, CO2, and several polycarboxylic acids were formed in all systems. The primary characteristics observed in the latter system were: (1) Higher yield of the decomposition of acetic acid; (2) Lower yield of the formation of polycarboxylic acids; (3) No effect on the formation of methane; (4) Higher yield of the formation of carbon dioxide; and (5) The reduction of Fe3+ in the octahedral sites of Na-montmorillonite. A possible reaction scheme was proposed to account for the observed changes. The results are important in understanding heterogeneous processes in radiation catalysis and might be significant to prebiotic chemistry.

Non-NASA Center↗