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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
NASA NTRS2007

Catalytic dehydrogenation of amine borane complexes

A method of generating hydrogen includes the steps of providing an amine borane (AB) complex, at least one hydrogen generation catalyst, and a solvent, and mixing these components. Hydrogen is generated. The hydrogen produced is high purity hydrogen suitable for PEM fuel cells. A hydrolytic in-situ hydrogen generator includes a first compartment that contains an amine borane (AB) complex, a second container including at least one hydrogen generation catalyst, wherein the first or second compartment includes water or other hydroxyl group containing solvent. A connecting network permits mixing contents in the first compartment with contents in the second compartment, wherein high purity hydrogen is generated upon mixing. At least one flow controller is provided for controlling a flow rate of the catalyst or AB complex.

Mohajeri, Nahid↗
NASA NTRS2009

Catalytic dehydrogenation of amine borane complexes

A method of generating hydrogen includes the steps of providing an amine borane (AB) complex, at least one hydrogen generation catalyst, and a solvent, and mixing these components Hydrogen is generated. The hydrogen produced is high purity hydrogen suitable for PEM fuel cells. A hydrolytic in-situ hydrogen generator includes a first compartment that contains an amine borane (AB) complex, a second container including at least one hydrogen generation catalyst, wherein the first or second compartment includes water or other hydroxyl group containing solvent. A connecting network permits mixing contents in the first compartment with contents in the second compartment, wherein high purity hydrogen is generated upon mixing. At least one flow controller is provided for controlling a flow rate of the catalyst or AB complex.

Mohajeri, Nahid↗
NASA NTRS2010

Hydrogen peroxide catalytic decomposition

Nitric oxide in a gaseous stream is converted to nitrogen dioxide using oxidizing species generated through the use of concentrated hydrogen peroxide fed as a monopropellant into a catalyzed thruster assembly. The hydrogen peroxide is preferably stored at stable concentration levels, i.e., approximately 50%-70% by volume, and may be increased in concentration in a continuous process preceding decomposition in the thruster assembly. The exhaust of the thruster assembly, rich in hydroxyl and/or hydroperoxy radicals, may be fed into a stream containing oxidizable components, such as nitric oxide, to facilitate their oxidation.

Parrish, Clyde F.↗
NASA NTRS2010

Cyclic catalytic upgrading of chemical species using metal oxide materials

Processes are disclosure which comprise alternately contacting an oxygen-carrying catalyst with a reducing substance, or a lower partial pressure of an oxidizing gas, and then with the oxidizing gas or a higher partial pressure of the oxidizing gas, whereby the catalyst is alternately reduced and then regenerated to an oxygenated state. In certain embodiments, the oxygen-carrying catalyst comprises at least one metal oxide-containing material containing a composition having one of the following formulas: (a) Ce.sub.xB.sub.yB'.sub.zB''O.sub..delta., wherein B=Ba, Sr, Ca, or Zr; B'=Mn, Co, or Fe; B''=Cu; 0.01<x<0.99; 0<y<0.6; 0<z<0.5; and 1<.delta.<2.2; (b) Sr.sub.vLa.sub.wB.sub.xB'.sub.yB''.sub.zO.sub..delta., wherein B=Co or Fe; B'=Al or Ga; B''=Cu; 0.01<v<1.4; 0.1<w<1.6; 0.1<x<1.9; 0.1<y<0.9; 0<z<2.2; and 3<.delta.<5.5).

White, James H.↗
NASA NTRS2011

Catalytic Generation of Lift Gases for Balloons

A lift-gas cracker (LGC) is an apparatus that generates a low-molecular-weight gas (mostly hydrogen with smaller amounts of carbon monoxide and/or carbon dioxide) at low gauge pressure by methanol reforming. LGCs are undergoing development for use as sources of buoyant gases for filling zero-gauge-pressure meteorological and scientific balloons in remote locations where heavy, high-pressure helium cylinders are not readily available. LGCs could also be used aboard large, zero-gauge-pressure, stratospheric research balloons to extend the duration of flight.

Zubrin, Robert↗
NASA NTRS2011

Possible Increase in Nitric Oxide Production by Lightning Discharges Due to Catalytic Effects of Ice Particles

We address the question of whether ice crystals with habits typically encountered by lightning discharges may serve as catalysts for the production of NOx by lightning. If so, and if the effect is sufficiently large, it would need to be taken into account in estimates of global NOx production by lightning. In this study, we make a series of plausible assumptions about the temperatures and concentrations of reactant species in the environment of discharges and we postulate a mechanism by which ice crystals could adsorb nitrogen atoms. We then compare production rates between uncatalyzed and catalyzed reactions at 2000 K, 3000 K, and 4000 K, temperatures observed in lightning channels during the cool-down period after a return stroke. Catalyzed NO production rates are greater at 2000 K, whereas uncatalyzed production occurs most rapidly at 4000 K. The channel temperature stays around 2000 K for a longer period of time than at 4000 K. The longer residence time at 2000 K is sufficient to allow fresh reactants to participate in the mix in. Therefore, our results suggest that nearly three times as much NO per flash is produced by ice-catalyzed reactions as compared with uncatalyzed reactions.

Peterson, Harold↗
NASA NTRS2012

Development of a Catalytic Wet Air Oxidation Method to Produce Feedstock Gases from Waste Polymers

Given the high cost of space launch, the repurposing of biological and plastic wastes to reduce the need for logistical support during long distance and long duration space missions has long been recognized as a high priority. Described in this paper are the preliminary efforts to develop a wet air oxidation system in order to produce fuels from waste polymers. Preliminary results of partial oxidation in near supercritical water conditions are presented. Inherent corrosion and salt precipitation are discussed as system design issues for a thorough assessment of a second generation wet air oxidation system. This work is currently being supported by the In-Situ Resource Utilization Project.

Kulis, Michael J.↗
NASA NTRS2014

Organic Analysis of Catalytic Fischer-Tropsch Type Synthesis Products: Are they Similar to Organics in Chondritic Meteorites?

Fischer-Tropsch Type (FTT) synthesis of organic compounds has been hypothesized to occur in the early solar nebula that formed our Solar System. FTT is a collection of abiotic chemical reactions that convert a mixture of carbon monoxide and hydrogen over nano-catalysts into hydrocarbons and other more complex aromatic compounds. We hypothesized that FTT can generate similar organic compounds as those seen in chondritic meteorites; fragments of asteroids that are characteristic of the early solar system. Specific goals for this project included: 1) determining the effects of different FTT catalyst, reaction temperature, and cycles on organic compounds produced, 2) imaging of organic coatings found on the catalyst, and 3) comparison of organic compounds produced experimentally by FTT synthesis and those found in the ordinary chondrite LL5 Chelyabinsk meteorite. We used Pyrolysis Gas Chromatography Mass Spectrometry (PY-GCMS) to release organic compounds present in experimental FTT and meteorite samples, and Scanning Electron Microscopy (SEM) to take images of organic films on catalyst grains.

Yazzie, Cyriah A.↗
NASA NTRS2013

Cyclic Catalytic Upgrading of Chemical Species Using Metal Oxide Materials

Processes are disclosure which comprise alternately contacting an oxygen-carrying catalyst with a reducing substance, or a lower partial pressure of an oxidizing gas, and then with the oxidizing gas or a higher partial pressure of the oxidizing gas, whereby the catalyst is alternately reduced and then regenerated to an oxygenated state. In certain embodiments, the oxygen-carrying catalyst comprises at least one metal oxide-containing material containing a composition having the following formulas: (a) Ce(sub x)B(sub y)B'(sub z)B''O(sub gamma; wherein B=Ba, Sr, Ca, or Zr; B'=Mn, Co, and/or Fe; B''=Cu; 0.01<x<0.99; 0<y<0.6; 0<z<0.5; (b) Ce(sub 1-x-y) Ni(sub x) B(sub y) O(sub 2-*), wherein B=Zr, Ba, Ca, La, or K; 0.02<x<0.1; 0<y<0.1; and 0.02<*<0.15; and 1<delta<2.2 and (c) coal ash either as a catalyst material itself or as a support for said unary or binary metal oxides.

White, James H.↗
NASA NTRS2015

Pyrolysis-GCMS Analysis of Solid Organic Products from Catalytic Fischer-Tropsch Synthesis Experiments

Abiotic synthesis of complex organic compounds in the early solar nebula that formed our solar system is hypothesized to occur via a Fischer-Tropsch type (FTT) synthesis involving the reaction of hydrogen and carbon monoxide gases over metal and metal oxide catalysts. In general, at low temperatures (less than 200 C), FTT synthesis is expected to form abundant alkane compounds while at higher temperatures (greater than 200 C) it is expected to product lesser amounts of n-alkanes and greater amounts of alkene, alcohol, and polycyclic aromatic hydrocarbons (PAHs). Experiments utilizing a closed-gas circulation system to study the effects of FTT reaction temperature, catalysts, and number of experimental cycles on the resulting solid insoluble organic products are being performed in the laboratory at NASA Goddard Space Flight Center. These experiments aim to determine whether or not FTT reactions on grain surfaces in the protosolar nebula could be the source of the insoluble organic matter observed in meteorites. The resulting solid organic products are being analyzed at NASA Johnson Space Center by pyrolysis gas chromatography mass spectrometry (PY-GCMS). PY-GCMS yields the types and distribution of organic compounds released from the insoluble organic matter generated from the FTT reactions. Previously, exploratory work utilizing PY-GCMS to characterize the deposited organic materials from these reactions has been reported. Presented here are new organic analyses using magnetite catalyst to produce solid insoluble organic FTT products with varying reaction temperatures and number of experimental cycles.

Locke, Darren R.↗
NASA NTRS2015

Bulk Preparation of Holey Graphene via Controlled Catalytic Oxidation

A scalable method allows preparation of bulk quantities of holey carbon allotropes with holes ranging from a few to over 100 nm in diameter. Carbon oxidation catalyst nanoparticles are first deposited onto a carbon allotrope surface in a facile, controllable, and solvent-free process. The catalyst-loaded carbons are then subjected to thermal treatment in air. The carbons in contact with the carbon oxidation catalyst nanoparticles are selectively oxidized into gaseous byproducts such as CO or CO.sub.2, leaving the surface with holes. The catalyst is then removed via refluxing in diluted nitric acid to obtain the final holey carbon allotropes. The average size of the holes correlates strongly with the size of the catalyst nanoparticles and is controlled by adjusting the catalyst precursor concentration. The temperature and time of the air oxidation step, and the catalyst removal treatment conditions, strongly affect the morphology of the holes.

Watson, Kent↗
NASA NTRSDate not supplied

In Vitro Selections with RNAs of Variable Length Converge on a Robust Catalytic Core

In vitro selection is a powerful tool that can be used to understand basic principles of molecular evolution. We used in vitro selection to understand how changes in length and the accumulation of point mutations enable the evolution of functional RNAs. Using RNA populations of various lengths, we performed a series of in vitro experiments to select for ribozymes with RNA ligase activity. We identified a core ribozyme structure that was robust to changes in RNA length, high levels of mutagenesis, and increased selection pressure. Elaboration on this core structure resulted in improved activity which we show is consistent with a larger trend among functional RNAs in which increasing motif size can lead to an exponential improvement in fitness. We conclude that elaboration on conserved core structures is a preferred mechanism in RNA evolution. This conclusion, drawn from selections of RNAs from random sequences, is consistent with proposed evolutionary histories of specific biological RNAs. More generally, our results indicate that modern RNA structures can be used to infer ancestral structures. Our observations also suggest a mechanism by which structural outcomes of early RNA evolution would be largely reproducible even though RNA fitness landscapes consist of disconnected clusters of functional sequences.

In vitro evolution↗
NASA NTRS1997

The Effect of Diffusional Transport and Surface Catalysis on the Aerothermodynamic Heating for Martian Atmospheric Entry

For the reentry heating of 70-degree blunt sphere-cones entering Mars at velocities in excess of 6 km/sec, a study was performed to determine the magnitude of both convective and catalytic heating on the cone forebody. Case studies of the peak heating conditions for the current NASA Mars Pathfinder entry probe, as well as the peak heating conditions of the proposed NASA Mars 2001 aerobraking orbiter mission were performed. Since the actual behavior of the chemical recombination of Mars atmosphere hypersonic shock layer species on heat shield materials is not known, and no experimental studies of any consequence have been done to determine surface reaction rates for the CO2 system, a parametric analysis of various reaction schemes and surface catalytic mechanistic models was performed. In many cases the actual Mars entry probe will have a heat shield composed of an ablative material which can either partially or completely preclude the existence of catalytic surface recombination phenomena. The extent of this blockage effect has not been examined at this time and is not considered in this effort. Instead only non-ablative computations are performed to separately evaluate the full extent of the surface catalysis and related diffusional phenomena. Parametric studies include peak heating point comparisons of non-catalytic, partially catalytic and fully catalytic total surface heat transfer for three difference surface recombination catalytic mechanisms (with and without simultaneous CO + O and O + O recombination) as well as with different species diffusion models. Diffusion model studies include constant Schmidt number (equal diffusivities) and the bifurcation, approximate multi-component diffusion model. Since the gas phase reaction kinetics for the Mars CO2 based atmosphere have also not been validated, the effect of two different (fast and slow) sets of gas kinetics on heat transfer is presented.

Henline, William D.↗
NASA NTRS2008

Nano-Engineered Catalysts for Direct Methanol Fuel Cells

Nano-engineered catalysts, and a method of fabricating them, have been developed in a continuing effort to improve the performances of direct methanol fuel cells as candidate power sources to supplant primary and secondary batteries in a variety of portable electronic products. In order to realize the potential for high energy densities (as much as 1.5 W h/g) of direct methanol fuel cells, it will be necessary to optimize the chemical compositions and geometric configurations of catalyst layers and electrode structures. High performance can be achieved when catalyst particles and electrode structures have the necessary small feature sizes (typically of the order of nanometers), large surface areas, optimal metal compositions, high porosity, and hydrophobicity. The present method involves electrodeposition of one or more catalytic metal(s) or a catalytic-metal/polytetrafluoroethylene nanocomposite on an alumina nanotemplate. The alumina nanotemplate is then dissolved, leaving the desired metal or metal/polytetrafluoroethylene-composite catalyst layer. Unlike some prior methods of making fine metal catalysts, this method does not involve processing at elevated temperature; all processing can be done at room temperature. In addition, this method involves fewer steps and is more amenable to scaling up for mass production. Alumina nanotemplates are porous alumina membranes that have been fabricated, variously, by anodizing either pure aluminum or aluminum that has been deposited on silicon by electronbeam evaporation. The diameters of the pores (7 to 300 nm), areal densities of pores (as much as 7 x 10(exp 10)sq cm), and lengths of pores (up to about 100 nm) can be tailored by selection of fabrication conditions. In a given case, the catalytic metal, catalytic metal alloy, or catalytic metal/ polytetrafluoroethylene composite is electrodeposited in the pores of the alumina nanotemplate. The dimensions of the pores, together with the electrodeposition conditions, determine the sizes and surface areas of the catalytic particles. Hence, the small features and large surface areas of the porosity translate to the desired small particle size and large surface area of the catalyst (see figure). When polytetrafluoroethylene is included, it is for the purpose of imparting hydrophobicity in order to prevent water from impeding the desired diffusion of gases through the catalyst layer. To incorporate polytetrafluoroethylene into a catalytic-metal/polytetrafluoroethylene nanocomposite, one suspends polytetrafluoroethylene nanoparticles in the electrodeposition solution. The polytetrafluoroethylene content can be varied to obtain the desired degree of hydrophobicity and permeability by gas.

Myung, Nosang↗
NASA NTRS1995

Supporting technology for the development of Controlled Ecological Life Support Systems (CELSS)

To support the development of Controlled Ecological Life Support Systems (CELSS) in the space program, a metabolic simulator has been selected for use in a closed chamber to test functions of the CELSS. This metabolic simulator is a catalytic reactor which oxidizes the methyl acetate to produce carbon dioxide and water vapor. In this project, kinetic studies of catalytic oxidation of methyl acetate were conducted using monolithic and pellet catalysts with 0.5% (by weight) platinum (Pt) on aluminum oxide (Al2O3). The reaction was studied at a pressure of one atmosphere and at temperatures varying from 160 C to 420 C. By-products were identified at the exit of the preheater and reactor. For the kinetic study with the monolithic catalyst, a linear regression method was used to correlate the kinetic data with zero-order, first-order and Langmuir-Hinshelwood models. Results indicate that the first-order model represents the data adequately at low concentrations of methyl acetate. For higher concentrations of methyl acetate, the Langmuir-Hinshelwood model best represents the kinetic data. Both rate constant and adsorption equilibrium constants were estimated from the regression. A Taguchi orthogonal array (L(sub 9)) was used to investigate the effects of temperature, flow rate, and concentration on the catalytic oxidation of methyl acetate. For the monolithic catalyst, temperature exerts the most significant effect, followed by concentration of methyl acetate. For the pellet catalyst, reaction temperature is the most significant factor, followed by gas flow rate and methyl acetate concentration. Concentrations of either carbon dioxide or oxygen were seen to have insignificant effect on the methyl acetate conversion process. Experimental results indicate that the preheater with glass beads can accomplish thermal cracking and catalytic reaction of methyl acetate to produce acetic acid, methanol, methyl formate, and 1-propanol. The concentration of all by-products was measured in ppmv (parts per million by volume). At higher temperatures, greater amounts of these products are produced, as expected. In all cases, methanol was the predominant concentration detected, followed by methyl formate. At temperatures lower than 320 C for the P-type monolithic catalyst, methanol, acetic acid, and acetone were detected, whereas, for the E-type monolithic catalyst, only methanol was detected at 160 C. Both P and E types of the monolithic catalyst were specified with the same substrates (ceramic), washcoat (Al2O3), and promoter (Pt). However, the manufacturing and treatment procedures were quite different. It was therefore concluded that the performance of the E-type monolithic catalyst is superior to that of the P-type for oxidation of methyl acetate. At higher reaction temperatures, e.g., above 420 C, all reactants and byproducts were completely oxidized using these two types of monolithic catalyst to produce carbon dioxide and water vapor. A complex heterogenous catalytic reaction mechanism was proposed to explain the formation of the byproducts (methanol, acetic acid, and methyl formate) as the methyl acetate traveled through the preheater packed with glass beads. The by-product, 1-propanol, may be formed only through a homogeneous reaction, since it is difficult to develop a reasonable sequence of heterogeneous reaction steps to explain its formation. The homogeneous thermal decomposition of methyl acetate to form free radicals was proposed to explain the formation of 1-propanol, and also methanol, in the preheater. A dual-site catalytic reaction mechanism was proposed for the oxidation of methyl acetate over Pt/Al2O3 monolithic catalyst. The dual-site mechanism describes the chemisorption of oxygen molecules as well as a physical adsorption of methyl acetate on the active sites. On the active sites, methyl acetate is oxidized rapidly to form carbon dioxide and water vapor. A rate equation derived from this mechanism gives the Langmuir-Hinshelwood rate formula which has been observed from the experimental data obtained in this project for high methyl acetate concentration (greater than 1000 ppmv) over a monolithic catalyst. If the oxygen concentration is very high and methyl acetate concentration is very low, the reaction rate equation is then reduced to a first-order with respect to methyl acetate concentration. The first-order model has also been observed from the experimental data obtained in this project for low methyl acetate concentration (less than 1000 ppmv).

Li, Ku-Yen↗
NASA NTRS1991

Controlled evolution of an RNA enzyme

It is generally thought that prior to the origin of protein synthesis, life on earth was based on self-replicating RNA molecules. This idea has become especially popular recently due to the discovery of catalytic RNA (ribozymes). RNA has both genotypic and phenotypic properties, suggesting that it is capable of undergoing Darwinian evolution. RNA evolution is likely to have played a critical role in the early history of life on earth, and thus is important in considering the possibility of life elsewhere in the solar system. We have constructed an RNA-based evolving system in the laboratory, combining amplification and mutation of an RNA genotype with selection of a corresponding RNA phenotype. This system serves as a functional model of a primitive organism. It can also be used as a tool to explore the catalytic potential of RNA. By altering the selection constraints, we are attempting to modify the substrate specificity of an existing ribozyme in order to develop ribozymes with novel catalytic function. In this way, we hope to gain a better understanding of RNA's catalytic versatility and to assess its suitability for the role of primordial catalyst. All of the RNA enzymes that are known to exist in contemporary biology carry out cleavage/ligation reactions involving RNA substrates. The Tetrahymena ribozyme, for example, catalyzes phosphoester transfer between a guanosine containing and an oligopyrimidine containing substrate. We tested the ability of mutant forms of the Tetrahymena ribozyme to carry out a comparable reaction using DNA, rather than RNA substrate. An ensemble of structural variants of the ribozyme was prepared and tested for their ability to specifically cleave d(GGCCCTCT-A3TA3TA) at the phosphodiester bond following the sequence CCCTCT. We recovered a mutant form of the enzyme that cleaves DNA more efficiently than does the wild-type. Beginning with this selected mutant we have now scattered random mutations throughout the ribozyme and have begun an evolutionary search to further expand the catalytic repertoire of RNA.

Joyce, G. F.↗
NASA NTRS1995

Analytical studies of hypersonic viscous dissociated flows

This project primarily dealt with integral boundary-layer solution techniques that are directly applicable to the problem of determining aerodynamic heating rates of hypersonic vehicles like X-33 in the vicinity of stagnation points, windward centerlines, and swept-wing leading edges. The analyses include effects of finite-rate gas chemistry across the boundary layer and finite-rate catalysis of atom recombination at the surface. A new approach for combining the insight afforded by integral boundary-layer analysis with comprehensive (and expensive) computational fluid dynamic (CFD) flowfield solutions of the thin-layer Navier-Stokes equations was developed. The approach extracts CFD derived quantities at the wall and at the boundary layer edge for inclusion in a post-processing boundary-layer analysis. The post-processed data base allows a designer at a workstation to ask and answer the following questions: (1) How much does the heating change if one uses a thermal protection system (TPS) with different catalytic properties than was used in the original CFD solution? (2) How does the heating change when one moves the interface of two different TPS materials with different catalytic efficiencies for the purpose of reducing vehicle weight and expense? The answer to the second question is particularly critical, because abrupt changes from low catalytic efficiency to high catalytic efficiency can lead to localized increase in heating which exceeds the usually conservative estimate provided by a fully catalytic wall assumption. A secondary issue that was addressed involves the prediction of heating levels in the vicinity of sharp corners that are transverse to or aligned with the flow. An example of the first case is heating at the edge of the COMET reentry module. An example of the second case is heating along the side edge of a deflected body flap on an SSV. The difficulty of putting grids in the vicinity of such corners with continuously varying metric coefficients causes problems in CFD predictions. A preliminary theory for prediction that says the heating at the corner is X percent of the heating N boundary-layer thicknesses inboard was developed. This will prove useful to analytically evaluate the possible benefits of rounding the edges of these configurations and defining how much rounding is sufficient.

Inger, George R.↗