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NASA NTRS1980

Cathode catalyst for primary phosphoric fuel cells

Alkylation of Vulcan XC-72 provided the most stable bond type for linking CoTAA to the surface of the carbon; this result is based on data obtained by cyclic voltammetry, pulse voltammetry and by release of 14C from bonded CoTAA. Half-cell tests at 100 C in 85% phosphoric acid showed that CoTAA bonded to the surface of carbon (Vulcan XC-72) via an alkylation procedure is a more active catalyst than is platinum based on a factor of two improvement in Tafel slope; dimeric CoTAA has catalytic activity equal to platinum. Half-cell tests also showed that bonded CoTAA catalysts do not suffer a loss in potential when air is used as a fuel rather than oxygen. Commercially available PTFE was shown to be stable for four months in 200 C 85% phosphoric acid based on lack of change in surface wetting properties, IR and physical characteristics. When stressed electrochemically in 150 C 85% phosphoric acid, PTFE also showed no changes after one month.

Walsh, F.↗

NASA NTRS1991

Kaolinite-catalyzed air oxidation of hydrazine: Consideration of several compositional, structural and energetic factors in surface activation

Clay minerals have been shown to have numerous, curious, energetic properties by virtue of ultra-violet light release which can be triggered by gentle environmental changes such as wetting and dewetting by a variety of liquids, unique among them water and hydrazine. Since both water and hydrazine play multiple key roles in the air-oxidation of hydrazine on kaolinite surfaces, this reaction would seem to have prime potential for studying interrelationships of energy storage, release and chemical reactivity of clay surfaces, capacities basic to either the Bernal or Cairns-Smith roles of minerals in the origin of life. Establishment of the capacity for stored electronic energy to significantly alter surface chemistry is important, regardless of the reaction chosen to demonstrate it. Hydrazine air oxidation is overawingly complex, given the possibilities for step-wise control and monitoring of parameters. In the light of recently extended characterization of the kaolinite and model sheet catalysts we used to study hydrazine oxidation and gamma-irradiated silica, previous studies of hydrazine air-oxidation on aluminosilicate surfaces have been reevaluated. Our former conclusion remains intact that, whereas trace structural and surface contaminants do play some role in the catalysis of oxidation, they are not the only, nor even the dominant, catalytic centers. Initial intermediates in the oxidation can now be proposed which are consistent with production via O(-)-centers as well as ferric iron centers. The greater than square dependence of the initial reaction rate on the weight of the clay is discussed in the light of these various mechanistic possibilities.

Coyne, L. M.↗

NASA NTRS2001

An Overview of the SOLVE-THESEO 2000 Campaign

Between November 1999 and April 2000, two major field experiments, the SAGE III Ozone Loss and Validation Experiment (SOLVE) and the Third European Stratospheric Experiment on Ozone (THESEO 2000), collaborated to form the largest field campaign yet mounted to study Arctic ozone loss. This international campaign involved more than 500 scientists from over 20 countries spread across the high and mid-latitudes of the northern hemisphere. The main scientific aims of SOLVE-THESEO 2000 were to study (a) the processes leading to ozone loss in the Arctic vortex and (b) the effect on ozone amounts over northern mid-latitudes. The campaign included satellites, heavy lift balloon launches, 6 different aircraft, ground stations, and scores of ozone-sonde. Campaign activities were principally conducted in 3 intensive measurement phases centered on early December 1999, late January 2000, and early March 2000. Observations made during the campaign showed that temperatures were unusually cold in the polar lower stratosphere over the course of the 1999-2000 winter. These cold temperatures resulted in the formation of extensive polar stratospheric clouds (PSCs) across the Arctic. Heterogeneous chemical reactions on the surfaces of the PSC particles produced high levels of reactive chlorine within the polar vortex by early January. This reactive chlorine catalytically destroyed about 60% of the ozone in a layer near 20 km between late January and mid-March 2000.

Newman, Paul A.↗

NASA NTRS2010

A Self-Perpetuating Catalyst for the Production of Complex Organic Molecules in Protostellar Nebulae

The formation of abundant carbonaceous material in meteorites is a long standing problem and an important factor in the debate on the potential for the origin of life in other stellar systems. Many mechanisms may contribute to the total organic content in protostellar nebulae, ranging from organics formed via ion-molecule and atom-molecule reactions in the cold dark clouds from which such nebulae collapse, to similar ion-molecule and atom-molecule reactions in the dark regions of the nebula far from the proto star, to gas phase reactions in sub-nebulae around growing giant planets and in the nebulae themselves. The Fischer-Tropsch-type (FTT) catalytic reduction of CO by hydrogen was once the preferred model for production of organic materials in the primitive solar nebula. The Haber-Bosch catalytic reduction of N2 by hydrogen was thought to produce the reduced nitrogen found in meteorites. However, the clean iron metal surfaces that catalyze these reactions are easily poisoned via reaction with any number of molecules, including the very same complex organics that they produce and both reactions work more efficiently in the hot regions of the nebula. We have demonstrated that many grain surfaces can catalyze both FTT and HB-type reactions, including amorphous iron and magnesium silicates, pure silica smokes as well as several minerals. Although none work as well as pure iron grains, and all produce a wide range of organic products rather than just pure methane, these materials are not truly catalysts.

Nuth, Joseph A.↗

NASA NTRS1988

Laboratory studies of sticking coefficients and heterogeneous reactions important in the stratosphere

The discovery of ozone depletion during spring in the Antarctic stratosphere has received wide spread attention. Both meteorological and chemical mechanisms have been used in attempts to explain this observation. The chemical theory focused on the chlorofluoromethanes released into the atmosphere. However, gas-phase, homogeneous reactions alone in the model can not adequately explain such a depletion. Heterogeneous reactions on ice surfaces could be important in the Antarctic stratosphere. These reactions are thought to convert ClONO2 and N2O5 into HNO3 in the solid phase while Cl2, HOCl, and ClNO2 are released into the stratosphere as gas-phase products. The photolysis of Cl2, HOCl, and ClNO2, then produces active chlorine which subsequently removes ozone through several catalytic cycles, including the Cl2O2 mechanism. The polar stratospheric clouds are thought to consist of mixtures of water ice, nitric acid, and sulfuric acid. Condensation of HCl onto the PSC's could provide active surfaces for heterogeneous reactions.

Leu, Ming-Taun↗

NASA NTRS2005

Development of Solid State Thermal Sensors for Aeroshell TPS Flight Applications

In-situ Thermal Protection System (TPS) sensors are required to provide verification by traceability of TPS performance and sizing tools. Traceability will lead to higher fidelity design tools, which in turn will lead to lower design safety margins, and decreased heatshield mass. Decreasing TPS mass will enable certain missions that are not otherwise feasible, and directly increase science payload. NASA Ames is currently developing two flight measurements as essential to advancing the state of TPS traceability for material modeling and aerothermal simulation: heat flux and surface recession (for ablators). The heat flux gage is applicable to both ablators and non-ablators and is therefore the more generalized sensor concept of the two with wider applicability to mission scenarios. This paper describes the continuing development of a thermal microsensor capable of surface and in-depth temperature and heat flux measurements for TPS materials appropriate to Titan, Neptune, and Mars aerocapture, and direct entry. The thermal sensor is a monolithic solid state device composed of thick film platinum RTD on an alumina substrate. Choice of materials and critical dimensions are used to tailor gage response, determined during calibration activities, to specific (forebody vs. aftbody) heating environments. Current design has maximum operating temperature of 1500K, and allowable constant heat flux of q=28.7 W/cm(sup 2), and time constants between 0.05 and 0.2 seconds. The catalytic and radiative response of these heat flux gages can also be changed through the use of appropriate coatings. By using several co-located gages with various surface coatings, data can be obtained to isolate surface heat flux components due to radiation, catalycity and convection. Selectivity to radiative heat flux is a useful feature even for an in-depth gage, as radiative transport may be a significant heat transport mechanism for porous TPS materials in Titan aerocapture.

Martinez, Ed↗

NASA NTRS2003

Current Developments in Future Planetary Probe Sensors for TPS

In-situ Thermal Protection System (TPS) sensors are required to provide traceability of TPS performance and sizing tools. Traceability will lead to higher fidelity design tools, which in turn will lead to lower design safety margins, and decreased heatshield mass. Decreasing TPS mass will enable certain missions that are not otherwise feasible, and directly increase science payload. NASA Ames is currently developing two flight measurements as essential to advancing the state of TPS traceability for material modeling and aerothermal simulation: heat flux and surface recession (for ablators). The heat flux gage is applicable to both ablators and non-ablators and is therefore the more generalized sensor concept of the two with wider applicability to mission scenarios. This paper describes the development of a microsensor capable of surface and in-depth temperature and heat flux measurements for TPS materials appropriate to Titan, Neptune, and Mars aerocapture, and direct entry. The thermal sensor will be monolithic solid state devices composed of thick film platinum RTD on an alumina substrate. Choice of materials and critical dimensions are used to tailor gage response, determined during calibration activities, to specific (forebody vs. aftbody) heating environments. Current design has maximum operating temperature of 1500 K, and allowable constant heat flux of q=28.7 watts per square centimeter, and time constants between 0.05 and 0.2 seconds. The catalytic and radiative response of these heat flux gages can also be changed through the use of appropriate coatings. By using several co-located gages with various surface coatings, data can be obtained to isolate surface heat flux components due to radiation, catalycity and convection. Selectivity to radiative heat flux is a useful feature even for an in-depth gage, as radiative transport may be a significant heat transport mechanism for porous TPS materials in Titan aerocapture. This paper also reports on progress to adapt a previously flown surface recession sensor, based on the Jupiter probe Galileo Analog Resistance Ablation Detector (ARAD), to appropriate aerocapture conditions.

Martinez, Ed↗

NASA NTRS2008

Mitigating Problems in Measuring Hypergolic Fuels

To monitor hydrazine concentrations accurately and safely, hydrazine is converted into a stable derivative that will be monitored and correlated to the actual hydrazine concentration. The hydrazine's reactivity is harnessed to produce a chemical reaction that will form a stable gas-phase derivative which will not react or decompose before it reaches the detector. Hydrazine, monomethylhydrazine, and unsymmetrical dimethylhydrazine belong to a class of compounds known as hypergolic fuels. These fuels self-ignite upon mixing with hypergolic oxidizer (dinitrogen tetroxide), without need of a spark or other ignition source. The resulting reaction produces thrust with exceptionally high energy, making these compounds particularly useful as rocket propellants. Hydrazines are also highly toxic and corrosive. The combined properties of reactivity, corrosivity, and toxicity present the potential for a leak, a disastrous situation in a hypergol-loaded system. Consequently, leak detection is of the utmost importance in protecting equipment and personnel. Hydrazine vapor quantification presents many challenges in addition to the safety concerns. The reactivity of these compounds causes thermal and catalytic decomposition, which results in significant losses. Further complications arise from the sticky nature of hydrazine. Molecules adsorb irreversibly to virtually any surface they make contact with before detection, which results in instrument drift. These properties make it difficult to accurately quantify hydrazines. Current analytical methods seek to minimize these interactions. After an extensive literature search to determine appropriate chemical reactions, a method was devised to quantify hydrazines, without the limitations of monitoring hydrazines.

Source record↗

NASA NTRS1981

Cathode catalysts for primary phosphoric acid fuel cells

Alkylation or carbon Vulcan XC-72, the support carbon, was shown to provide the most stable bond type for linking cobalt dehydrodibenzo tetraazannulene (CoTAA) to the surface of the carbon; this result is based on data obtained by cyclic voltammetry, pulse voltammetry and by release of 14C from bonded CoTAA. Half-cell tests at 100 C in 85% phosphoric acid showed that CoTAA bonded to the surface of carbon (Vulcan XC-72) via an alkylation procedure is a more active catalyst than is platinum based on a factor of two improvement in Tafel slope; dimeric CoTAA had catalytic activity equal to platinum. Half-cell tests also showed that bonded CoTAA catalysts do not suffer a loss in potential when air is used as a fuel rather than oxygen. Commercially available polytetrafluroethylene (PTFE) was shown to be unstable in the fuel cell environment with degradation occurring in 2000 hours or less. The PTFE was stressed at 200 C in concentrated phosphoric acid as well as electrochemically stressed in 150 C concentrated phosphoric acid; the surface chemistry of PTFE was observed to change significantly. Radiolabeled PTFE was prepared and used to verify that such chemical changes also occur in the primary fuel cell environment.

Source record↗

NASA NTRS2001

Mechanisms for Midlatitude Ozone Loss: Heterogeneous Chemistry in the Lowermost Stratosphere?

The question of midlatitude ozone erosion by chlorine free radical catalysis is examined. We present and analyze simultaneous, high-resolution observations of ClO, H2O, tropopause height, particle reactive surface area, and ice saturation occurrence frequency obtained from the NASA ER-2 aircraft. The objective is to test the hypothesis that the existence of cirrus clouds or cold aerosols in the first few kilometers above the tropopause at midlatitudes is responsible for increasing the ratio of chlorine free radicals to total inorganic chlorine, thus amplifying the rate of catalytic ozone destruction. The observations reveal a sharp decrease in ice saturation frequency at the tropopause, a marked degree of undersaturation just above the tropopause, a corresponding sharp gradient in the product of cold aerosol reactive surface area and reaction probability, gamma-S(sub a), and, finally, the consistent absence of enhanced concentrations of ClO immediately above the tropopause. These results suggest that midlatitude ozone loss is not controlled in situ by the mechanism of cirrus cloud and/or cold aerosol enhancement of chlorine radicals in the vicinity of the tropopause.

Smith, Jessica B.↗

NASA NTRS1980

Catalytic honeycomb combustor - Steady-state model and comparison with experiment

A steady-state lean combustion model for monolithic catalytic combustors is given. The model, consisting of several semi-global chemical reaction steps in the gas-phase and on the surface, is capable of analyzing CO and THC emissions. In the model computation presented, the influence of operating and design parameters on the minimum combustor length is studied. Special attention is given to the effect of after-bed gas-phase reaction space. Comparison with experimental data indicates good agreement in the range of parameters covered.

Tien, J. S.↗

NASA NTRS1985

Solar-Heated Gasifier

Catalytic coal and biomass gasifer system heated by solar energy. Sunlight from solar concentrator focused through quartz window onto ceramic-honeycomb absorber surface, which raises temperature of reactant steam, fluidizing gas, and reactor walls.

Qader, S. A.↗

NASA NTRS1994

The chemical reactivity of the Martian soil and implications for future missions

Possible interpretations of the results of the Viking Biology Experiments suggest that greater than 1 ppm of a thermally labile oxidant, perhaps H2O2, and about 10 ppm of a thermally stable oxidant are present in the martian soil. We reexamine these results and discuss implications for future missions, the search for organics on Mars, and the possible health and engineering effects for human exploration. We conclude that further characterization of the reactivity of the martian regolith materials is warrented-although if our present understanding is correct the oxidant does not pose a hazard to humans. There are difficulties in explaining the reactivity of the Martian soil by oxidants. Most bulk phase compounds that are capable of oxidizing H2O to O2 per the Gas Exchange Experiment (GEx) are thermally labile or unstable against reduction by atmospheric CO2. Models invoking trapped O2 or peroxynitrates (NOO2(-)) require an unlikely geologic history for the Viking Lander 2 site. Most suggested oxidants, including H2O2, are expected to decompose rapidly under martian UV. Nonetheless, we conclude that the best model for the martian soil contains oxidants produced by heterogeneous chemical reactions with a photochemically produced atmospheric oxidant. The GEx results may be due to catalytic decomposition of an unstable oxidizing material by H2O. We show that interfacial reaction sites covering less than 1% of the available soil surfaces could explain the Viking Biology Experiments results.

Zent, Aaron P.↗

NASA NTRS1991

Predicted rocket and shuttle effects on stratospheric ozone

The major chemical effluents of either solid- or liquid-fueled rockets that can potentially perturb stratospheric ozone include chlorine compounds (HCl), nitrogen compounds (NO(x)), and hydrogen compounds (H2 and H2O). Radicals (Cl, ClO, H, OH, HO2, NO, and NO2) formed directly or indirectly from rocket exhaust can cause the catalytic destruction of ozone. Other exhaust compounds that could presumably lead to ozone destruction either by direct reaction with ozone or by providing a surface for heterogeneous processes include the particulates Al2O3, ice, and soot. These topics are discussed in terms of the possible effects of rocket exhausts on stratospheric ozone.

Harwood, Robert S.↗

NASA NTRS2010

Three Methods of Detection of Hydrazines

Three proposed methods for measuring trace quantities of hydrazines involve ionization and detection of hydrazine derivatives. These methods are intended to overcome the limitations of prior hydrazine- detection methods. Hydrazine (Hz), monomethylhydrazine (MMH), and unsymmetrical dimethylhydrazine (UDMH) are hypergolic fuels and are highly reactive, toxic, and corrosive. A capability to measure concentrations of hydrazines is desirable for detecting leaks and ensuring safety in aerospace settings and in some industrial settings in which these compounds are used. One of the properties (high reactivity) that make it desirable to detect trace amounts of hydrazines also makes it difficult to detect hydrazines and measure their concentrations accurately using prior methods: significant amounts are lost to thermal and catalytic decomposition prior to detection. Further complications arise from the sticky nature of hydrazines: Sample hydrazine molecules tend to become irreversibly adsorbed onto solid surfaces with which they come into contact during transport to detectors, giving rise to drift in detector responses. In each proposed method, the reactive, sticky nature of hydrazines would be turned to advantage by providing a suitably doped substrate surface with which the hydrazines would react. The resulting hydrazine derivatives would be sufficiently less sticky and sufficiently more stable so that fewer molecules would be lost to decomposition or adsorption during transport. Consequently, it would be possible to measure concentration with more sensitivity and less error than in prior techniques. The first proposed method calls for the use of a recently developed technique known as desorption electrospray ionization (DESI), in which a pneumatically assisted micro -electrospray at ambient pressure is directed at a surface of interest. In this case, the surface of interest would be that of a substrate described above.

Griffin, Timothy↗

NASA NTRS1987

Characterization of the LTC catalyst: Performance against common air pollutants

One of the important qualities of the Low-Temperature Catalyst (LTC) is the rapid oxidation of carbon monoxide to carbon dioxide under a wide variety of conditions. The catalytic material is a palladium-copper activated complex which reacts with various contaminant molecules through a continuous oxidation/reduction cycle. The alumina substrate enhances LTC activity with its favorable surface chemistry and very high surface area. About 10 percent surface water is necessary to facilitate the oxidation of CO. This reaction shows a log-log dependence on contact time, suggesting a Langmuir-Hinshelwood mechanism. In the tube tests, LTC removed 90 to 100 percent of contaminating carbon monoxide in the temperature region of 20 to 4000 C, and at ambient over a range of 25 to 65 percent relative humidity. In contrast, NO2 is chemisorbed by the LTC/alumina material--the amount strongly dependent on temperature increases but independent of humidity. The LTC catalyst has demonstrated excellent capability to remove an important variety of hazardous pollutant gases which are common factors to poor indoor air quality. The Instapure Air Filtration System incorporates the LTC catalyst in a 50:50 mixture with activated carbon to effectively remove particulate, odors, and hazardous gases at room temperature and humidities. The ability to remove hazardous gases is unique for the category of portable air filtration equipment. The wide variety of pollutant gases that LTC removes suggests that catalytic technology is adaptable to a considerable range of commercial and industrial applications.

Collins, Marcia F.↗

NASA NTRS2013

Aerospace Fuels from Nonpetroleum Raw Materials

Recycling human metabolic and plastic wastes minimizes cost and increases efficiency by reducing the need to transport consumables and return trash, respectively, from orbit to support a space station crew. If the much larger costs of transporting consumables to the Moon and beyond are taken into account, developing waste recycling technologies becomes imperative and possibly mission enabling. Reduction of terrestrial waste streams while producing energy and/or valuable raw materials is an opportunity being realized by a new generation of visionary entrepreneurs; several relevant technologies are briefly compared, contrasted and assessed for space applications. A two-step approach to nonpetroleum raw materials utilization is presented; the first step involves production of supply or producer gas. This is akin to synthesis gas containing carbon oxides, hydrogen, and simple hydrocarbons. The second step involves production of fuel via the Sabatier process, a methanation reaction, or another gas-to-liquid technology, typically Fischer- Tropsch processing. Optimization to enhance the fraction of product stream relevant to transportation fuels via catalytic (process) development at NASA GRC is described. Energy utilization is a concern for production of fuels whether for operation on the lunar or Martian surface, or beyond. The term "green" relates to not only mitigating excess carbon release but also to the efficiency of energy usage. For space, energy usage can be an essential concern. Other issues of great concern include minimizing impurities in the product stream(s), especially those that are potential health risks and/or could de-grade operations through catalyst poisoning or equipment damage; technologies being developed to remove heteroatom impurities are discussed. Alternative technologies to utilize waste fluids, such as a propulsion option called the resistojet, are discussed. The resistojet is an electric propulsion technology with a powered thruster to vaporize and heat a propellant to high temperature, hot gases are subsequently passed through a converging-diverging nozzle expanding gases to supersonic velocities. A resistojet can accommodate many different fluids, including various reaction chamber (by-)products.

Palaszewski, B. A.↗

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↗