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NASA NTRS1989

Electrocatalysts for oxygen electrodes in fuel cells and water electrolyzers for space applications

In most instances separate electrocatalysts are needed to promote the reduction of O2 in the fuel cell mode and to generate O2 in the energy storage-water electrolysis mode in aqueous electrochemical systems operating at low and moderate temperatures (T greater than or equal to 200 C). Interesting exceptions are the lead and bismuth ruthenate pyrochlores in alkaline electrolytes. These catalysts on high area carbon supports have high catalytic activity for both O2 reduction and generation (1,2). Rotating ring-disk electrode measurements provide evidence that the O2 reduction proceeds by a parallel four-electron pathway. The ruthenates can also be used as self-supported catalysts to avoid the problems associated with carbon oxidation, but the electrode performance so far achieved in the research at Case Western Reserve University (CWRU) is considerably less. At the potentials involved in the anodic mode the ruthenate pyrochlores have substantial equilibrium solubility in concentrated alkaline electrolyte. This results in the loss of catalyst into the bulk solution and a decline in catalytic activity. Furthermore, the hydrogen generation counter electrode may become contaminated with reduction products from the pyrochlores (lead, ruthenium). A possible approach to this problem is to immobilize the pyrochlore catalyst within an ionic-conducting solid polymer, which would replace the fluid electrolyte within the porous gas diffusion O2 electrode. For bulk alkaline electrolyte, an anion-exchange polymer is needed with a transference number close to unity for the Oh(-) ion. Preliminary short-term measurements with lead ruthenates using a commercially available partially-fluorinated anion-exchange membrane as an overlayer on the porous gas-fed electrode indicate lower anodic polarization and virtually unchanged cathodic polarization.

Prakash, Jai↗

NASA NTRS2002

Characterization of Truncated Tumor-Associated NADH Oxidase (ttNOX)

Bacterial, plant and animal cells possess novel surface proteins that exhibit both NADH oxidation (NOX) or hydroquinone and protein disulfide-thiol interchange. These enzymatic activities alternate to yield oscillating patterns wjth period lengths of approximately 24 minutes. The catalytic period of NOX proteins are temperature compensated and gravity responsive. We report the cloning, expression and characterization of truncated tumor-associated NADH oxidase (ttNOX), in which the membrane spanning region has been deleted. The cDNA (originated from HeLa cells) was cloned into pET-34b and pET-14b (Novagen) vectors for E. coli expression. Optimized expression and purification protocols yielded greater than 300mg per liter of culture with greater than 95% purity. Circular dichroism data was collected from a 2.7mg/ml solution in a 0.1mm cuvette with variable scanning using an Olis RSM CD spectrophotometer. The ellipticity values were scanned from 190 to 260nm. The spectra recorded have characteristics for alpha proteins with band maxima at 216nm and a possible shoulder at 212nm at 12OC and 250 C. Protein crystal screens are in progress and, to date, only small crystals have been observed. The regular periodic oscillatory change in the ttNOX protein is indicative of a possible time-keeping functional role. A single protein possessing alternating catalytic activities, with a potential biological clock function, is unprecedented and structural determination is paramount to understanding this role.

Karr, Laurel J.↗

NASA NTRS2014

CO2 Reduction Assembly Prototype Using Microlith-Based Sabatier Reactor for Ground Demonstration

The utilization of CO2 to produce life support consumables, such as O2 and H2O, via the Sabatier reaction is an important aspect of NASA's cabin Atmosphere Revitalization System (ARS) and In-Situ Resource Utilization (ISRU) architectures for both low-earth orbit and long-term manned space missions. Carbon dioxide can be reacted with H2, obtained from the electrolysis of water, via Sabatier reaction to produce methane and H2O. Methane can be stored and utilized as propellant while H2O can be either stored or electrolyzed to produce oxygen and regain the hydrogen atoms. Depending on the application, O2 can be used to replenish the atmosphere in human-crewed missions or as an oxidant for robotic and return missions. Precision Combustion, Inc. (PCI), with support from NASA, has previously developed an efficient and compact Sabatier reactor based on its Microlith® catalytic technology and demonstrated the capability to achieve high CO2 conversion and CH4 selectivity (i.e., ≥90% of the thermodynamic equilibrium values) at high space velocities and low operating temperatures. This was made possible through the use of high-heat-transfer and high-surface-area Microlith catalytic substrates. Using this Sabatier reactor, PCI designed, developed, and demonstrated a stand-alone CO2 Reduction Assembly (CRA) test system for ground demonstration and performance validation. The Sabatier reactor was integrated with the necessary balance-of-plant components and controls system, allowing an automated, single "push-button" start-up and shutdown. Additionally, the versatility of the test system prototype was demonstrated by operating it under H2-rich (H2/CO2 of >4), stoichiometric (ratio of 4), and CO2-rich conditions (ratio of <4) without affecting its performance and meeting the equilibrium-predicted water recovery rates. In this paper, the development of the CRA test system for ground demonstration will be discussed. Additionally, the performance results from testing the system at various operating conditions and the results from durability testing will be presented.

Junaedi, Christian↗

NASA NTRS1987

Catalysts for long-life closed-cycle CO2 lasers

Long-life, closed-cycle operation of pulsed CO2 lasers requires catalytic CO-O2 recombination both to remove O2, which is formed by discharge-induced CO2 decomposition, and to regenerate CO2. Platinum metal on a tin (IV) oxide substrate (Pt/SnO2) has been found to be an effective catalyst for such recombination in the desired temperature range of 25 to 100 C. This paper presents a description of ongoing research at NASA-LaRC on Pt/SnO2 catalyzed CO-O2 recombination. Included are studies with rare-isotope gases since rare-isotope CO2 is desirable as a laser gas for enhanced atmospheric transmission. Results presented include: (1) achievement of 98% to 100% conversion of a stoichiometric mixture of CO and O2 to CO2 for 318 hours (greater than 1 x 10 to the 6th power seconds), continuous, at a catalyst temperature of 60 C, and (2) development of a technique verified in a 30-hour test, to prevent isotopic scrambling when CO-18 and O-18(2) are reacted in the presence of a common-isotope Pt/Sn O-16(2) catalyst.

Schryer, David R.↗

NASA NTRS1987

Research on catalysts for long-life closed-cycle CO2 laser oaperation

Long-life, closed-cycle operation of pulsed CO2 lasers requires catalytic CO-O2 recombination both to remove O2, which is formed by discharge-induced CO2 decomposition, and to regenerate CO2. Platinum metal on a tin-oxide substrate (Pt/SnO2) has been found to be an effective catalyst for such recombination in the desired temperature range of 25 to 100 C. This paper presents a description of ongoing research at NASA-Langley on Pt/SnO2 catalyzed CO-O2 recombination. Included are studies with rare-isotope gases since rare-isotope CO2 is desirable as a laser gas for enhanced atmospheric transmission. Results presented include: (1) the effects of various catalyst pretreatment techniques on catalyst efficiency; (2) development of a technique, verified in a 30-hour test, to prevent isotopic scrambling when C(O-18) and (O-18)2 are reacted in the presence of a common-isotope Pt/Sn(O-16)2 catalyst; and (3) development of a mathematical model of a laser discharge prior to catalyst introduction.

Sidney, Barry D.↗

NASA NTRS2011

Catalytic Microtube Rocket Igniter

Devices that generate both high energy and high temperature are required to ignite reliably the propellant mixtures in combustion chambers like those present in rockets and other combustion systems. This catalytic microtube rocket igniter generates these conditions with a small, catalysis-based torch. While traditional spark plug systems can require anywhere from 50 W to multiple kW of power in different applications, this system has demonstrated ignition at less than 25 W. Reactants are fed to the igniter from the same tanks that feed the reactants to the rest of the rocket or combustion system. While this specific igniter was originally designed for liquid methane and liquid oxygen rockets, it can be easily operated with gaseous propellants or modified for hydrogen use in commercial combustion devices. For the present cryogenic propellant rocket case, the main propellant tanks liquid oxygen and liquid methane, respectively are regulated and split into different systems for the individual stages of the rocket and igniter. As the catalyst requires a gas phase for reaction, either the stored boil-off of the tanks can be used directly or one stream each of fuel and oxidizer can go through a heat exchanger/vaporizer that turns the liquid propellants into a gaseous form. For commercial applications, where the reactants are stored as gases, the system is simplified. The resulting gas-phase streams of fuel and oxidizer are then further divided for the individual components of the igniter. One stream each of the fuel and oxidizer is introduced to a mixing bottle/apparatus where they are mixed to a fuel-rich composition with an O/F mass-based mixture ratio of under 1.0. This premixed flow then feeds into the catalytic microtube device. The total flow is on the order of 0.01 g/s. The microtube device is composed of a pair of sub-millimeter diameter platinum tubes connected only at the outlet so that the two outlet flows are parallel to each other. The tubes are each approximately 10 cm long and are heated via direct electric resistive heating. This heating brings the gasses to their minimum required ignition temperature, which is lower than the auto-thermal ignition temperature, and causes the onset of both surface and gas phase ignition producing hot temperatures and a highly reacting flame. The combustion products from the catalytic tubes, which are below the melting point of platinum, are injected into the center of another combustion stage, called the primary augmenter. The reactants for this combustion stage come from the same source but the flows of non-premixed methane and oxygen gas are split off to a secondary mixing apparatus and can be mixed in a near-stoichiometric to highly lean mixture ratio. The primary augmenter is a component that has channels venting this mixed gas to impinge on each other in the center of the augmenter, perpendicular to the flow from the catalyst. The total crosssectional area of these channels is on a similar order as that of the catalyst. The augmenter has internal channels that act as a manifold to distribute equally the gas to the inward-venting channels. This stage creates a stable flame kernel as its flows, which are on the order of 0.01 g/s, are ignited by the combustion products of the catalyst. This stage is designed to produce combustion products in the flame kernel that exceed the autothermal ignition temperature of oxygen and methane.

Schneider, Steven J.↗

NASA NTRS1990

Non-catalytic coatings for hypersonic vehicle applications

CVD coatings of boron-oxygen-silicon and aluminum-boron-oxygen and silicon compositions were applied to alpha 2 and gamma titanium-aluminide alloys, and tested under simulated earth reentry conditions to evaluate oxidation protection, recombination effifiency and total emittance under cyclic exposures between temperatures of 300 and 1255 K. The degree of oxidation protection afforded to the alloys was evaluated from the amount of specimen weight gain after a 100 hour exposure to air at atmospheric pressure and at a temperature of 1255 K. Data are presented for two types of coatings, a monolithic and a multilayer, which have recombination efficiencies from 0.005 to 0.020 after ten one-half hour long simulated reentry cycles. Total normal emittance was 0.80 or greater and weight gain was less than 10 g/sq m both coating types. Compositional and morphological changes resulting from the exposures are discussed in relation to time-dependent variations in recombination efficiency.

Cunnington, G. R.↗

NASA NTRS1994

Water Purification

The Vision Catalyst Purifier employs the basic technology developed by NASA to purify water aboard the Apollo spacecraft. However, it also uses an "erosion" technique. The purifier kills bacteria, viruses, and algae by "catalytic corrosion." A cartridge contains a silver-impregnated alumina bed with a large surface area. The catalyst bed converts oxygen in a pool of water to its most oxidative state, killing over 99 percent of the bacteria within five seconds. The cartridge also releases into the pool low levels of ionic silver and copper through a controlled process of erosion. Because the water becomes electrochemically active, no electricity is required.

Source record↗

NASA NTRS2008

Carbothermal Processing of Lunar Regolith Using Methane

The processing of lunar regolith for the production of oxygen is a key component of the In-Situ Resource Utilization plans currently being developed by NASA. Among various candidate processes, the modeling of oxygen production by hydrogen reduction, molten salt electrolysis, and carbothermal processing are presently being pursued. In the carbothermal process, a portion of the surface of the regolith in a container is heated by exposure to a heat source such as a laser beam or a concentrated solar heat flux, so that a small zone of molten regolith is established. The molten zone is surrounded by solid regolith particles that are poor conductors of heat. A continuous flow of methane is maintained over the molten regolith zone. Our model is based on a mechanism where methane pyrolyzes when it comes in contact with the surface of the hot molten regolith to form solid carbon and hydrogen gas. Carbon is deposited on the surface of the melt, and hydrogen is released into the gas stream above the melt surface. We assume that the deposited carbon mixes in the molten regolith and reacts with metal oxides in a reduction reaction by which gaseous carbon monoxide is liberated. Carbon monoxide bubbles through the melt and is released into the gas stream. Oxygen is produced subsequently by (catalytically) processing the carbon monoxide downstream. In this paper, we discuss the development of a chemical conversion model of the carbothermal process to predict the rate of production of carbon monoxide.

Balasubramaniam, R.↗

NASA NTRS2009

Carbothermal Processing of Lunar Regolith Using Methane

Balasubramaniam, R.↗

NASA NTRS1979

The advanced low-emissions catalytic-combuster program. Phase 1: Description and status

An overview of the ongoing program is presented. Objectives, plan, schedule, pollution and performance goals, catalyst advantages, present problems, and the present status of identified combustor concepts are discussed. The possible increase in upper atmosphere oxides of nitrogen (NOx) levels due to aircraft number density increases was predicted to adversely decrease ozone concentration levels. A technique for achieving low NOx emission levels was experimentally demonstrated with a lean, premixing prevaporizing flame-tube combustor.

Szaniszlo, A. J.↗

NASA NTRS1990

Fuel-rich catalytic combustion: A fuel processor for high-speed propulsion

Fuel-rich catalytic combustion of Jet-A fuel was studied over the equivalence ratio range 4.7 to 7.8, which yielded combustion temperatures of 1250 to 1060 K. The process was soot-free and the gaseous products were similar to those obtained in the iso-octane study. A carbon atom balance across the catalyst bed calculated for the gaseous products accounted for about 70 to 90 percent of the fuel carbon; the balance was condensed as a liquid in the cold trap. It was shown that 52 to 77 percent of the fuel carbon was C1, C2, and C3 molecules. The viability of using fuel-rich catalytic combustion as a technique for preheating a practical fuel to very high temperatures was demonstrated. Preliminary results from the scaled up version of the catalytic combustor produced a high-temperature fuel containing large amounts of hydrogen and carbon monoxide. The balance of the fuel was completely vaporized and in various stages of pyrolysis and oxidation. Visual observations indicate that there was no soot present.

Brabbs, Theodore A.↗

NASA NTRS1990

Fuel-rich catalytic combustion - A fuel processor for high-speed propulsion

Fuel-rich catalytic combustion of Jet-A fuel was studied over the equivalence ratio range 4.7 to 7.8, which yielded combustion temperatures of 1250 to 1060 K. The process was soot-free and the gaseous products were similar to those obtained in the iso-octane study. A carbon atom balance across the catalyst bed calculated for the gaseous products accounted for about 70 to 90 percent of the fuel carbon; the balance was condensed as a liquid in the cold trap. It was shown that 52 to 77 percent of the fuel carbon was C1, C2, and C3 molecules. The viability of using fuel-rich catalytic combustion as a technique for preheating a practical fuel to very high temperatuers was demonstrated. Preliminary results from the scaled up version of the catalytic combustor produced a high-temperature fuel containing large amounts of hydrogen and carbon monoxide. The balance of the fuel was completely vaporized and in various stages of pyrolysis and oxidation. Visual observations indicate that there was no soot present.

Brabbs, Theodore A.↗

NASA NTRS2005

Sol-Gel Process for Making Pt-Ru Fuel-Cell Catalysts

A sol-gel process has been developed as a superior alternative to a prior process for making platinum-ruthenium alloy catalysts for electro-oxidation of methanol in fuel cells. The starting materials in the prior process are chloride salts of platinum and ruthenium. The process involves multiple steps, is time-consuming, and yields a Pt-Ru product that has relatively low specific surface area and contains some chloride residue. Low specific surface area translates to incomplete utilization of the catalytic activity that might otherwise be available, while chloride residue further reduces catalytic activity ("poisons" the catalyst). In contrast, the sol-gel process involves fewer steps and less time, does not leave chloride residue, and yields a product of greater specific area and, hence, greater catalytic activity. In this sol-gel process (see figure), the starting materials are platinum(II) acetylacetonate [Pt(C5H7O2)2, also denoted Pt-acac] and ruthenium(III) acetylacetonate [Ru(C5H7O2)3, also denoted Ru-acac]. First, Pt-acac and Ru-acac are dissolved in acetone at the desired concentrations (typically, 0.00338 moles of each salt per 100 mL of acetone) at a temperature of 50 C. A solution of 25 percent tetramethylammonium hydroxide [(CH3)4NOH, also denoted TMAH] in methanol is added to the Pt-acac/Ruacac/ acetone solution to act as a high-molecular-weight hydrolyzing agent. The addition of the TMAH counteracts the undesired tendency of Pt-acac and Ru-acac to precipitate as separate phases during the subsequent evaporation of the solvent, thereby helping to yield a desired homogeneous amorphous gel. The solution is stirred for 10 minutes, then the solvent is evaporated until the solution becomes viscous, eventually transforming into a gel. The viscous gel is dried in air at a temperature of 170 C for about 10 hours. The dried gel is crushed to make a powder that is the immediate precursor of the final catalytic product. The precursor powder is converted to the final product in a controlled-atmosphere heat treatment. Desirably, the final product is a phase-pure (Pt phase only) Pt-Ru powder with a high specific surface area. The conditions of the controlled- atmosphere heat are critical for obtaining the aforementioned desired properties. A typical heat treatment that yields best results for a catalytic alloy of equimolar amounts of Pt and Ru consists of at least two cycles of heating to a temperature of 300 C and holding at 300 C for several hours, all carried out in an atmosphere of 1 percent O2 and 99 percent N2. The resulting powder consists of crystallites with typical linear dimensions of <10 nm. Tests have shown that the powder is highly effective in catalyzing the electro-oxidation of methanol.

Narayanan, Sekharipuram↗

NASA NTRS1994

A Coupled Soil-Atmosphere Model of H2O2 on Mars

The Viking Gas Chromatograph Mass Spectrometer failed to detect organic compounds on Mars, and both the Viking Labeled Release and the Viking Gas Exchange experiments indicated a reactive soil surface. These results have led to the widespread belief that there are oxidants in the martian soil. Since H2O2 is produced by photochemical processes in the atmosphere of Mars, and has been shown in the laboratory to reproduce closely the Viking LR results, it is a likely candidate for a martian soil oxidant. Here, we report on the results of a coupled soil/atmosphere transport model for H202 on Mars. Upon diffusing into the soil, its concentration is determined by the extent to which it is adsorbed and by the rate at which it is catalytically destroyed. An analytical model for calculating the distribution of H202 in the martian atmosphere and soil is developed. The concentration of H202 in the soil is shown to go to zero at a finite depth, a consequence of the nonlinear soil diffusion equation. The model is parameterized in terms of an unknown quantity, the lifetime of H202 against heterogeneous catalytic destruction in the soil. Calculated concentrations are compared with a H202 concentration of 30 nmoles/cu cm, inferred from the Viking Labeled Release experiment. A significant result of this model is that for a wide range of H202 lifetimes (up to 105 years), the extinction depth was found to be less than 3 m. The maximum possible concentration in the top 4 cm is calculated to be approx. 240 nmoles/cu cm, achieved with lifetimes of greater than 1000 years. Concentrations higher than 30 nmoles/cu cm require lifetimes of greater than 4.3 terrestrial years. For a wide range of H202 lifetimes, it was found that the atmospheric concentration is only weakly coupled with soil loss processes. Losses to the soil become significant only when lifetimes are less than a few hours. If there are depths below which H202 is not transported, it is plausible that organic compounds, protected from an oxidizing environment, may still exist. They would have been deposited by meteors, or be the organic remains of past life.

Bullock, Mark A.↗

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 NTRS1981

High temperature durable catalyst development

A program has been carried out to develop a catalytic reactor capable of operation in environments representative of those anticipated for advanced automotive gas turbine engines. A reactor consisting of a graded cell honeycomb support with a combination of noble metal and metal oxide catalyst coatings was built and successfully operated for 1000 hr. At an air preheat temperature of 740 K and a propane/air ratio of 0.028 by mass, the adiabatic flame temperature was held at about 1700 K. The graded cell monolithic reaction measured 5 cm in diameter by 10.2 cm in length and was operated at a reference velocity of 14.0 m/s at 1 atm. Measured NOx levels remained below 5 ppm, while unburned hydrocarbon concentrations registered near zero and carbon monoxide levels were nominally below 20 ppm.

Snow, G. C.↗

NASA NTRS1992

Thermal control/oxidation resistant coatings for titanium-based alloys

Extensive research and development efforts have been expended toward development of thermal control and environmental protection coatings for NASP and generic hypersonic vehicle applications. The objective of the coatings development activities summarized here was to develop light-weight coatings for protecting advanced titanium alloys from oxidation in hypersonic vehicle applications. A number of new coating concepts have been evaluated. Coated samples were exposed to static oxidation tests at temperatures up to 1000 C using a thermogravimetric apparatus. Samples were also exposed to simulated hypersonic flight conditions for up to 10 hr to determine their thermal and chemical stability and catalytic efficiency. The emittance of samples was determined before and after exposure to simulated hypersonic flight conditions.

Clark, Ronald K.↗