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NASA NTRS2014

Novel Catalysts and Processing Technologies for Production of Aerospace Fuels from Non-Petroleum Raw Materials

Transportation fuels production (including aerospace propellants) from non-traditional sources (gases, waste materials, and biomass) has been an active area of research and development for decades. Reducing terrestrial waste streams simultaneous with energy conversion, plentiful biomass, new low-cost methane sources, and/or extra-terrestrial resource harvesting and utilization present significant technological and business opportunities being realized by a new generation of visionary entrepreneurs. We examine several new approaches to catalyst fabrication and new processing technologies to enable utilization of these non-traditional raw materials. Two basic processing architectures are considered: a single-stage pyrolysis approach that seeks to basically re-cycle hydrocarbons with minimal net chemistry or a two-step paradigm that involves production of supply or synthesis gas (mainly carbon oxides and hydrogen) followed by production of fuel(s) via Sabatier or methanation reactions and/or Fischer-Tropsch synthesis. Optimizing the fraction of product stream relevant to targeted aerospace (and other transportation) fuels via modeling, catalyst fabrication and novel reactor design are described. Energy utilization is a concern for production of fuels for either terrestrial or space operations; renewable sources based on solar energy and/or energy efficient processes may be mission enabling. Another important issue is minimizing impurities in the product stream(s), especially those potentially posing risks to personnel or operations through (catalyst) poisoning or (equipment) damage. Technologies being developed to remove (and/or recycle) heteroatom impurities are briefly discussed as well as the development of chemically robust catalysts whose activity are not diminished during operation. The potential impacts on future missions by such new approaches as well as balance of system issues are addressed.

propellants↗

NASA NTRS2005

Mechanically Strong, Lightweight Porous Materials Developed (X-Aerogels)

Aerogels are attractive materials for a variety of NASA missions because they are ultralightweight, have low thermal conductivity and low-dielectric constants, and can be readily doped with other materials. Potential NASA applications for these materials include lightweight insulation for spacecraft, habitats, and extravehicular activity (EVA) suits; catalyst supports for fuel cell and in situ resource utilization; and sensors for air- and water-quality monitoring for vehicles, habitats, and EVA suits. Conventional aerogels are extremely fragile and require processing via supercritical fluid extraction, which adds cost to the production of an aerogel and limits the sizes and geometries of samples that can be produced from these materials. These issues have severely hampered the application of aerogels in NASA missions.

Leventis, Nicholas↗

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 NTRS2008

Catalyst for treatment and control of post-combustion emissions

The present invention utilizes two precious metals with two to five different metal-oxides in a layered matrix to convert CO, HCs, and NOx to CO.sub.2, and N.sub.2 by oxidation of two components and reduction of the other in a moderately high temperature gaseous environment containing excess oxygen.

Upchurch, legal representative, Wilhelmina 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 NTRS1994

Investigation of catalytic reduction and filter techniques for simultaneous measurements of NO, NO2, and HNO3 in the stratosphere

A concept for measuring stratospheric NOy-species is presented which utilizes the catalytic reduction of NO2 and HNO3 over heated metal catalysts and the chemisorption of HNO3 on Nylon. Using the Max Planck Institute for Aeronomy (MPAE) chemiluminescent balloon-borne sonde, stratospheric NO and NO2 profiles have been measured since 1983. NO is detected by chemiluminescence produced in reaction with O3 while NO2 needs first to be converted to NO over a heated stainless steel catalyst. To improve this technique for simultaneously measuring HNO3, the catalytic reduction of NO2 and HNO3 over several metal catalysts and the chemisorption of NO2 and HNO3 on Nylon have been investigated in laboratory tests. The results of these tests under simulated stratospheric conditions are presented in detail in this paper. They demonstrate that the simultaneous measurement of NO, NO2 and HNO3 is indeed possible with the combination of stainless steel or Au as a catalyst and a nylon filter.

Wendt, J.↗

NASA NTRS2019

Study of Sabatier Catalyst Performance for a Mars ISRU Propellant Production Plant

NASA is currently developing technologies for use in the field of in-situ resource utilization (ISRU). One of the technologies being advanced is the Sabatier, or methanation, reactor which converts carbon dioxide and hydrogen into methane gas and water at high temperatures. This paper discusses the catalyst life and performance issues for these reactors that would be expected on Mars and describes the test methods employed and observed results. The various catalysts were tested in their capacity for the continuous production of methane gas via the Sabatier reaction and the possible effects of launch vibration loads, exposure to liquid water, particulate contamination, and chemical contamination to the overall observed reaction efficacy of the catalysts evaluated.

Franco, Carolina↗

NASA NTRS2019

Study of Sabatier Catalyst Performance for a Mars ISRU Propellant Production Plant

Franco, Carolina↗

NASA NTRS1976

A status of progress for the Laser Isotope Separation (LIS) process

An overview of the Laser Isotope Separation (LIS) methodology is given together with illustrations showing a simplified version of the LIS technique, an example of the two-photon photoionization category, and a diagram depicting how the energy levels of various isotope influence the LIS process. Applications were proposed for the LIS system which, in addition to enriching uranium, could in themselves develop into programs of tremendous scope and breadth. These include the treatment of radioactive wastes from light-water nuclear reactors, enriching the deuterium isotope to make heavy-water, and enriching the light isotopes of such elements as titanium for aerospace weight-reducing programs. Economic comparisons of the LIS methodology with the current method of gaseous diffusion indicate an overwhelming advantage; the laser process promises to be 1000 times more efficient. The technique could also be utilized in chemical reactions with the tuned laser serving as a universal catalyst to determine the speed and direction of a chemical reaction.

Delionback, L. M.↗

NASA NTRS1988

Measurements of NO and total reactive odd-nitrogen, NOy, in the Antarctic stratosphere

Measurements of NO and total reactive N, NOy, were made as part of the Airborne Antarctic Ozone Experiment conducted in Punta Arenas, Chile during Aug. and Sept. 1987. The total reactive N reservoir includes the species NO, NO2, NO3, N2 O5, HNO3, and ClONO2. The instrument was located on board the NASA ER2 aircraft which conducted 12 flights over the Antarctic continent reaching altitudes of 18 km at 72 deg S latitude. The NOy technique utilized the conversion of component NOy species to NO on a gold catalyst and the subsequent detection of NO by the chemiluminescence reaction of NO with ozone. Since the inlet sample line is heated and the catalyst operates at 300 C, NOy incorporated in aerosols evaporates and is converted to NO. NO was measured on two separate flights by removing the catalyst from the sample inlet line.

Fahey, D. W.↗

NASA NTRS1985

Negative electrode catalyst for the iron chromium redox energy storage system

A redox cell which operates at elevated temperatures and which utilizes the same two metal couples in each of the two reactant fluids is disclosed. Each fluid includes a bismuth salt and may also include a lead salt. A low cost, cation permselective membrane separates the reactant fluids.

Gahn, R. 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 Glenn Research Center 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. Another issue of great concern is minimizing impurities in the product stream(s), especially those that are potential health risks and/or could degrade 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, Bryan A.↗

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 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 NTRS1983

ECUT: Energy Conversion and utilization Technologies program biocatalysis research activity. Generation of chemical intermediates by catalytic oxidative decarboxylation of dilute organic acids

A rhodium-based catalyst was prepared and preliminary experiments were completed where the catalyst appeared to decarboxylate dilute acids at concentrations of 1 to 10 vol%. Electron spin resonance spectroscoy was used to characterize the catalyst as a first step leading toward modeling and optimization of rhodium catalysts. Also, a hybrid chemical/biological process for the production of hydrocarbons has been assessed. These types of catalysts could greatly increase energy efficiency of this process.

Distefano, S.↗

NASA NTRS2017

Electrochemical Detection of Biological Catalysts as Signatures of Extant Life

Liquid water is the quintessential ingredient for life. Biochemistry as we know it is not possible without it. There are two places in the Solar System, other than the Earth, where liquid water is known to exist: Europa and Enceladus. Cassini’s recent discovery of Enceladus’ ocean plumes has excited the scientific community about the possibility for liquid sampling and search for life. Characteristics of life are self-sustainability, its ability to evolve, and self-enclosure. To enable these, chemical energy must be utilized, information must be stored, and enclosing membranes must be built. Many of these processes are accomplished with the use of biological catalysts. To search for life in the ocean worlds, detection of biological catalysts serves as a strong marker of biological activity and thus life.

Koehne, J. E.↗

NASA NTRS2003

Review of Laser Ablation Process for Single Wall Carbon Nanotube Production

Different types of lasers are now routinely used to prepare single wall carbon nanotubes (SWCNTs). The original method developed by researchers at Rice University utilized a "double pulse laser oven" process. A graphite target containing about 1 atomic percent of metal catalysts is ablated inside a 1473K oven using laser pulses (10 ns pulse width) in slow flowing argon. Two YAG lasers with a green pulse (532 nm) followed by an IR pulse (1064 nm) with a 50 ns delay are used for ablation. This set up produced single wall carbon nanotube material with about 70% purity having a diameter distribution peaked around 1.4 nm. The impurities consist of fullerenes, metal catalyst clusters (10 to 100 nm diameter) and amorphous carbon. The rate of production with the initial set up was about 60 mg per hour with 10Hz laser systems. Several researchers have used variations of the lasers to improve the rate, consistency and study effects of different process parameters on the quality and quantity of SWCNTs. These variations include one to three YAG laser systems (Green, Green and IR), different pulse widths (nano to microseconds as well as continuous) and different laser wavelengths (Alexandrite, CO, CO2, free electron lasers in the near to far infrared). It is noted that yield from the single laser (Green or IR) systems is only a fraction of the two laser systems. The yield seemed to scale up with the repetition rate of the laser systems (10 to 60 Hz) and depended on the beam uniformity and quality of the laser pulses. The shift to longer wavelength lasers (free electron, CO and CO2) did not improve the quality, but increased the rate of production because these lasers are either continuous (CW) or high repetition rate pulses (kHz to MHz). The average power and the peak power of the lasers seem to influence the yields. Very high peak powers (MegaWatts per square centimeter) are noted to increase ablation of bigger particles with reduced yields of SWCNTs. Increased average powers seem to help the conversion of the carbon from target into vapor phase to improve formation of nanotubes. The use of CW far infrared lasers reduced the need for the oven, at the expense of controlled ablation. Some of these variations are tried with different combinations and concentrations of metal catalysts (Nickel with Cobalt, Iron, Palladium and Platinum) different buffer gases (e.g. Helium); with different oven temperatures (Room temperature to 1473K); under different flow conditions (1 to 1000 kPa) and even different porosities of the graphite targets. It is to be noted that the original Cobalt and Nickel combination worked best, possibly because of improved carbonization with stable crystalline phases. The mean diameter and yield seemed to increase with increasing oven temperatures. Thermal conductivity of the buffer gas and flow conditions dictate the quality as well as quantity of the SWCNTs. Faster flows, lower pressures and heavier gases seem to increase the yields. This review will attempt to cover all these variations and their relative merits. Possible growth mechanisms under these different conditions will also be discussed.

Arepalli, Sivaram↗

NASA NTRS2011

Characterization of Catalyst Materials for Production of Aerospace Fuels

Due to environmental, economic, and security issues, there is a greater need for cleaner alternative fuels. There will undoubtedly be a shift from crude oil to non-petroleum sources as a feedstock for aviation (and other transportation) fuels. Additionally, efforts are concentrated on reducing costs coupled with fuel production from non-conventional sources. One solution to this issue is Fischer-Tropsch gas-to-liquid technology. Fischer-Tropsch processing of synthesis gas (CO/H2) produces a complex product stream of paraffins, olefins, and oxygenated compounds such as alcohols and aldehydes. The Fisher-Tropsch process can produce a cleaner diesel oil fraction with a high cetane number (typically above 70) without any sulfur or aromatic compounds. This process is most commonly catalyzed by heterogeneous (in this case, silver and platinum) catalysts composed of cobalt supported on alumina or unsupported alloyed iron powders. Physisorption, chemisorptions, scanning electron microscopy (SEM), and energy dispersive spectroscopy (EDS) are described to better understand the potential performance of Fischer-Tropsch cobalt on alumina catalysts promoted with silver and platinum. The overall goal is to preferentially produce C8 to C18 paraffin compounds for use as aerospace fuels. Progress towards this goal will eventually be updated and achieved by a more thorough understanding of the characterization of catalyst materials. This work was supported by NASA s Subsonic Fixed Wing and In-situ Resource Utilization projects.

DeLaRee, Ana B.↗