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At least 613 records · Page 34

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NASA NTRS2001

A Survey of Alternative Oxygen Production Technologies

Utilization of the Martian atmosphere for the production of fuel and oxygen has been extensively studied. The baseline fuel production process is a Sabatier reactor, which produces methane and water from carbon dioxide and hydrogen. The oxygen produced from the electrolysis of the water is only half of that needed for methane-based rocket propellant, and additional oxygen is needed for breathing air, fuel cells and other energy sources. Zirconia electrolysis cells for the direct reduction of CO2 arc being developed as an alternative means of producing oxygen, but present many challenges for a large-scale oxygen production system. The very high operating temperatures and fragile nature of the cells coupled with fairly high operating voltages leave room for improvement. This paper will survey alternative oxygen production technologies, present data on operating characteristics, materials of construction, and some preliminary laboratory results on attempts to implement each. Our goal is to significantly improve upon the characteristics of proposed zirconia cells for oxygen production. To achieve that goal we are looking at electrolytic systems that operate at significantly lower temperatures, preferably below 31C to allow the incorporation of liquid CO2 in the electrolyte. Our preliminary results indicate that such a system will have much higher current densities and have simpler cathode construction than a porous gas feed electrode system. Such a system could be achieved based on nonaqueous electrolytes or ionic liquids. We are focusing our research on the anode reaction that will produce oxygen from a product generated at the cathode using CO2 as the feed. Operation at low temperatures also will open up the full range of polymer and metal materials, allowing a more robust system design to withstand the rigors of flight, landing, and long term unattended operation on the surface of Mars.

Lueck, Dale E.↗

NASA NTRS2000

A Survey of Alternative Oxygen Production Technologies

Lueck, Dale E.↗

DOE OSTI2024

AP-XPS Study of the Reaction of O 2 and CO 2 with Zn–Au(111) Surface Alloys: Activation of O–O/C–O Bonds and the Formation of ZnO

Synchrotron-based ambient-pressure X-ray photoelectron spectroscopy (AP-XPS) was used to study the dissociation of O 2 and CO 2 on Zn-Au(111) alloys which contained 0.2-0.3 monolayers of zinc. Although Au(111) is inert, the alloys displayed a high activity for the cleavages of O-O and C-O bonds at room temperature with the formation of ZnO x species. Dissociative adsorption of O 2 at 300 K destroyed the alloys and the results of AP-XPS pointed to the co-existence of two types of oxygen species on the surface: ZnO x and chemisorbed O atoms (O chem ) on Au or the Au-ZnO interface. Annealing from room temperature to 600 K induced a O chem → ZnO x transformation that reflected the poor stability of O atoms on Au(111). The Zn-Au(111) systems exhibited a reactivity towards CO 2 that was much larger than that seen for Au(111), Cu(111) or surfaces of late transition metals like, Ni, Pd or Pt. At 300 K, CO 2 underwent partial dissociation depositing large amounts of O chem on the surface with minor formation of ZnO x . In addition, the deposited O chem reacted with CO 2 to form surface carbonate groups. Dosing of CO 2 at 500-600 K mainly led to the formation of ZnO x and the surface carbonate almost disappeared. In the presence of hydrogen, i.e. reaction feeds with a CO 2 to H 2 ratio of 1:3, the surface chemistry at 300 K was very similar to that seen for pure CO 2 with the formation of ZnO x and carbonate groups. In contrast, at 500-600 K, reaction with hydrogen induced the removal of ZnO x and CO 3 /HCOO species. Finally, our AP-XPS results are consistent with the idea that CO 2 hydrogenation on AuZn alloys involves a redox process where there is sequential oxidation by CO 2 and reduction by H 2 to yield methanol.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Reduction of Ultrafine Hematite for a Spouting Bed Chemical Looping Process - Presentation

Chemical looping combustion research has been a topic of great interest since the mid-1990s, although the concept can be traced much further back. It is a combustion technology for fuel utilization that uses a two-reactor system to produce a carbon free effluent stream from the air reactor and a carbon dioxide rich stream from the fuel reactor with oxygen shuttled between the reactors with an oxygen carrier. Chemical looping combustion has been studied extensively because of this inherent separation of the carbon dioxide combustion product from the atmospheric nitrogen over that past 25 years with hundreds of research papers and tens of books. The oxygen carrier is, in general, a solid such as naturally occurring hematite or an engineered carrier like a copper and iron oxide supported on alumina. System technical and economic research activities conducted at the National Energy Technology Laboratory have shown that the costs associated with the carrier, initial and replacement, are a significant factor in the economic viability of the technology. To overcome this economic challenge, the work reported on in this paper investigates the use of a waste iron oxide as the chemical looping oxygen carrier. This waste material is quite unique as it has a particle size of 0.7 um. Given the particle size, the reactions are quite fast. However, the development of a contactor reactor to mix the fuel with the carrier is a fluidization challenge as the material is a Geldart group C material and highly cohesive. Normally, Geldart group C materials are fluidized with either a vibrating bed. This technique is acceptable for low temperature pharmaceuticals production but does not lend itself to much larger reactors used for power production or operation at temperatures in the order of 1100 to 1200 C. Therefore, a hydrodynamic solution was needed to break up the cohesive structures to replace the vibration. In this instance, it was hypothesized that a spouting bed of large Geldart group B or Geldart group D particles could provide the necessary energy to break up the cohesive structures of the Geldart group C material. This paper presents the reduction performance for this novel carrier material in a laboratory spouting bed reactor.

Breault, Ronald↗

NASA NTRS2005

Control of Effluent Gases from Solid Waste Processing using Impregnated Carbon Nanotubes

One of the major problems associated with solid waste processing technologies is effluent contaminants that are released in gaseous forms from the processes. This is a concern in both biological as well as physicochemical solid waste processing. Carbon dioxide (CO2), the major gas released, does not present a serious problem and there are currently in place a number of flight-qualified technologies for CO2 removal. However, a number of other gases, in particular NOx, SO2, NH3, and various hydrocarbons (e.g. CH4) do present health hazards to the crew members in space habitats. In the present configuration of solid waste processing in the International Space Station (ISS), some of these gases are removed by the Trace Contaminant Control System (TCCS), demands a major resupply. Reduction of the resupply can be effective by using catalyst impregnated carbon nanotubes. For example, NO decomposition to N2 and O2 is thermodynamically favored. Data showing decomposition of NO on metal impregnated carbon nanotubes is presented. Comparisons are made of the existing TCCS systems with the carbon nanotube based technology for removing NOx based on mass/energy penalties.

Li, Jing↗

DOE OSTI2021

Life Cycle Analysis of Renewable Natural Gas and Lactic Acid Production from Waste Feedstocks

Producing fuels and chemicals from waste is considered economically favorable, due to low feedstock cost, and environmentally favorable, due to avoided emissions from conventional waste management practices. In this study, we evaluate the life cycle greenhouse gas (GHG) emission reduction benefits of renewable natural gas (RNG) and lactic acid (LA) production from four types of wet waste feedstocks (wastewater sludge, food waste, swine manure, and fats, oil, and grease [FOG]) via anaerobic digestion (AD) and LA fermentation, respectively. RNG can be used as an alternative to fossil natural gas, while LA from waste feedstocks can displace conventional LA production pathways (mainly from corn via fermentation). Providing comprehensive life cycle GHG emissions of the combinations of waste feedstocks and products through different routes helps identify the GHG hotspots and show where emissions savings come from. The results show that the carbon intensities (CIs) of waste-derived RNG and LA are much lower than those of their counterparts. We estimated the life cycle GHG emissions for RNG to be between -146 and 27 g carbon dioxide equivalent (CO2e)/MJ, much lower than the CI of fossil fuels. Waste-derived LA pathways also show substantially lower CIs, ranging from -4.2 to -1.4 kgCO2e/kg LA, compared to the CIs of LA from corn and corn stover (1.2 and 0.3 kgCO2e/kg LA, respectively). We will also discuss that the low CIs of waste-derived products can come from low yields leading to high emission credits. Thus, life cycle analysis results presented per weight of treated waste can be used to support decisions about which waste feedstocks and products are to be used for sustainable waste valorization. In addition, we found that monetary emission reduction credits can play an important role in driving waste valorization.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2024

Natural Gas Combined Cycle Power Plants with Carbon Capture and Exhaust Gas Recycle

This is a presentation given at the 3rd International Conference on Energy and Environment. The presentation highlights analysis work conducted by NETL to assess the cost and performance for natural gas combined cycle (NGCC) power plants that incorporate solvent-based post combustion carbon dioxide (CO2) capture and exhaust gas recycle (EGR). Increasing the inlet CO2 concentration by EGR is expected to improve the efficiency of the capture system and reduce its cost, however the analysis results show that the cost improvement is minimal as is the cost of capture reduction.

Hackett, Gregory↗

DOE OSTI2023

Using high pressure solutions of polyfluoroacrylate and CO 2 to Seal cement cracks for improved wellbore integrity

Polyfluoroacrylate (PFA) is a hydrophobic and oleophobic polymer that is soluble in high pressure carbon dioxide (CO 2 ). In this study, the ability of PFA-CO 2 solutions to greatly reduce the apparent permeability of split or cracked Portland cement cylindrical samples is assessed. The apparent permeability values of confined samples were determined before and after treatment with PFA-CO 2 solutions. In four tests, PFA-CO 2 solutions were continuously displacing pure CO 2 from the cracked cement and the decrease in apparent permeability due to PFA adsorption and wettability alteration was monitored. The lowest apparent permeability cracked cement sample (81 nD) was completely sealed with a very small amount of solution. Samples with initial apparent permeabilities of 89 μD and 29.4 mD exhibited 92% and 99% reductions in permeability, respectively, before the experiments had to be stopped because of the excessively large increase in pressure drop. A 50% reduction in apparent permeability was observed with a 3.80 mD sample. Four other split cement samples (bound together with tape) with an initial apparent permeability in the 9.0–70 mD range were removed from the core holder and immersed in a PFA-CO 2 solution for 24 h to allow for PFA adsorption. Then the PFA-CO 2 solution was depressurized, allowing for the deposition of additional PFA from the solution within the crack as the pressure fell below the cloud point pressure of the PFA-CO 2 solution. These four samples were then confined again in a core holder and apparent permeability reductions of 29–93% were observed. Finally, results from these eight experiments indicates that the more substantial reductions in the nD – mD apparent permeability of the cracked cement correlated to lower initial crack permeability, higher PFA concentration, and slower injection rate of the PFA-CO 2 solution into the crack.

58 GEOSCIENCES↗

DOE OSTI2022

High-Pressure Laminar Flame Speeds and Markstein Lengths of Syngas Flames Diluted in Carbon Dioxide and Helium

Abstract New laminar flame speed and burned-gas Markstein length data for H2–CO–O2–CO2–He mixtures have been measured from spherically expanding flames. Experiments were conducted at 10 atm and room temperature for H2:CO ratios ranging from 2:1 to 1:4 and for overall CO2 mole fractions from 0% to 30%. CO2 dilution had little effect on Markstein length, but CO2 dilutions of 10%, 20%, and 30% caused average reductions in flame speed of 47%, 73%, and 89%, respectively, regardless of H2:CO ratio. The study was designed to isolate the dilution effect of CO2 on flame speed, and a detailed analysis using the FCO2 method was used to show that the chemical-kinetic participation of CO2 was responsible for up to 20% of the reduction in flame speed. Hence, the majority (80% or more) of the reduction in flame speed due to CO2 is from the thermal effect. Accurate flame speed predictions were produced by five different chemical kinetics mechanisms for most conditions, with the slight exception of high-CO, high-CO2 mixtures. A thorough sensitivity analysis highlighted the larger effect of CO2 dilution on the important kinetics reactions than the effect of changing H2:CO. Sensitivity analysis also showed that the chain branching reaction H2O + O ⇌ OH + OH could be modified (albeit beyond its uncertainty) to achieve more accurate flame speed predictions, but also indicated that further improvement of flame speed modeling would require changes to many lesser reactions.

Engineering↗

NASA NTRS1991

Chemical approaches to carbon dioxide utilization for manned Mars missions

Use of resources available in situ is a critical enabling technology for a permanent human presence in space. A permanent presence on Mars, e.g., requires a large infrastructure to sustain life under hostile conditions. As a resource on Mars, atmospheric CO2 is as follows: abundant; available at all points on the surface; of known presence; chemically simple; and can be obtained by simple compression. Many studies focus on obtaining O2 and the various uses for O2 including life support and fuel; discussion of CO, the coproduct from CO2 fixation revolves around its uses as a fuel, being oxidized back to CO2. Several new proposals are studied for CO2 fixation through chemical, photochemical, and photoelectrochemical means. For example, the reduction of CO2 to hydrocarbons such as acetylene (C2H2) can be accomplished with H2. C2H2 has a theoretical vacuum specific impulse of approx. 375 secs. Potential uses were also studied of CO2, as obtained or further reduced to carbon, as a reducing agent in metal oxide processing to form metals or metal carbides for use as structural or power materials; the CO2 can be recycled to generate O2 and CO.

Hepp, Aloysius F.↗

NASA NTRS1972

Advances in pyroelectric infrared detectors.

Recent improvements in the pyroelectric detector have been due to the development of locked-in polarization, further reduction of the FET leakage current, and reduction of short circuit noise. The pyroelectric detector has been successfully employed in these typical applications: (1) thermograph using a single detector and X-Y scanner, (2) focal plane reticle scanner, (3) linear array thermal imaging system, (4) pyroelectric image tube, (5) radiometers (vertical temperature profile radiometer, carbon dioxide sensor), (6) high speed spectrometer, and (7) laser detector.

Beerman, H. P.↗

NASA NTRS2007

Development of a Rapid Cycling CO2 and H2O Removal Sorbent

The National Aeronautics and Space Administration (NASA) planned future missions set stringent demands on the design of the Portable Life Support System (PLSS), requiring dramatic reductions in weight, decreased reliance on supplies and greater flexibility on the types of missions. Use of regenerable systems that reduce weight and volume of the Extravehicular Mobility Unit (EMU) is of critical importance to NASA, both for low orbit operations and for long duration manned missions. The carbon dioxide and humidity control unit in the existing PLSS design is relatively large, since it has to remove and store eight hours worth of carbon dioxide (CO2). If the sorbent regeneration can be carried out during the Extravehicular Activity (EVA) with a relatively high regeneration frequency, the size of the sorbent canister and weight can be significantly reduced. TDA Research, Inc. is developing compact, regenerable sorbent materials to control CO2 and humidity in the space suit ventilation loop. The sorbent can be regenerated using space vacuum during the EVA, eliminating all CO2 and humidity duration-limiting elements in the life support system. The material also has applications in other areas of space exploration including long duration exploration missions requiring regenerable technologies and possibly the Crew Exploration Vehicle (CEV) spacecraft. This paper summarizes the results of the sorbent development, testing, and evaluation efforts to date.

Alptekin, Gokhan↗

DOE OSTI2023

Microwave Regeneration and Thermal and Oxidative Stability of Imidazolium Cyanopyrrolide Ionic Liquid for Direct Air Capture of Carbon Dioxide

Abstract Understanding the oxidative and thermal degradation of CO 2 sorbents is essential for assessing long‐term sorbent stability in direct air capture (DAC). The potential degradation pathway of imidazolium cyanopyrrolide, an ionic liquid (IL) functionalized for superior CO 2 capacity and selectivity, is evaluated under accelerated degradation conditions to elucidate the secondary reactions that can occur during repetitive absorption‐desorption thermal‐swing cycles. The combined analysis from various spectroscopic, chromatographic, and thermal gravimetric measurements indicated that radical and S N 2 mechanisms in degradation are encouraged by the nucleophilicity of the anion. Thickening of the liquid and gas evolution are accompanied by 50 % reduction in CO 2 capacity after a 7‐day exposure to O 2 under 80 °C. To prevent long exposure to conventional thermal heating, microwave (MW) regeneration of the CO 2 ‐reactive IL is used, where dielectric heating at 80 and 100 °C rapidly desorbs CO 2 and regenerates the IL without any measurable degradation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1975

Evaluation and characterization of the methane-carbon dioxide decomposition reaction

A program was conducted to evaluate and characterize the carbon dioxide-methane (CO2-CH4) decomposition reaction, i.e., CO2 + CH4 = 2C + 2H2O. The primary objective was to determine the feasibility of applying this reaction at low temperatures as a technique for recovering the oxygen (O2) remaining in the CO2 which exits mixed with CH4 from a Sabatier CO2 reduction subsystem (as part of an air revitalization system of a manned spacecraft). A test unit was designed, fabricated, and assembled for characterizing the performance of various catalysts for the reaction and ultraviolet activation of the CH4 and CO2. The reactor included in the test unit was designed to have sufficient capacity to evaluate catalyst charges of up to 76 g (0.17 lb). The test stand contained the necessary instrumentation and controls to obtain the data required to characterize the performance of the catalysts and sensitizers tested: flow control and measurement, temperature control and measurement, product and inlet gas analysis, and pressure measurement. A product assurance program was performed implementing the concepts of quality control and safety into the program effort.

Davenport, R. J.↗

NASA NTRS1988

Photochemical and thermal modeling in the early atmosphere of the earth

The simplest carbon compounds, present in the terrestrial and planetary atmospheres, exhibit a wide range of oxidation states, carbon dioxide and methane being the most oxidized and the most reduced form of carbon, respectively. The question arises as to the origin and the interconversion among the carbon species. The chemical pathways for the conversion of CH4 to CO and CO2 are for the most part known. The reverse process, the reduction of CO to CH4 is however, poorly understood. A new reaction is proposed, H2CO + H + M yields CH3O + M, which might play a fundamental role in the reduction of CO or CH4. An update is presented of nitrile photochemistry on Titan.

Yung, Yuk L.↗

NASA NTRS1996

Heterogeneous Photocatalytic Oxidation of Atmospheric Trace Contaminants

Heterogeneous photocatalysis involves the use of a light-activated catalyst at room temperature in order to carry out a desired reaction. In the presence of molecular oxygen, illumination of the n-type semiconductor oxide titanium dioxide (TiO2) provides for production of highly active forms of oxygen, such as hydroxyl radicals, which are able to carry out the complete oxidative destruction of simple hydrocarbons such as methane, ethane, ethylene, propylene, and carbon monoxide. This broad oxidation potential, coupled with the ability with sufficient residence time to achieve complete oxidation of simple hydrocarbon contaminants to carbon dioxide and water, indicated that heterogeneous photocatalysis should be examined for its potential for purification of spacecraft air. If a successful catalyst and photoreactor could be demonstrated at the laboratory level, such results would allow consideration of photocatalysts as a partial or complete replacement of adsorption systems, thereby allowing for reduction in lift-off weight of a portion of the life support system for the spacecraft, or other related application such as a space station or a conventional commercial aircraft. The present research was undertaken to explore this potential through achievement of the following plan of work: (a) ascertain the intrinsic kinetics of conversion of pollutants of interest in spacecraft, (b) ascertain the expected lifetime of catalysts through examination of most likely routes of catalyst deactivation and regeneration, (c) model and explore experimentally the low pressure drop catalytic monolith, a commercial configuration for automotive exhaust control, and (d) examine the kinetics of multicomponent conversions. In the recent course of this work, we have also discovered how to increase catalyst activity via halide promotion which has allowed us to achieve approximately 100% conversion of an aromatic contaminant (toluene) in a very short residence time of 5-6 milliseconds.

Ollis, David F.↗

NASA NTRS1996

Heterogeneous Photocatalytic Oxidation of Atmospheric Trace Contaminants

Heterogeneous photocatalysis involves the use of a light-activated catalyst at room temperature in order to carry out a desired reaction. In the presence of molecular oxygen, illumination of the n-type semiconductor oxide titanium dioxide (TiO2) provides for production of highly active forms of oxygen, such as hydroxyl radicals, which are able to carry out the complete oxidative destruction of simple hydrocarbons such as methane, ethane, ethylene, propylene, and carbon monoxide. This broad oxidation potential, coupled with the ability with sufficient residence time to achieve complete oxidation of simple hydrocarbon contaminants to carbon dioxide and water, indicated that heterogeneous photocatalysis should be examined for its potential for purification of spacecraft air. If a successful catalyst and photoreactor could be demonstrated at the laboratory level, such results would allow consideration of photocatalysts as a partial or complete replacement of adsorption systems, thereby allowing for reduction in lift-off weight of a portion of the life support system for the spacecraft, or other related application such as a space station or a conventional commercial aircraft. The present research was undertaken to explore this potential through achievement of the following plan of work: (a) ascertain the intrinsic kinetics of conversion of pollutants of interest in spacecraft, (b) ascertain the expected lifetime of catalysts through examination of most likely routes of catalyst deactivation and regeneration (c) model and explore experimentally the low pressure drop catalytic monolith, a commercial configuration for automotive exhaust control (d) examine the kinetics of multicomponent conversions. In the recent course of this work, we have also discovered how to increase catalyst activity via halide promotion which has allowed us to achieve approximately 100% conversion of an aromatic contaminant (toluene) in a very short residence time of 5-6 milliseconds.

Ollis, David F.↗

NASA NTRS1997

Searching for Biogeochemical Cycles on Mars

The search for life on Mars clearly benefits from a rigorous, yet broad, definition of life that compels us to consider all possible lines of evidence for a martian biosphere. Recent studies in microbial ecology illustrate that the classic definition of life should be expanded beyond the traditional definition of a living cell. The traditional defining characteristics of life are threefold. First, life is capable of metabolism, that is, it performs chemical reactions that utilize energy and also synthesize its cellular constituents. Second, life is capable of self-replication. Third, life can evolve in order to adapt to environmental changes. An expanded, ecological definition of life also recognizes that life is a community of organisms that must interact with their nonliving environment through processes called biogeochemical cycles. This regenerative processing maintains, in an aqueous conditions, a dependable supply of nutrients and energy for growth. In turn, life can significantly affect those processes that control the exchange of materials between the atmosphere, ocean, and upper crust. Because metabolic processes interact directly with the environment, they can alter their surroundings and thus leave behind evidence of life. For example, organic matter is produced from single-carbon-atom precursors for the biosynthesis of cellular constituents. This leads to a reservoir of reduced carbon in sediments that, in turn, can affect the oxidation state of the atmosphere. The harvesting of chemical energy for metabolism often employs oxidation-reduction reactions that can alter the chemistry and oxidation state of the redox-sensitive elements carbon, sulfur, nitrogen, iron, and manganese. Have there ever been biogeochemical cycles on Mars? Certain key planetary processes can offer clues. Active volcanism provides reduced chemical species that biota can use for organic synthesis. Volcanic carbon dioxide and methane can serve as greenhouse gases. Thus the persistence of volcanism on Mars may well have influenced the persistence of a martian biosphere. The geologic processing of the crust can affect the availability of nutrients and also control the deposition of minerals that could have served as a medium for the preservation of fossil information. Finally, the activity of liquid water is crucial to life. Was there ever an Earth-like hydrologic cycle with rainfall? Has aqueous activity instead been restricted principally to hydrothermal activity below the surface? To what extent did the inorganic chemistry driven by sunlight and hydrothermal activity influence organic chemistry (prebiotic chemical evolution)? This paper addresses these and other key questions.

DesMarais, David J.↗