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At least 235 records · Page 13

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DOE OSTI2023

OH Roaming and Beyond in the Unimolecular Decay of the Methyl-Ethyl-Substituted Criegee Intermediate: Observations and Predictions

Alkene ozonolysis generates short-lived Criegee intermediates that are a significant source of hydroxyl (OH) radicals. Here this study demonstrates that roaming of the separating OH radicals can yield alternate hydroxycarbonyl products, thereby reducing the OH yield. Specifically, hydroxybutanone has been detected as a stable product arising from roaming in the unimolecular decay of the methyl-ethyl-substituted Criegee intermediate (MECI) under thermal flow cell conditions. The dynamical features of this novel multistage dissociation plus a roaming unimolecular decay process have also been examined with ab initio kinetics calculations. Experimentally, hydroxybutanone isomers are distinguished from the isomeric MECI by their higher ionization threshold and distinctive photoionization spectra. Moreover, the exponential rise of the hydroxybutanone kinetic time profile matches that for the unimolecular decay of MECI. A weaker methyl vinyl ketone (MVK) photoionization signal is also attributed to OH roaming. Complementary multireference electronic structure calculations have been utilized to map the unimolecular decay pathways for MECI, starting with 1,4 H atom transfer from a methyl or methylene group to the terminal oxygen, followed by roaming of the separating OH and butanonyl radicals in the long-range region of the potential. Roaming via reorientation and the addition of OH to the vinyl group of butanonyl is shown to yield hydroxybutanone, and subsequent C–O elongation and H-transfer can lead to MVK. A comprehensive theoretical kinetic analysis has been conducted to evaluate rate constants and branching yields (ca. 10–11%) for thermal unimolecular decay of MECI to conventional and roaming products under laboratory and atmospheric conditions, consistent with the estimated experimental yield (ca. 7%).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1989

Model system studies with a phase separated membrane bioreactor

The operation and evaluation of a bioreactor designed for high intensity oxygen transfer in a microgravity environment is described. The reactor itself consists of a zero headspace liquid phase separated from the air supply by a long length of silicone rubber tubing through which the oxygen diffuses in and the carbon dioxide diffuses out. Mass transfer studies show that the oxygen is film diffusion controlled both externally and internally to the tubing and not by diffusion across the tube walls. Methods of upgrading the design to eliminate these resistances are proposed. Cell growth was obtained in the fermenter using Saccharomyces cerevisiae showing that this concept is capable of sustaining cell growth in the terrestial simulation.

Petersen, G. R.↗

NASA NTRS1994

Simplex turbopump design

Turbomachinery used in liquid rocket engines typically are composed of complex geometries made from high strength-to-weight super alloys and have long design and fabrication cycle times (3 to 5 years). A simple, low-cost turbopump is being designed in-house to demonstrate the ability to reduce the overall cost to $500K and compress life cycle time to 18 months. The simplex turbopump was designed to provide a discharge pressure of 1500 psia of liquid oxygen at 90 lbm/s. The turbine will be powered by gaseous oxygen. This eliminates the need for an inter-propellant seal typically required to separate the fuel-rich turbine gases from the liquid oxygen pump components. Materials used in the turbine flow paths will utilize existing characterized metals at 800 deg R that are compatible with a warm oxygen environment. This turbopump design would be suitable for integration with a 40 K pound thrust hybrid motor that provides warm oxygen from a tapped-off location to power the turbine. The preliminary and detailed analysis was completed in a year by a multiple discipline, concurrent engineering team. Manpower, schedule, and cost data were tracked during the process for a comparison to the initial goal. The Simplex hardware is the procurement cycle with the expectation of the first test to occur approximately 1.5 months behind the original schedule goal.

Marsh, Matt↗

NASA NTRSDate not supplied

Advanced Metal Separation (AMS) via Marangoni Effect-driven Separation

For practical, economical, and sustainable human missions to the Moon, processing of lunar regolith and metal oxides is necessary for localized production of oxygen (O2) and metals that can be repurposed as rocket propellant, life support O2, and in-space manufactured parts. The primary candidates for in-situ resource utilization (ISRU) regolith processing are carbothermic reductions and molten regolith electrolysis (MRE) which both produce oxygen and a reduced, deoxygenated metallic slag. A metal separation technique is still required to capture and purify metals from the deoxygenated slag for reuse in areas such as metallic part fabrication, structural or design frameworks, and metal catalyst production. The Marangoni Effect is best explained as mass transfer along an interface driven by surface tension gradients induced by temperature and concentration differences. Due to the temperature gradients, molten metal can be transported in this fashion to create thin films. This method can transport molten metal in the absence of gravity or mechanical motion and greatly increases the available surface area for a vacuum fractional separation process. In this study, a novel vacuum furnace induces the Marangoni Effect to fractionally decompose and separate valuable metals (e.g., aluminum) from thin films of molten metal via vacuum distillation. The proposed work will examine lunar regolith, metal-based recycling feedstocks, and metallic slags produced from the carbothermal reduction of regolith. Data and observations from this study could produce a simple yet effective method of refining lunar derived metals by taking advantage of the high vacuum environment present on the lunar surface.

ISRU↗

DOE OSTI2020

Influence of fuel ash on the recoverability of copper from the spent material of chemical looping combustion

Chemical looping combustion (CLC) is an advanced energy production technology that inherently separates the CO 2 generated. The oxygen needed for fuel conversion is supplied by the oxygen carrier. When using copper-based oxygen carriers, oxygen carrier attrition is a challenge to the process economics, unless the attrited copper that is mixed with fuel ash in the spent material can be recovered by, for instance, acid leaching. However, fuel ash may transform the attrited copper into certain complexes of low leachability (e.g., CuAl 2 O 4 ), hindering the copper recovery. In this study, the copper content in the spent material was first evaluated. The effects of ash composition and copper content on the occurrence mode of copper in spent material were predicted by thermodynamic modeling. Redox cycles of simulated spent materials based on various coal ashes were performed to reveal the characteristics of CuAl 2 O 4 /CuFe 2 O 4 formation. The CuO-Al 2 O 3 reaction was investigated under the temperatures and solid residence times experienced in CLC. The materials were analyzed by X-ray diffraction. The results suggest that the fuel ash with a high Al/Ca ratio may lower the recoverability of copper when the temperature is above 925 °C. The slow formation of CuFe 2 O 4 is not expected to affect the copper recovery.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1972

Development of a solid electrolyte carbon dioxide and water reduction system for oxygen recovery

A 1/4-man solid electrolyte oxygen regeneration system, consisting of an electrolyzer, a carbon deposition reactor, and palladium membranes for separating hydrogen, was operated continuously in a 180-day test. Oxygen recovery from the carbon dioxide-water feed was 95%. One percent of the oxygen was lost to vacuum with the hydrogen off-gas. In a space cabin, the remaining 4% would have been recycled to the cabin and recovered. None of the electrolysis cells used in the 180-day test failed. Electrolysis power rose 20% during the test; the average power was 283.5 watts/man. Crew time was limited to 18 min/day of which 12 min/day was used for removing carbon. The success achieved in operating the system can be attributed to an extensive component development program, which is described. Stability of operation, ease of control, and flexibility in feed composition were demonstrated by the life test.

Elikan, L.↗

NASA NTRS1988

A model to predict the removal of oxygen from air using a zirconia solid electrolyte membrane

A finite difference mathematical model has been developed to predict the removal of oxygen from air using a zirconia separation cell. The model predicts the electrical and mass transfer processes in circular disk cells with either axial or radial current flow in the electrodes and in tubular cells with axial current flow in the electrodes. Representative results are presented and discussed.

Marner, W. J.↗

NASA NTRS1990

Design and analysis of composite primary structures for advanced launch vehicles

The current status of the Lightweight Composite Intertank Structures (LCIS) study, a program aimed at developing technologies required to apply advanced composite materials to launch vehicle primary structures, is reviewed. The launch system concept used for establishing design requirements consisted of a fully reusable winged booster and a partially reusable core vehicle. The component selected from this system for design and manufacturing studies was the core vehicle intertank adapter, a component consisting of approximately 26-ft diameter by 25 ft long stiffened cylindrical structure that separates the liquid hydrogen and liquid oxygen tanks on the core vehicle. The discussion covers the program approach, design requirements, material properties, structural analysis, and the test program.

Rix, C.↗

NASA NTRS1997

STS-82 Mission Highlight Presentation

The STS-82 is the second in a series of planned service missions to the Hubble Space Telescope (HST). The flight crew of STS-82, Cmdr. Kenneth D. Bowersox, Pilot Scott J. Horowitz, Mission specialists, Mark C. Lee, Steven A. Hawley, Gregory J. Harbaugh, Steven L. Smith, and Joseph R. Tanner can be seen performing pre-launch activities preparing for the night launch. The crew meets the press for pre-launch photos before being transported to the launch pad. Several views can be seen of the final inspection team on the O level and the crew being readied in the 'white room'. Launch activities such as the oxygen vent hood retraction, liftoff, SRB separation, and personnel activities in the Houston Integrated Mission Control room are viewed. Subsequent footage is provided of the crew's activities during the HST rendezvous and docking, Extravehicular Activities (EVA's) preparation and EVA numbers 1, 3 and 5. During the first EVA the earth can be seen clearly in a reflection off of HST's offshroud during its 60th orbit crossing the equator. The HST deployment and views of the Hale-Bopp comet are clearly seen before Discovery's reentry and landing. After reentry a beautiful view of Discovery moving at 10,400 mph can be seen looking east from Mission Control. The ususal twin sonic boom precedes Discovery's touchdown on runway 15 at Kennedy Space Center. This second HST service mission orbited Earth 150 times and traveled 1.4 million miles.

Source record↗

NASA NTRS1994

Oscillating behavior of carbohydrate granule formation and dinitrogen fixation in the cyanobacterium Cyanothece sp. strain ATCC 51142

It has been shown that some aerobic, unicellular, diazotrophic cyanobacteria temporally separate photosynthetic O2 evolution and oxygen-sensitive N2 fixation. Cyanothece sp. ATCC strain 51142 is an aerobic, unicellular, diazotrophic cyanobacterium that fixes N2 during discrete periods of its cell cycle. When the bacteria are maintained under diurnal light-dark cycles, N2 fixation occurs in the dark. Similar cycling is observed in continuous light, implicating a circadian rhythm. Under N2-fixing conditions, large inclusion granules form between the thylakoid membranes. Maximum granulation, as observed by electron microscopy, occurs before the onset of N2 fixation, and the granules decrease in number during the period of N2 fixation. The granules can be purified from cell homogenates by differential centrifugation. Biochemical analyses of the granules indicate that these structures are primarily carbohydrate, with some protein. Further analyses of the carbohydrate have shown that it is a glucose polymer with some characteristics of glycogen. It is proposed that N2 fixation is driven by energy and reducing power stored in these inclusion granules. Cyanothece sp. strain ATCC 51142 represents an excellent experimental organism for the study of the protective mechanisms of nitrogenase, metabolic events in cyanobacteria under normal and stress conditions, the partitioning of resources between growth and storage, and biological rhythms.

Non-NASA Center↗

NASA NTRS2008

NDE for the ARES I Upper Stage Common Bulkhead

The current design of the ARES 1 Upper Stage uses a common bulkhead to separate the liquid hydrogen and liquid oxygen tanks. The bulkhead consists of aluminum face sheets bonded to a Phenolic honeycomb core. The face sheets, or domes, are friction stir welded to Y-rings that connect the bulkhead to the barrel sections of the liquid hydrogen and liquid oxygen tanks. Load between the Y-rings is carried by an externally attached bolting ring. The development of nondestructive evaluation methods for the ARES I Upper Stage Common Bulkhead are outlined in this presentation. Methods for inspecting the various components of the bulkhead are covered focusing in on the dome skins, core-to-dome bond lines and friction stir welds as well as structural details like the fastener holes. Thermography, shearography and ultrasonic methods are discussed for the bond lines. Eddy current methods are discussed for the fastener holes and dome skins. A combination of phased array ultrasound, liquid penetrant and radiography are to being investigated for use on the friction stir welds. Keywords: Composite materials, NDE, Cryogenic structures

Walker, James↗

DOE OSTI2022

Polybenzimidazole-derived carbon molecular sieve hollow fiber membranes with tailored oxygen selective transport

Polymer membrane carbonization is a promising strategy to obtain carbon molecular sieve (CMS) membrane materials with tailorable cavity size distributions for high gas selectivities beyond that attained from traditional polymer membrane materials. Despite their already demonstrated exceptional separation performance characteristics for several gas separation applications (e.g. CO 2 /CH 4 and H 2 /CO 2 ), further development of CMS membranes having high O 2 /N 2 perm-selectivity for energy-efficient high-purity O 2 production has proven challenging. Herein, we explore CMS hollow fiber membranes (HFMs) derived from highly rigid and tightly-packed polybenzimidazole (PBI) materials. Nearly defect-free PBI-derived CMS HFMs were fabricated and evaluated for O 2 /N 2 separation performance for the first time. The micro-structural and O 2 selective gas separation characteristics of PBI-CMS HFMs pyrolyzed at different pyrolysis conditions were intensively studied. With rigorous carbonization protocol optimization, we obtained highly O 2 permselective PBI-CMS HFMs having O 2 /N 2 selectivities approaching 14, enabling high purity O 2 production. The PBI-CMS HFM O 2 /N 2 separation performance dependence on operating conditions (e.g. temperature and feed pressure) are reported.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Performance of a Natural Gas Solid Oxide Fuel Cell System With and Without Carbon Capture

The fuel cell program at the United States Department of Energy (DOE) National Energy Technology Laboratory (NETL) is focused on the development of low-cost, highly efficient, and reliable fossil-fuel-based solid oxide fuel cell (SOFC) power systems that can generate environmentally-friendly electric power with at least 90 percent carbon capture. NETL’s SOFC technology development roadmap is aligned with near-term market opportunities in the distributed generation sector to validate and advance the technology while paving the way for utility-scale natural gas (NG)- and coal-derived synthesis gas-fueled applications via progressively larger system demonstrations. The present study represents a part of a series of system evaluations being carried out at NETL to aid in prioritizing technological advances along research pathways to the realization of utility-scale SOFC systems, a transformational goal of the fuel cell program. In particular, the system performance of utility-scale NG fuel cell (NGFC) systems with and without carbon dioxide (CO2) capture is presented. The NGFC system analyzed features an external auto-thermal reformer (ATR) feeding the fuel to the SOFC system consisting of planar anode-supported SOFC with separated anode and cathode off-gas streams. In systems with CO2 capture, an air separation unit (ASU) is used to provide the oxygen for the ATR and for the combustion of unutilized fuel in the SOFC anode exhaust along with a CO2 purification unit to provide a nearly pure CO2 stream suitable for transport for usage in enhanced oil recovery operations or for storage in underground saline formations. Remaining thermal energy in the exhaust gases is recovered in a bottoming steam Rankine cycle while supplying any process heat requirements. A reduced order model (ROM) developed at the Pacific Northwest National Laboratory (PNNL) is used to predict the SOFC performance. The ROM, while being computationally effective for system studies, provides other detailed information about the state of the stack, such as the internal temperature gradient, generally not available from simple performance models often used to represent the SOFC. Such additional information can be important in system optimization studies to preclude operation under off-design conditions that can adversely impact overall system reliability. The NGFC system performance was analyzed by varying salient system parameters, including the percent of internal (to the SOFC module) NG reformation—ranging from 0 to 100 percent—fuel utilization, and current density. The impact of advances in underlying SOFC technology on electrical performance was also explored.

solid oxide fuel cell (SOFC), natural gas fuel cel↗

NASA NTRS1991

Oxygen isotope studies of ordinary chondrites

Several stages in the evolution of ordinary chondritic meteorites are recorded in the oxygen isotopic composition of the meteorites and their separable components (chondrules, fragments, clasts, and matrix). The whole-rock isotopic compositions reflect the iron-group of the meteorite (H, L, or LL). Isotopic uniformity of H3 to H6 and L3 to L6 are consistent with closed-system metamorphism within each parent body. LL3 chondrites differ slightly from LL4 to LL6, implying a small degree of open-system aqueous alteration and carbon reduction. On the scale of individual chondrules, the meteorites are isotopically heterogeneous, allowing recognition of the solar-nebular processes of chondrule formation. Chondrules for all classes of ordinary chondrites are derived from a common population, which was separate from the population of chondrules in carbonaceous or enstatite chondrites. Chondrules define an isotopic mixing line dominated by exchange between (O - 16)-rich and (O - 16)-poor reservoirs. The oxygen isotopic compositions of chondrites serve as 'fingerprints' for identification of genetic association with other meteorite types (achondrites and iron) and for recognition of source materials in meteoritic breccias.

Clayton, Robert N.↗

NASA NTRS2019

Oxygen Production System for Refueling Human Landing System Elements

Current NASA plans for lunar exploration include a human lunar landing system, comprised of separate descent andascent modules, with the eventual goal of reusability. Different oxygen production processes were studied to evaluatethe feasibility of producing 10 tons of oxygen per year assuming a high latitude landing location. The study includesconsideration of packaging the ISRU components on the descent module, methods to transfer the regolith from theexcavators to the processing plant which may be mounted well above the lunar surface, and general concept ofoperations for excavation, oxygen production, and liquefaction and storage. A solar-based power system was alsodesigned and packaged on the lander, including the use of direct solar thermal energy where appropriate.

Linne, Diane↗

NASA NTRS1981

Drive mechanism for the shuttle orbiter/external tank propellant disconnect

The Space Shuttle design required development of a large, 0.43-m (17-in.) nominal diameter separable disconnect for the liquid hydrogen and liquid oxygen propellant lines at the orbiter-to-external-tank interface. The disconnect must provide for shutoff of the propellant flow area by simultaneous action of two rotary flapper valves (orbiter and external tank) prior to disconnect separation. In the case of pneumatic system failure, the rotary flapper valves are closed automatically through mechanical interlocking linkage during disconnect separation. The mechanism must meet requirements while accommodating changes in bearing clearances and linkage geometry over a wide temperature range from ambient to 20.37 K (-423°F). The mechanical design of the separable disconnect, kinematics of the drive mechanism, and the analysis and test methods used to verify proper operation and qualification for the Space Shuttle dynamic environments are presented.

E. Thomas↗

DOE OSTI2021

Effect of Branch Length on the Structural and Separation Properties of Hyperbranched Poly(1,3-dioxolane)

Polymers containing poly(ethylene oxide) (PEO) demonstrate superior membrane CO 2 /N 2 separation properties owing to their polar ether oxygen groups exhibiting strong affinity toward CO2. Poly(1,3-dioxolane) (PDXL) shows an ether oxygen content higher than PEO and is expected to have higher CO 2 /N 2 solubility selectivity. However, similar to PEO, the high crystallinity of PDXL greatly reduces its gas permeability. Herein, amorphous PDXL-based hyperbranched polymers were synthesized by ring opening of 1,3-dioxolane (DXL) to form poly(1,3-dioxolane) acrylate (DXLAn) followed by photopolymerization. The repeating unit of DXL (n) or branch length was systematically varied from 4 to 12 to yield amorphous polymers. The chemical and physical properties of the obtained polymers (PDXLAn) were thoroughly evaluated and used to interpret pure- and mixed-gas transport characteristics. The polymers exhibit attractive CO 2 /N 2 and CO 2 /CH 4 separation properties. For example, PDXLA8 exhibits a CO 2 permeability of 220 Barrer and CO 2 /N 2 selectivity of 56 at 35 °C, surpassing Robeson’s 2008 upper bound, and it shows robust separation performance when evaluated with simulated flue gas at 60 °C. This study demonstrates that hyperbranched structures are an effective route to construct amorphous yet highly polar polymers and that chain end groups are instrumental in determining the structural and gas transport characteristics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2011

Mars Atmospheric Capture and Gas Separation

The Mars atmospheric capture and gas separation project is selecting, developing, and demonstrating techniques to capture and purify Martian atmospheric gases for their utilization for the production of hydrocarbons, oxygen, and water in ISRU systems. Trace gases will be required to be separated from Martian atmospheric gases to provide pure C02 to processing elements. In addition, other Martian gases, such as nitrogen and argon, occur in concentrations high enough to be useful as buffer gas and should be captured as welL To achieve these goals, highly efficient gas separation processes will be required. These gas separation techniques are also required across various areas within the ISRU project to support various consumable production processes. The development of innovative gas separation techniques will evaluate the current state-of-the-art for the gas separation required, with the objective to demonstrate and develop light-weight, low-power methods for gas separation. Gas separation requirements include, but are not limited to the selective separation of: (1) methane and water from un-reacted carbon oxides (C02- CO) and hydrogen typical of a Sabatier-type process, (2) carbon oxides and water from unreacted hydrogen from a Reverse Water-Gas Shift process, (3) carbon oxides from oxygen from a trash/waste processing reaction, and (4) helium from hydrogen or oxygen from a propellant scavenging process. Potential technologies for the separations include freezers, selective membranes, selective solvents, polymeric sorbents, zeolites, and new technologies. This paper and presentation will summarize the results of an extensive literature review and laboratory evaluations of candidate technologies for the capture and separation of C02 and other relevant gases.

Muscatello, Anthony↗