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NASA NTRS1992

Spectral identification of chemisorbed CO2 and application to Mars analog materials

The goal of this work is to identify the spectral signature of chemisorbed CO2, to test the efficacy of carbonate formation on Mars-analog materials via CO2 chemisorption, and to identify the surface-chemical characteristics of good chemisorbents, with the intent of assessing the possible geochemical importance of CO2 chemisorption as a quasipermanent CO2 sink in the Martian environment. Our approach is to search for infrared spectral bands that result from chemisorption of CO2 molecules onto chemical reagents and Mars-analog materials, and to identify the salient differences in adsorbents that favor strong, permanent CO2 chemisorption. The total amount of CO2 in the early Martian atmosphere, and consequent surface temperatures, are unknown. A CO2 greenhouse may not have been an adequate mechanism under any circumstances; however, it if were, then most of that CO2 must still be in the near-surface environment; no escape mechanism that could remove it after the decline of channeling has been identified. The only plausible reservoir is carbonate, and there are various remote sensing techniques that can be used to search for it. We are investigating CO2 chemisorption as a permanent CO2 sink, and to aid in interpretation of remotely sensed IR spectra of Mars. A common effect reported in CO2 adsorption studies is the formation of a layer of carbonate or bicarbonate anions on adsorbents that have OH- groups available on their surfaces. Inorganic hydroxyls occur on phyllosilicates, amorphous silicates, metal oxides and hydroxides; it is the most abundant and reactive surface functional group on the surfaces of terrestrial silicates. The process responsible for the reaction is chemisorption. Chemisorption is distinguished from physical adsorption in that there is a transfer of electrons between species, and the formation of a chemical bond. The heat of chemisorption is typically of the same order as heats of chemical reaction (i.e., a few hundred to a few thousand kJ/mole), as opposed to heats of physical adsorption (a few kJ per mole). Chemisorption is an activated process that is promoted by an increase in temperature - quite the opposite of physical adsorption. Chemisorption is not reversible in the sense that physical adsorption is.

Zent, A. P.↗

NASA NTRS1989

Photochemistry of biogenic gases

The relationship between the biosphere and the atmosphere is examined, emphasizing the composition and photochemistry and chemistry of the troposphere and stratosphere. The reactions of oxygen, ozone, and hydroxyl are reviewed and the fate of the biogenic gases ammonia, methane, reduced sulfur species, reduced halogen species, carbon monoxide, nitric oxide, nitrous oxide, nitrogen, and carbon dioxide are described. A list is given of the concentration and sources of the various gases.

Levine, Joel S.↗

NASA NTRS1992

Hybrid rocket fuel combustion and regression rate study

The objectives of this study are to develop hybrid fuels (1) with higher regression rates and reduced dependence on fuel grain geometry and (2) that maximize potential specific impulse using low-cost materials. A hybrid slab window motor system was developed to screen candidate fuels - their combustion behavior and regression rate. Combustion behavior diagnostics consisted of video and high speed motion pictures coverage. The mean fuel regression rates were determined by before and after measurements of the fuel slabs. The fuel for this initial investigation consisted of hydroxyl-terminated polybutadiene binder with coal and aluminum fillers. At low oxidizer flux levels (and corresponding fuel regression rates) the filled-binder fuels burn in a layered fashion, forming an aluminum containing binder/coal surface melt that, in turn, forms into filigrees or flakes that are stripped off by the crossflow. This melt process appears to diminish with increasing oxidizer flux level. Heat transfer by radiation is a significant contributor, producing the desired increase in magnitude and reduction in flow dependency (power law exponent) of the fuel regression rate.

Strand, L. D.↗

NASA NTRS1993

Molecular-Weight-Controlled, End-Capped Polybenzimidazoles

Novel molecular-weight-controlled end-capped poly(arylene ether benzimidazole)s (PAEBI's) prepared by nucleophilic displacement reaction of di(hydroxyl)benzimidazole monomers with activated aromatic dihalides. Polymers prepared at various molecular weights by upsetting stoichiometry of monomers and end-capped with monohydroxybenzimidazole. Exhibit favorable physical and mechanical properties, improved solubility in polar aprotic solvents and better compression moldability. Potential applications as adhesives, coatings, films, fibers, membranes, moldings, and composite matrix resins.

Connell, John W.↗

NASA NTRS1991

Source gases: Concentrations, emissions, and trends

Source gases are defined as those gases that influence levels of stratospheric ozone (O3) by transporting species containing halogen, hydrogen, and nitrogen to the stratosphere. Examples are the CFC's, methane (CH4), and nitrous oxide (N2O). Other source gases that also come under consideration in an atmospheric O3 context are those that are involved in the O3 or hydroxyl (OH) radical chemistry of the troposphere. Examples are CH4, carbon monoxide (CO), and nonmethane hydrocarbons (NMHC's). Most of the source gases, along with carbon dioxide (CO2) and water vapor (H2O), are climatically significant and thus affect stratospheric O3 levels by their influence on stratospheric temperatures. Carbonyl sulphide (COS) could affect stratospheric O3 through maintenance of the stratospheric sulphate aerosol layer, which may be involved in heterogeneous chlorine-catalyzed O3 destruction. The previous reviews of trends and emissions of source gases, either from the context of their influence on atmospheric O3 or global climate change, are updated. The current global abundances and concentration trends of the trace gases are given in tabular format.

Fraser, Paul J.↗

NASA NTRS1991

The vibrational spectrum of H2O3: An ab initio investigation

Theoretically determined frequencies and absorption intensities are reported for the vibrational spectrum of the covalent HOOOH and hydrogen bonded HO---HOO intermediates that may form in the reaction of the hydroxyl and hydroperoxyl radicals. Basis sets of DZP quality, augmented by diffuse and second sets of polarization functions have been used with CASSCF wave functions. The calculated harmonic vibrational frequencies of HOOOH have been corrected with empirical factors and presented in the form of a 'stick' spectrum. The oxygen backbone vibrations, predicted to occur at 519, 760, and 870 cm(exp -1), are well separated from most interferences, and may be the most useful for the species' identification. In the case of the hydrogen bonded isomer, emphasis has been placed upon prediction of the shifts in the intramolecular vibrational frequencies that take place upon formation of the complex. In particular, the HO stretch and HOO bend of HO2 are predicted to have shifts of -59 and 53 cm(exp -1), respectively, which should facilitate their identification. It is also noted that the antisymmetric stretching frequency of the oxygen backbone in HOOOH exhibits a strong sensitivity to the degree of electron correlation, such as has been previously observed for the same mode in ozone.

Jackels, Charles F.↗

NASA NTRS1992

Resonance lamp absorption measurement of OH number density and temperature in expansion tube scramjet engine tests

In this paper, we report results of hydroxyl radical and static temperature measurements performed in the General Applied Science Laboratories-NASA HYPULSE expansion tube facility using the microwave resonance lamp absorption technique. Data were obtained as part of a series of hydrogen/air and hydrogen/oxygen combustion tests at stagnation enthalpies corresponding to Mach 17 flight speeds. Data from a representative injector configuration is compared to a full Navier-Stokes CFD solution.

Lempert, Walter R.↗

NASA NTRS1992

Velocity distributions of H and OH produced through solar photodissociation of H2O

The calculated velocity distributions of atomic hydrogen and hydroxyl radicals produced through solar photodissociation of gaseous water molecules are presented. Under collisionless conditions, the calculation was carried out using the most recent available data for the production of H and OH through photodissociation of H2O from its dissociation onset throughout the EUV region. Because the lack of data in certain spectral regions, only upper and lower bounds to the velocity distributions can be obtained. The results show that the H atoms and OH radicals produced exhibit multiple velocity groups. Since most of the current cometary modeling uses a single velocity of 20 km/s associated with the photodissociation of H2O, the present results may be useful in interpreting the many peaks observed in the velocity distributions of cometary atomic hydrogen.

Wu, C. Y. Robert↗

NASA NTRS1993

Status of the CNRS-LCSR program on high pressure droplet vaporization and burning

Depending on the surrounding flow and thermodynamic conditions, a single droplet may experience several gasification regimes, ranging from the envelope flame regime to pure vaporization. In practical situations, such as rocket propulsion or diesel combustion, the size distribution of droplets is, at best, bimodal, so that the possibility exists for the simultaneous presence of various regimes. For example, very small droplets are transported by the gas phase with zero relative velocity. This picture validates then the spherical symmetry hypothesis applied to the droplet and to the diffusion flame enveloping it. On the other hand, for larger droplets, a relative velocity exists due to drag forces. The most important influence of forced convection on droplet burning is the possibility to extinguish globally the envelope flame, or to establish a flame stabilized in the wake region. The burning rates of these regimes differ strongly. The characteristic time of droplet gasification is also influenced by the surrounding pressure and temperature. A parametric investigation of single droplet burning regimes is then helpful in providing the necessary physical ideas for sub-grid models used in spray combustion numerical prediction codes. The CNRS-LCSR experimental program on droplet vaporization and burning deals with these various regimes: stagnant and convective monocomponent droplet burning convective mono and bicomponent droplet vaporization; high temperature convective mono and biocomponent droplet vaporization; burning regimes of hydrazine and hydroxyl-ammonium-nitrate based monopropellant droplets and the vaporization regimes of liquid oxygen droplets. Studies on interacting droplets and on liquid aluminum droplets will start in the near future. The influence of high pressure is a common feature of all these studies. This paper summarizes the status of the CNRS-LCSR program on the effects of high pressure on monocomponent single droplet burning and vaporization, and some recent results obtained under normal and reduced gravity conditions with suspended droplets are presented. In the work described here, parabolic flights of an aircraft is used to create a reduced gravity environment of the order of 10(exp -2) g.

Chauveau, Christian↗

NASA NTRS1993

Molecular processes in comets

A major effort was expended in developing procedures for calculating by quantum-mechanical methods the cross sections for the photodissociation of the hydroxyl radical OH. The molecule OH is the primary dissociation product of water and observations of OH when combined with a determination of the lifetime of OH in the solar radiation field can be used to calculate the rate of release of water from comets. There are many possible photodissociation channels whose efficiency depends upon the details of the spectrum of the radiation. We have calculated the potential energy curves of all the states of OH that can be reached by electric dipole absorption from the ground X(exp 2)(Pi) state by photons with energies up to about 12 eV.

Dalgarno, A.↗

NASA NTRS1992

Summertime measurements of selected nonmethane hydrocarbons in the Arctic and Subarctic during the 1988 Arctic Boundary Layer Expedition (ABLE 3A)

The concentration distributions of several nonmethane hydrocarbons (NMHIC) in the Arctic and Subarctic regions of Alaska are discussed using data obtained during July and August of 1988 as part of the Arctic Boundary Layer Expedition (ABLE 3A). Plume enhancement of some or all of the measured NMHIC were observed on more than half of the 33 missions flown during the project. The usual summer vertical profile of reactive hydrocarbons at these high latitudes has elevated concentrations at high altitudes, with mixing ratio variations largely controlled by hydroxyl radical reactions. Wildfires were established as a significant source of various NMHIC. Biomass burning emission ratios relative to ethane were established for ethyne (0.38 +/- 0.04) and propane (0.08 +/- 0.03). Activities associated with oil drilling are a probable source of enhanced levels of alkanes observed as much as 300 km northeast of Prudhoe Bay.

Blake, Donald R.↗

NASA NTRS1992

Simultaneous temperature and multispecies measurement in a lifted hydrogen diffusion flame

UV spontaneous vibrational Raman scattering and laser-induced predissociative fluorescence (LIPF) techniques are combined and applied to a lifted hydrogen jet diffusion flame. Simultaneous, temporally and spatially resolved point measurements of temperature, major species concentrations (H2, O2, N2, H2O), and absolute hydroxyl radical concentration (OH) are obtained with a 'single' excimer laser for the first time. For OH measurements, the use of LIPF makes quenching corrections unnecessary. Results demonstrate that fuel and oxidizer are in a rich, premixed, and unignited condition in the center core of the lifted flame base. In the lifted zone, combustion occurs in an intermittent annular turbulent flame brush and strong finite-rate chemistry effects result in nonequilibrium values of temperature, major species, and OH radicals. Downstream in the slow three-body recombination zone, the major species concentrations are in partial equilibrium, the OH concentrations are in superequilibrium, and the temperatures are in subequilibrium. Far downstream in the flame, equilibrium values of temperature, OH radical, and major species are found.

Cheng, T. S.↗

NASA NTRS1992

Post-treatment of reclaimed waste water based on an electrochemical advanced oxidation process

The purification of reclaimed water is essential to water reclamation technology life-support systems in lunar/Mars habitats. An electrochemical UV reactor is being developed which generates oxidants, operates at low temperatures, and requires no chemical expendables. The reactor is the basis for an advanced oxidation process in which electrochemically generated ozone and hydrogen peroxide are used in combination with ultraviolet light irradiation to produce hydroxyl radicals. Results from this process are presented which demonstrate concept feasibility for removal of organic impurities and disinfection of water for potable and hygiene reuse. Power, size requirements, Faradaic efficiency, and process reaction kinetics are discussed. At the completion of this development effort the reactor system will be installed in JSC's regenerative water recovery test facility for evaluation to compare this technique with other candidate processes.

Verostko, Charles E.↗

NASA NTRS1993

Development and testing of 11- and 24-inch hybrid motors under the joint government/industry IR&D program

Establishment of a test facility and associated 11-in.-diameter motor for hybrid propulsion technology development at NASA's George C. Marshall Space Flight Center is discussed in this paper. Results of twenty 11-in.-diameter motor tests with a UTF-29901 (60 percent polycyclopentadiene, 40 percent hydroxyl-terminated polybutadiene)/gaseous oxygen propellant system are presented. Tests at this scale have developed fuel regression correlations for comparison with results of yet-to-be-completed, 24-in.-diameter motor tests; demonstrated combustion efficiency levels in the 95 percent range for both single- and multiple-port grain configurations; have shown smooth and stable throttling characteristics over flight-type throttle ranges; and have begun to establish criteria for stable combustion in hybrid motors. The testing of 24-in. motors has not as yet been initiated and is not addressed.

Boardman, T. A.↗

NASA NTRS1993

Rate constants for the reactions of OH with HFC-134a (CF3CH2F) and HFC-134 (CHF2CHF2)

Measurements of rate constants for HFC-134 (CF2HCF2H) relative to CH3CCl3, HFC-125, and HFC-134a are reported. The measurements were made in a slow-flow, temperature controlled photochemical reactor, and were based on relative rates of disappearance of the parent compounds as measured by FTIR spectroscopy. Hydroxyl radicals were generated by 254-nm photolysis of O3 in the presence of water vapor. NASA/JPL rate constants for the reference compounds are used to derive temperature-dependent rate constants of both compounds. Rate constants obtained from the different reference compounds are in excellent agreement. The presently recommended rate constant for HFC-134a is about 25 percent too high.

Demore, W. B.↗

NASA NTRS1993

An aircraft instrument design for in situ tropospheric OH measurements by laser induced fluorescence at low pressures

The hydroxyl radical (OH) is important for many processes involved in tropospheric chemistry. For instance, it initiates the photochemical degradation of gases that cause global climate change, such as methane and the chlorofluorocarbon substitutes (HCFCs). Because of its reactivity, its abundances are less than 0.1 pptv. Thus, OH has been very difficult to measure accurately, despite its importance. Techniques have evolved, however, so that good measurements of tropospheric OH abundances are now possible. One of these techniques that is adaptable to aircraft measurements is the laser induced fluorescence detection of the OH radical in a detection chamber at low pressures. The current ground-based instrument, which can be readily adapted to aircraft, can detect OH abundances of 1.4 x 10 exp 5 OH molecules/cu cm with S/N = 2 in 30 sec, and 5 x 10 exp 4/cu cm in 5 min.

Brune, William H.↗

NASA NTRS1993

Isolation of new ribozymes from a large pool of random sequences

An iterative in vitro selection procedure was used to isolate a new class of catalytic RNAs (ribozymes) from a large pool of random-sequence RNA molecules. These ribozymes ligate two RNA molecules that are aligned on a template by catalyzing the attack of a 3'-hydroxyl on an adjacent 5'-triphosphate - a reaction similar to that employed by the familiar protein enzymes that synthesize RNA. The corresponding uncatalyzed reaction also yields a 3',5'-phosphodiester bond. In vitro evolution of the population of new ribozymes led to improvement of the average ligation activity and the emergence of ribozymes with reaction rates 7 million times faster than the uncatalyzed reaction rate.

Bartel, David P.↗

NASA NTRS1955

Chemical Action of Halogenated Agents in Fire Extinguishing

The action of halogenated agents in preventing flame propagation in fuel-air mixtures in laboratory tests is discussed in terms of a possible chemical mechanism. The mechanism chosen is that of chain-breaking reactions between agent and active particles (hydrogen and oxygen atoms and hydroxyl radicsls). Data from the literature on the flammability peaks of n-heptane agent-air mixtures are treated. Ratings of agent effectiveness in terms of the fuel equivalent of the agent, based on both fuel and agent concentrations at the peak, are proposed as preferable to ratings in terms of agent concentration alone. These fuel-equivalent ratings are roughly correlated by reactivities assigned to halogen and hydrogen atoms in the agent molecules. It is concluded that the presence of hydrogen in agent need not reduce its fire-fighting ability, provided there is enough halogen to make the agent nonflammable. A method is presented for estimating from quenching-distance data a rate constant for the reaction of agent with active particles. A quantitative result is obtained for methyl bromide. This rate constant predicts the observed peak concentration of methyl bromide quite well. However, more data are needed to prove the validity of the method. The assumption that hal.ogenatedagents act mainly by chain-bresking reactions with active particles is consistent with the experimental facts and should help guide the selection of agents for further tests.

Belles, Frank E.↗