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NASA NTRS2006

Following the Water: the Evolution of Ice-forming Regions in the Early Solar Nebula

The abundances of water-vapor and water-ice during the first ten million years of the protoplanetary solar nebula are simulated using a new condensation/sublimation model. This study builds on a "snow line" model reported in ApJ 627 L153 (2005); it uses a simple phenomenological model where water vapor molecules evolve from solar atomic abundance and eventually condenses to ice at colder points in the nebula once the water-vapor partial pressure exceeds a value determined by the phase diagram for water. The synthesis of water vapor from elementary species is modeled with a chemical network consisting of about 400 species and 4000 reactions. The evolution of the icy zone (and its relative abundance of solid ice) is traced from a limited region in the early hotter disk to its final state at the time when the gas is expelled and a planetary system begins to form. Possible effects of this dynamic motion on disk chemistry and organic molecule formation are also described.

Davis, Sanford S.↗

NASA NTRS2000

Biological Moleculars: Have Most of Our Problems Already Been Solved?

Evolution has resulted in biological machinery that engineers have great reason to envy and at present can only poorly mimic. This is not just a curiosity as biological systems perform many functions that are desired industrial processes. Examples include photosynthesis, chemosynthesis, energy storage, low temperature chemical conversion, reproducible manufacture of chemical compounds, etc. The bases of biological machinery are the proteins and nucleic acids that comprise living organisms. Each molecule functions as a part of a biological machine. In many cases the molecule can be properly regarded as a stand alone machine of its own. Concepts and methods for harnessing the power of biological molecules exist but are often overlooked in the industrial world. Some are old and appear crude but are quite effective, e.g. the fermentation of grains and fruits. Currently, there is a revolution in progress regarding the harnessing biological processes. These include techniques such as genetic manipulation via polymerase chain reaction, forced evolution also known as evolution in a test tube, determination of molecular structure, and combinatorial chemistry. The following is a brief discussion on how these processes are performed and how they may relate to industrial and aerospace processes.

Downey, James P.↗

NASA NTRS1994

Evolution of heliobacteria: implications for photosynthetic reaction center complexes

The evolutionary position of the heliobacteria, a group of green photosynthetic bacteria with a photosynthetic apparatus functionally resembling Photosystem I of plants and cyanobacteria, has been investigated with respect to the evolutionary relationship to Gram-positive bacteria and cyanobacteria. On the basis of 16S rRNA sequence analysis, the heliobacteria appear to be most closely related to Gram-positive bacteria, but also an evolutionary link to cyanobacteria is evident. Interestingly, a 46-residue domain including the putative sixth membrane-spanning region of the heliobacterial reaction center protein show rather strong similarity (33% identity and 72% similarity) to a region including the sixth membrane-spanning region of the CP47 protein, a chlorophyll-binding core antenna polypeptide of Photosystem II. The N-terminal half of the heliobacterial reaction center polypeptide shows a moderate sequence similarity (22% identity over 232 residues) with the CP47 protein, which is significantly more than the similarity with the Photosystem I core polypeptides in this region. An evolutionary model for photosynthetic reaction center complexes is discussed, in which an ancestral homodimeric reaction center protein (possibly resembling the heliobacterial reaction center protein) with 11 membrane-spanning regions per polypeptide has diverged to give rise to the core of Photosystem I, Photosystem II, and of the photosynthetic apparatus in green, purple, and heliobacteria.

NASA Program Exobiology↗

NASA NTRS1988

The evolution of nitrogen cycling

The energetics of nitrogen transformation reactions and the evolution of nitrogen cycling are examined. It is suggested that meteor impact-produced fixed nitrogen could have caused the entire reservoir of the earth's N2 to convert into fixed nitrogen at the end of accretion. The abiotic fixation rate on the early earth by lightning is estimated at about 1-3 X 10 to the 16th molecules of NO/J. It is found that biological nitrogen fixation may have evolved after the development of an aerobic atmosphere. It is shown that HNO could eventually become NO2(-) and NO3(-) after reaching the earth's surface. It is concluded that the evolutionary sequence for the biological transformation of nitrogen compounds is ammonification - denitrification - nitrification - nitrogen fixation.

Mancinelli, Rocco L.↗

NASA NTRS1999

Observations from the Microgravity Smoldering Combustion (MSC) Ultrasound Imaging System (UIS)

The Microgravity Smoldering Combustion (MSC) experiment is a study of the smolder characteristics of porous combustible materials in a microgravity environment. The objective of the study is to provide a better understanding of the controlling mechanisms of smolder, both in microgravity and normal earth gravity. Experiments have been conducted aboard the NASA Space Shuttle in the GAS-CAN, an apparatus requiring completely remote operation. Future GAS-CAN experiments will utilize an ultrasound imaging system (UIS). Thermocouples are currently used to measure temperature and reaction front velocities, but a less intrusive method is desirable, as smolder is affected by heat transfer along the thermocouple. It is expected that the UIS will eventually replace the existing array of thermocouples as a non-intrusive technique without compromising data acquisition. Smoldering is defined as a non-flaming, self-sustaining, propagating, exothermic, surface reaction, deriving its principal heat from heterogeneous oxidation of the fuel. Smolder of cable insulation is of particular concern in the space program; to date there have been a few minor incidents of overheated and charred cables and electrical components reported on Space Shuttle flights. Recently, the establishment of the International Space Station and other space facilities has increased interest in the study of smoldering in microgravity because of the need to preempt the possibility, and/or to minimize the effect of a smolder initiated fire during the operation of these facilities. The ignition and propagation of smolder are examined using both thermocouples and the UIS. The UIS has been implemented into the MSC flight hardware. The system provides information about local permeability variations within a smoldering sample, which can, in turn, be interpreted to track the propagation of the smolder reaction. The method utilizes the observation that transmission of an ultrasonic signal through a porous material increases with increasing permeability. Since a propagating smolder reaction leaves behind a char that is higher in permeability than the original (unburnt) material, ultrasonic transmission can be employed to monitor the progress of the primary reaction front, char evolution (i.e. material left by the smolder reaction), pyrolysis, and condensation fronts.

Walther, D.C.↗

NASA NTRS1974

Hot hydrogen atoms - Initiators of reactions of interest in interstellar chemistry and evolution

Hot hydrogen atoms possess kinetic (or translational) energy in excess of that to be expected if the atoms were in thermal equilibrium with the surroundings. In the investigation reported the hot hydrogen atoms were generated by the photolysis of donor molecules. The light sources for the photolysis were 1000-watt xenon or 500-watt mercury lamps combined with a filter system. The experiments show that hot hydrogen atoms can initiate reactions among simple molecules to produce biomolecules of significance.

Hong, K.-Y.↗

NASA NTRS1982

Chemical evolution. XL - Clay-mediated oxidation of diaminomaleonitrile

The inhibition of the oligomerization of HCN by montmorillonite clays is shown to be caused by oxidation of diaminomaleonitrile (DAMN) by ferric ion in the clay lattice, with ferrous ion and oxalic acid the reaction products. It is demonstrated that diiminosuccinonitrile is the initial reaction product and is rapidly hydrolized to oxalic acid and HCN. The same oxidative transformations are effected by ferric ion bound to Dowex 50, ferric ion in solution, and Ni(NH3)6(2+). The rate of reaction of DAMN indicates no catalytic role for the clay in the oxidation of DAMN, and little reaction of the latter was observed with montmorillonite in which the bulk of the iron was in the divalent state. The possible significance of these redox reactions to chemical evolution is discussed.

Ferris, J. P.↗

NASA NTRS2002

Oxygen Mass Flow Rate Generated for Monitoring Hydrogen Peroxide Stability

Recent interest in propellants with non-toxic reaction products has led to a resurgence of interest in hydrogen peroxide for various propellant applications. Because peroxide is sensitive to contaminants, material interactions, stability and storage issues, monitoring decomposition rates is important. Stennis Space Center (SSC) uses thermocouples to monitor bulk fluid temperature (heat evolution) to determine reaction rates. Unfortunately, large temperature rises are required to offset the heat lost into the surrounding fluid. Also, tank penetration to accomodate a thermocouple can entail modification of a tank or line and act as a source of contamination. The paper evaluates a method for monitoring oxygen evolution as a means to determine peroxide stability. Oxygen generation is not only directly related to peroxide decomposition, but occurs immediately. Measuring peroxide temperature to monitor peroxide stability has significant limitations. The bulk decomposition of 1% / week in a large volume tank can produce in excess of 30 cc / min. This oxygen flow rate corresponds to an equivalent temperature rise of approximately 14 millidegrees C, which is difficult to measure reliably. Thus, if heat transfer were included, there would be no temperature rise. Temperature changes from the surrounding environment and heat lost to the peroxide will also mask potential problems. The use of oxygen flow measurements provides an ultra sensitive technique for monitoring reaction events and will provide an earlier indication of an abnormal decomposition when compared to measuring temperature rise.

Ross, H. Richard↗

NASA NTRS1971

The role of phosphates in chemical evolution.

The hypohydrous thermal reaction between inorganic phosphates and nucleoside was investigated. The products of the reactions have been identified, and an attempt has been made to determine the mechanism. It was found that orthophosphates can be readily converted into condensed phosphates which are effective phosphorylating agents. Thermal polymerization of inorganic orthophosphates at moderate temperature as a general source of polyphosphates might have provided efficient phosphorylation and condensing agents for primordial syntheses.

Ponnamperuma, C.↗

NASA NTRS1973

Chemical evolution of cosmic clouds

Reaction rate characteristics of interstellar matter were studied by the reaction of hydrogen cyanide and molecular hydrogen at about 1000 K at an HCN to H2 ratio of 1 to 100 to simulate the large excess of cosmic hydrogen. It was found that HCN decays with a half life of about 20 hours and that a large surface increases the reaction rate as a function of temperature. Reaction rates may be considerable increased by energetic processes that produce free radicals and ions.

Down, B. D.↗

NASA NTRS2002

Continuous In Vitro Evolution of a Ribozyme that Catalyzes Three Successive Nucleotidyl Addition Reactions

Variants of the class I ligase ribozyme, which catalyzes joining of the 3' end of a template bound oligonucleotide to its own 5' end, have been made to evolve in a continuous manner by a simple serial transfer procedure that can be carried out indefinitely. This process was expanded to allow the evolution of ribozymes that catalyze three successive nucleotidyl addition reactions, two template-directed mononucleotide additions followed by RNA ligation. During the development of this behavior, a population of ribozymes was maintained against an overall dilution of more than 10(exp 406). The resulting ribozymes were capable of catalyzing the three-step reaction pathway, with nucleotide addition occurring in either a 5' yieldig 3' or a 3' yielding 5' direction. This purely chemical system provides a functional model of a multi-step reaction pathway that is undergoing Darwinian evolution.

McGinness, Kathleen E.↗

NASA NTRS1982

Thermonuclear processes and accretion onto neutron star envelopes - X-ray burst and transient sources

A Lagrangian, fully implicit, one-dimensional hydrodynamic computer code is used to investigate the evolution of thermonuclear runaways in the thick accreted hydrogen-rich envelopes of 1.0-solar-mass neutron stars having radii of 10 km and 20 km. The simulations produce outbursts that range in time scale from about 2000 seconds to more than a day. For the 10-km study, the peak effective temperature is 3.3 x 10 to the 7th K, and the peak luminosity is 2 x 10 to the 5th solar luminosities. The 20-km neutron star produces a peak effective temperature and luminosity of 5.3 x 10 to the 6th K and 5.9 x 10 to the 2nd solar luminosities. Also investigated are the effects of changes in the rates of the O-14(alpha, proton) and O-15(alpha, gamma) reactions on the evolution. Hydrodynamic expansion on the 10-km neutron star produces a precursor lasting about 10 to the -6th sec. The evolution of a gas cloud impacting the surface of a 20-km, 1-solar-mass neutron star is studied in an attempt to simulate the magnetospheric gate model of the X-ray burst sources.

Starrfield, S.↗

NASA NTRS1993

The mineralogic evolution of the Martian surface through time: Implications from chemical reaction path modeling studies

Chemical reaction path calculations were used to model the minerals that might have formed at or near the Martian surface as a result of volcano or meteorite impact driven hydrothermal systems; weathering at the Martian surface during an early warm, wet climate; and near-zero or sub-zero C brine-regolith reactions in the current cold climate. Although the chemical reaction path calculations carried out do not define the exact mineralogical evolution of the Martian surface over time, they do place valuable geochemical constraints on the types of minerals that formed from an aqueous phase under various surficial and geochemically complex conditions.

Plumlee, G. S.↗

NASA NTRS1973

Spectroscopic and photochemical study of molecules important in chemical evolution

The primary broad goals of this research are to investigate (1) the possible reactions responsible for generation of compounds important in chemical evolution, and (2) reactions of compounds important in chemical evolution. In both cases the interest includes molecules that exist in interstellar space as well as those present on or near other planets and those which were thought to be present on or near the primitive earth.

Becker, R. S.↗

NASA NTRS1972

Chemical evolution of dense clouds

Chemical processes that could determine the molecular composition of the cloud during the several stages of its evolution are considered. Reactions at the relatively interstellar densities are emphasized.

Chappelle, E. W.↗

NASA NTRS1986

Systematic development of reduced reaction mechanisms for dynamic modeling

A method for systematically developing a reduced chemical reaction mechanism for dynamic modeling of chemically reactive flows is presented. The method is based on the postulate that if a reduced reaction mechanism faithfully describes the time evolution of both thermal and chain reaction processes characteristic of a more complete mechanism, then the reduced mechanism will describe the chemical processes in a chemically reacting flow with approximately the same degree of accuracy. Here this postulate is tested by producing a series of mechanisms of reduced accuracy, which are derived from a full detailed mechanism for methane-oxygen combustion. These mechanisms were then tested in a series of reactive flow calculations in which a large-amplitude sinusoidal perturbation is applied to a system that is initially quiescent and whose temperature is high enough to start ignition processes. Comparison of the results for systems with and without convective flow show that this approach produces reduced mechanisms that are useful for calculations of explosions and detonations. Extensions and applicability to flames are discussed.

Frenklach, M.↗

NASA NTRS1992

SiC particles from asymptotic giant branch stars - Mg burning and the s-process

The question of whether isotopically anomalous SiC particles found in meteorites originate in AGB stars is addressed. It is shown that if the peak helium shell flash temperatures of massive (6-9 solar masses) stars are about 10 percent larger than they are normally assumed to be, alpha particle reactions with the magnesium will become significant. Then the (Mg-29)(alpha, n)Si-29 reaction produces a large excess of Si-29. With a light element nuclear reaction network, the evolution of the silicon isotopic composition during AGB evolution is calculated. It is found that the experimentally determined correlation between excess Si-29 and excess Si-30 in SiC particles from carbonaceous chondrites can indeed be naturally produced in this way. It is suggested that if the large isotopically anomalous SiC particles carrying nearly pure-process krypton and xenon do indeed originate in AGB stars, those stars were massive and had peak shell flash temperatures near 450 KM.

Brown, Lawrence E.↗

NASA NTRS1976

The chemistry of planetary atmospheres

Present knowledge concerning the chemistry of planetary atmospheres is reviewed along with the theories which attempt to explain observational data. The known gross atmospheric compositions of the terrestrial and giant planets are listed, differences between the atmospheres of earth and Venus are discussed, and the atmospheres of the giant planets are described. The origin and evolution of the atmospheres of earth, Venus, Mars, Jupiter, Saturn, and Uranus are outlined, and chemical processes in the atmospheres are examined, particularly cloud formation. The question of organic synthesis and evolution in the reducing atmospheres of the giant planets is considered. It is noted that laboratory work on the individual chemical processes and reactions involved in the evolution of organic compounds in planetary atmospheres, comets, and interstellar space points to the inevitability of organic-compound synthesis in all these situations and to the pervasiveness of organic chemistry throughout the universe.

Huntress, W. T., Jr.↗