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NASA NTRS2013

Radiogenic Ingrowth of 40CA from Decay of 40K Provides a Powerful Tracer for Understanding the Origins of Felsic Magmas

Over time high K/Ca continental crust produces a unique Ca isotopic reservoir, with measurable 40Ca excesses compared to Earth's mantle (ɛCa=0). Thus, values of ɛCai > 1 indicate a significant crustal contribution to a magma. Values of ɛCai (<1) indistinguishable from mantle Ca indicate that the Ca in those magmas is either directly from the mantle, or is from partial melting of newly formed crust. So, whereas 40Ca excesses clearly define crustal contributions, mantle-like 40Ca/44Ca ratios are not as definitive. Here we present Ca isotopic measurements of intermediate to felsic igneous rocks from the western United States, and two crustal xenoliths found within the Fish Canyon Tuff (FCT). The two crustal xenoliths found within the 28.2 Ma FCT of the southern Rocky Mountain volcanic field (SRMVF) yield ɛCa values of ~4 and ~7.5, respectively. The 40Ca excesses of these possible source rocks are due to long-term in situ 40K decay and suggest that they are Precambrian in age. However, the FCT (ɛCai ~0.3) is within uncertainty of the mantle 40Ca/44Ca. Together, these data indicate that little Precambrian crust was involved in the petrogenesis of the FCT. Nd isotopic analyses of the FCT imply that it was generated from 10- 75% of an enriched component, and the Ca isotopic data appear to restrict that component to newly formed lower crust, or enriched mantle. However, the Ca isotopic data do permit assimilation of some crust with low Ca/Nd; decreasing the 143Nd/144Nd without adding much excess 40Ca to the FCT. Several other large tuffs from the SRMVF and from Yellowstone have ɛCai indistinguishable from the mantle. However, a few large tuffs from the SRMVF show significant 40Ca excesses. These tuffs (Wall Mountain, Blue Mesa, and Grizzly Peak) are likely sourced from near, or within the Colorado Mineral Belt. New isotopic measurements of Mesozoic and Tertiary granites from across the northern Great Basin show a range of ɛCai from 0 to ~3. In these samples ɛCai is generally correlated with ɛSri and is broadly negatively correlated with ɛNdi. However, for granites with similar ɛNdi at a given general location ɛCai can vary significantly (1 to 2 epsilon units). In rocks where low ɛNdi could also be due to melting from enriched reservoirs in the mantle lithosphere, the combination of high ɛCai with low ɛNdi clearly identifies crustal melts.

Mills, Ryan D.↗

NASA NTRS1994

Tank Made Of Connected Cooling Fins

New method of fabricating fin-cooled tank requires half as many arc-welding passes and features more efficient transfer of heat. Fins integral parts of tank structure. Requires only one welding pass per fin, and pass done on unobstructed inside of tank. With inside welding, fins longer and more closely spaced. Method proposed to build tank with 256 fins. Holds water in which radioisotope heat source immersed before use. Water absorbs bremsstrahlung radiation from isotope, and fins dissipate heat generated by absorption.

Schultz, Donald F.↗

NASA NTRS1994

Simulation of gamma-ray spectra for a variety of user-specified detector designs

The gamma-ray spectrum simulation program BSIMUL was designed to allow the operator to follow the path of a gamma-ray through a detector, shield and collimator whose dimensions are entered by the operator. It can also be used to simulate spectra that would be generated by a detector. Several improvements have been made to the program within the last few months. The detector, shield and collimator dimensions can now be entered through an interactive menu whose options are discussed below. In addition, spectra containing more than one gamma-ray energy can now be generated with the menu - for isotopes listed in the program. Adding isotopes to the main routine is also quite easy. Subroutines have been added to enable the operator to specify the material and dimensions of a collimator. This report details the progress made in simulating gamma-ray spectra for a variety of user-specified detector designs. In addition, a short discussion of work done in the related areas of pulse shape analysis and the spectral analysis is included. The pulse shape analysis and spectral analysis work is being performed pursuant to the requirements of contract F-94-C-0006, for the Advanced Research Projects Agency and the U.S. Air Force.

Rester, A. C., Jr.↗

NASA NTRS2015

NASA's Radioisotope Power Systems - Plans

NASA's Radioisotope Power Systems (RPS) Program continues to plan and implement content to enable planetary exploration where such systems could be needed, and to prepare more advanced RPS technology for possible infusion into future power systems. The 2014-2015 period saw significant changes, and strong progress. Achievements of near-term objectives have enabled definition of a clear path forward in which payoffs from research investments and other sustaining efforts can be applied. The future implementation path is expected to yield a higher-performing thermoelectric generator design, a more isotope-fuel efficient system concept design, and a robust RPS infrastructure maintained effectively within both NASA and the Department of Energy. This paper describes recent work with an eye towards the future plans that result from these achievements.

Program↗

NASA NTRS2013

Timescale of Petrogenetic Processes Recorded in the Mount Perkins Magma System, Northern Colorado River Extension Corridor, Arizona

The Miocene Mt. Perkins Pluton is a small composite intrusive body emplaced in the shallow crust as four separate phases during the earliest stages of crustal extension. Phase 1 (oldest) consists of isotropic hornblende gabbro and a layered cumulate sequence. Phase 2 consists of quartz monzonite to quartz monzodiorite hosting mafic microgranitoid enclaves. Phase 3 is composed of quartz monzonite and is subdivided into mafic enclave-rich zones and enclave-free zones. Phase 4 consists of aphanitic dikes of mafic, intermediate and felsic compositions hosting mafic enclaves. Phases 2-4 enclaves record significant isotopic disequilibrium with surrounding granitoid host rocks, but collectively enclaves and host rocks form a cogenetic suite exhibiting systematic variations in Nd-Sr-Pb isotopes that correlate with major and trace elements. Phases 2-4 record multiple episodes of magma mingling among cogenetic hybrid magmas that formed via magma mixing and fractional crystallization at a deeper crustal. The mafic end-member was alkali basalt similar to nearby 6-4 Ma basalt with enriched OIB-like trace elements and Nd-Sr-Pb isotopes. The felsic end-member was a subalkaline crustal-derived magma. Phase 1 isotropic gabbro exhibits elemental and isotopic compositional variations at relatively constant SiO2, suggesting generation of isotropic gabbro by an open-system process involving two mafic end-members. One end-member is similar in composition to the OIB-like mafic end-member for phases 2-4; the second is similar to nearby 11-8 Ma tholeiite basalt exhibiting low epsilon (sub Nd), and depleted incompatible trace elements. Phase 1 cumulates record in situ fractional crystallization of an OIB-like mafic magma with isotopic evidence of crustal contamination by partial melts generated in adjacent Proterozoic gneiss. The Mt Perkins pluton records a complex history in a lithospheric scale magma system involving two distinct mantle-derived mafic magmas and felsic magma sourced in the crust. Mixing and fractional crystallization of these magmas at various levels in the crust generated a suite of intermediate composition magmas. U-Pb zircon SHRIMP ages of phase 1 (15.7 +/- 0.2 Ma), phase 3 (15.8 +/- 0.2 Ma) and phase 4 (15.4 +/- 0.3 Ma) document a 100-300k year timescale for petrogenetic processes recorded in the Mt Perkins magma system.

Danielson, Lisa R.↗

NASA NTRS2013

The Origin of Carbon-bearing Volatiles in Surprise Valley Hot Springs in the Great Basin: Carbon Isotope aud Water Chemistry Characterizations

There are numerous hydrothermal fields within the Great Basin of North America, some of which have been exploited for geothermal resources. With methane and other carbon-bearing compounds being observed, in some cases with high concentrations, however, their origins and formation conditions remain unknown. Thus, studying hydrothermal springs in this area provides us an opportunity to expand our knowledge of subsurface (bio)chemical processes that generate organic compounds in hydrothermal systems, and aid in future development and exploration of potential energy resources as well. While isotope measurement has long been used for recognition of their origins, there are several secondary processes that may generate variations in isotopic compositions: oxidation, re-equilibration of methane and other alkanes with CO2, mixing with compounds of other sources, etc. Therefore, in addition to isotopic analysis, other evidence, including water chemistry and rock compositions, are necessary to identify volatile compounds of different sources. Surprise Valley Hot Springs (SVHS, 41º32'N, 120º5'W), located in a typical basin and range province valley in northeastern California, is a terrestrial hydrothermal spring system of the Great Basin. Previous geophysical studies indicated the presence of clay-rich volcanic and sedimentary rocks of Tertiary age beneath the lava flows in late Tertiary and Quaternary. Water and gas samples were collected for a variety of chemical and isotope composition analyses, including in-situ pH, alkalinity, conductivity, oxidation reduction potential (ORP), major and trace elements, and C and H isotope measurements. Fluids issuing from SVHS can be classified as Na-(Cl)-SO4 type, with the major cation and anion being Na+ and SO4 2-, respectively. Thermodynamic calculation using ORP and major element data indicated that sulfate is the most dominant sulfur species, which is consistent with anion analysis results. Aquifer temperatures at depth estimated by both dissolved SiO2 and Na-K-Ca geothermometers are in the range of 125.0 to 135.4 oC, and higher than the values measured at orifices (77.3 to 90.0 oC). CO2 and homologs of straight chain alkanes (C1-C5) were identified in gas samples. Carbon isotope values of alkanes increase with carbon numbers. The 13C fractionation between CO2 and dissolved inorganic carbon suggests they are out of carbon isotope equilibrium. The hypothesis regarding the formation of carbon-bearing compounds in SVHS may involve two processes: 1) Under high heat flow conditions which are caused by regional faulting and crustal extension, original high molecular weight organic compounds (kerogens) in clay-rich rocks decomposed to generate methane and other alkane homologs. 2) The SVHS area is associated with outflow structures, and distant from the heat source. Anaerobic oxidation of methane (AOM) with sulfate at shallow depth (< 90 oC) is suggested as being responsible for the generation of CO2 in SVHS.

Fu, Qi↗

NASA NTRS2013

The Origin of Carbon-bearing Volatiles in Surprise Valley Hot Springs in the Great Basin: Carbon Isotope and Water Chemistry Characterizations

There are numerous hydrothermal fields within the Great Basin of North America, some of which have been exploited for geothermal resources. With methane and other carbon-bearing compounds being observed, in some cases with high concentrations, however, their origins and formation conditions remain unknown. Thus, studying hydrothermal springs in this area provides us an opportunity to expand our knowledge of subsurface (bio)chemical processes that generate organic compounds in hydrothermal systems, and aid in future development and exploration of potential energy resources as well. While isotope measurement has long been used for recognition of their origins, there are several secondary processes that may generate variations in isotopic compositions: oxidation, re-equilibration of methane and other alkanes with CO2, mixing with compounds of other sources, etc. Therefore, in addition to isotopic analysis, other evidence, including water chemistry and rock compositions, are necessary to identify volatile compounds of different sources. Surprise Valley Hot Springs (SVHS, 41 deg 32'N, 120 deg 5'W), located in a typical basin and range province valley in northeastern California, is a terrestrial hydrothermal spring system of the Great Basin. Previous geophysical studies indicated the presence of clay-rich volcanic and sedimentary rocks of Tertiary age beneath the lava flows in late Tertiary and Quaternary. Water and gas samples were collected for a variety of chemical and isotope composition analyses, including in-situ pH, alkalinity, conductivity, oxidation reduction potential (ORP), major and trace elements, and C and H isotope measurements. Fluids issuing from SVHS can be classified as Na-(Cl)-SO4 type, with the major cation and anion being Na+ and SO4(2-), respectively. Thermodynamic calculation using ORP and major element data indicated that sulfate is the most dominant sulfur species, which is consistent with anion analysis results. Aquifer temperatures at depth estimated by both dissolved SiO2 and Na-K-Ca geothermometers are in the range of 125.0 to 135.4 C, and higher than the values measured at orifices (77.3 to 90.0 C). CO2 and homologs of straight chain alkanes (C1-C5) were identified in gas samples. Carbon isotope values of alkanes increase with carbon numbers. The C-13 fractionation between CO2 and dissolved inorganic carbon suggests they are out of carbon isotope equilibrium. The hypothesis regarding the formation of carbon-bearing compounds in SVHS may involve two processes: 1) Under high heat flow conditions which are caused by regional faulting and crustal extension, original high molecular weight organic compounds (kerogens) in clay-rich rocks decomposed to generate methane and other alkane homologs. 2) The SVHS area is associated with outflow structures, and distant from the heat source. Anaerobic oxidation of methane (AOM) with sulfate at shallow depth (< 90 C) is suggested as being responsible for the generation of CO2 in SVHS.

Fu, Qi↗

NASA NTRS1983

Dynamic crystallization experiments as constraints on chondrule genesis

The effectiveness of dynamic recrystallization experiments to reconstruct chondrule textures is evaluated. Consideration is given to the results of several experimental simulations of the silicate spheres of pyroxene-olivine chondrules, Si-rich chondrules, chondrites, droplet chondrules, and microporphyritic chondrules. It is shown that many chondrules have textures consistent with heating to 1400-1600 C, and cooling rates from a few degrees to several thousands of degrees per hour. It is shown that this physical constraint effectively rules out mechanisms for chondrule genesis which do not require instantaneous or very slow cooling. Analysis of the available textural, chemical, and isotopic data suggest that chondrules were generated from primordial particles, and several mechanisms might have assisted in chondrule heating as they settled down toward the median plane of the nebula. The most important of these mechanisms appear to be friction with the nebular gas and heating by flares.

Hewins, R. H.↗

NASA NTRS1971

Opacity probability distribution functions for electronic systems of CN and C2 molecules including their stellar isotopic forms.

The basis and techniques are presented for generating opacity probability distribution functions for the CN molecule (red and violet systems) and the C2 molecule (Swan, Phillips, Ballik-Ramsay systems), two of the more important diatomic molecules in the spectra of carbon stars, with a view to including these distribution functions in equilibrium model atmosphere calculations. Comparisons to the CO molecule are also shown. T he computation of the monochromatic absorption coefficient uses the most recent molecular data with revision of the oscillator strengths for some of the band systems. The total molecular stellar mass absorption coefficient is established through fifteen equations of molecular dissociation equilibrium to relate the distribution functions to each other on a per gram of stellar material basis.

Querci, F.↗

NASA NTRS2007

Isotopic Measurements in CAIs with the Nanosims: Implications to the understanding of the Formation process of Ca, Al-Rich Inclusions

Ca, Al-rich Inclusions (CAIs) preserve evidence of thermal events that they experienced during their formation in the early solar system. Most CAIs from CV and CO chondrites are characterized by large variations in O-isotopic compositions of primary minerals, with spinel, hibonite, and pyroxene being more O-16-rich than melilite and anorthite, with delta 17, O-18 = approx. -40%o (DELTA O-17 = delta O-17 - 0.52 x delta O-18 = approx. - 20%o ). These anomalous compositions cannot be accounted for by standard mass dependent fractionation and diffusive process of those minerals. It requires the presence of an anomalous oxygen reservoir of nucleosynthetic origin or mass independent fractionations before the formation of CAIs in the early solar system. The CAMECA NanoSIMS is a new generation ion microprobe that offers high sensitivity isotopic measurements with sub 100 nm spatial resolution. The NanoSIMS has significantly improved abilities in the study of presolar grains in various kind of meteorites and the decay products of extinct nuclides in ancient solar system matter. This instrument promises significant improvements over other conventional ion probes in the precision isotopic characterization of sub-micron scales. We report the results of our first O isotopic measurements of various CAI minerals from EK1-6-3 and 7R19-1(a) utilizing the JSC NanoSIMS 50L ion microprobe. We evaluate the measurement conditions, the instrumental mass fractionation factor (IMF) for O isotopic measurement and the accuracy of the isotopic ratio through the analysis of a San Carlos olivine standard and CAI sample of 7R19-1(a).

Ito, M.↗

NASA NTRS1991

Dynamic Isotope Surface Power Systems

The Dynamic Isotope Power Systems (DIPS) demonstration program, sponsored by the U.S. Department of Energy (DOE) with support funding from the National Aeronautics and Space Administration (NASA), is currently focused on the development of a standardized 2.5 kWe portable generator for multiple applications on the lunar or Martian surface. A variety of potential remote and mobile applications has been identified by NASA including surface rovers for both short and extended duration missions, remote power to science packages, and backup to central base power. Recent work focused on refining the 2.5 kWe design including assessing compatibility with the Martian environment to assure the design is suitable while imposing only a minor mass penalty on lunar operations. Additional work included a study performed to compare the DIPS with regenerative fuel cell systems for lunar mobile and remote power systems. Power requirements were reviewed and a modular system chosen for the comparison. Finally, a plan and cycle schematic were generated for an early demonstration of a prototypic isotope power Brayton system using the Antarctic as the test bed.

Hunt, Maribeth E.↗

NASA NTRS1993

Carbon and nitrogen in Type 2 supernova diamonds

Abundant diamonds found in meteorites seem either to have condensed within supernova interiors during their expansions and coolings or to have been present around those explosions. Either alternative allows implantation of Xe-HL prior to interstellar mixing. A puzzling feature is the near normalcy of the carbon isotopes, considering that the only C-rich matter, the He-burning shell, is pure C-12 in that region. That last fact has caused many to associate supernova carbon with C-12 carbon, so that its SUNOCONS have been anticipated as very C-12-rich. We show that this expectation is misleading because the C-13-rich regions of Type 2's have been largely overlooked in this thinking. We here follow the idea that the diamonds nucleated in the C-12-rich He shell, the only C-rich site for nucleation, but then attached C-13-rich carbon during turbulent encounters with overlying C-13-rich matter. That is, the initial diamonds continued to grow during the same collisional encounters that cause the Xe-HL implantation. Instead of interacting with the small carbon mass having 13/12 = 0.2 in the upper He zone, however, we have calculated the remnants of the initial H-burning core, which left behind C-13-rich matter as it receded during core hydrogen burning. Howard et al. described why the velocity mixing would be essential to understanding the implantation of both the Xe-H and Xe-L components. Velocity mixing is now known to occur from the X-ray and gamma-ray light curves of supernova 1987A. Using the stellar evolution code developed at Goettingen, we calculated at Clemson the evolution of a grid of massive stars up to the beginning of core He burning. We paid attention to all H-burning reactions throughout the star, to the treatment of both convection and semiconvection, and to the recession of the outer boundary of the convective H-burning core as the star expands toward a larger redder state. This program was to generate a careful map of the CNO isotope distribution as He burning begins. Our result for the 30 solar mass star is shown.

Clayton, Donald D.↗

NASA NTRS2001

Space Fission Propulsion System Development Status

Houts, Mike↗

NASA NTRS2001

Space Fission Propulsion System Development Status

The world's first man-made self-sustaining fission reaction was achieved in 1942. Since then fission has been used to propel submarines, generate tremendous amounts of electricity, produce medical isotopes, and provide numerous other benefits to society. Fission systems operate independently of solar proximity or orientation, and are thus well suited for deep space or planetary surface missions. In addition, the fuel for fission systems (enriched uranium) is virtually non-radioactive. The primary safety issue with fission systems is avoiding inadvertent system start. Addressing this issue through proper system design is straight-forward. Despite the relative simplicity and tremendous potential of space fission systems, the development and utilization of these systems has proven elusive. The first use of fission technology in space occurred 3 April 1965 with the US launch of the SNAP-10A reactor. There have been no additional US uses of space fission systems. While space fission systems were used extensively by the former Soviet Union, their application was limited to earth-orbital missions. Early space fission systems must be safely and affordably utilized if we are to reap the benefits of advanced space fission systems. NASA's Marshall Space Flight Center, working with Los Alamos National Laboratory (LANL), Sandia National Laboratories, and others, has conducted preliminary research related to a Safe Affordable Fission Engine (SAFE). An unfueled core has been fabricated by LANL, and resistance heaters used to verify predicted core thermal performance by closely mimicking heat from fission. The core is designed to use only established nuclear technology and be highly testable. In FY01 an energy conversion system and thruster will be coupled to the core, resulting in an 'end-to-end' nuclear electric propulsion demonstrator being tested using resistance heaters to closely mimic heat from fission. Results of the SAFE test program will be presented. The applicability of a SAFE-powered electric propulsion system to outer planet science missions will also be discussed.

Houts, M.↗

NASA NTRS2002

STARDUST and Interplanetary Dust Particles - Big Science from Small Samples

Comets are primitive bodies that are widely believed to be a reservoir of preserved interstellar and circumstellar grains, and molecular cloud materials (organics). Direct samples of cometary dust along with interstellar grains will be returned by the STARDUST Mission in 2006. Analyses of interplanetary dust particles (IDPs) and analogue materials in the laboratory provide constraints and serve as "ground truth" for evaluating various hypotheses on the nature of comets and interstellar grains. Anhydrous IDPs are the most primitive remnants of the primordial Solar System, and are our only known samples of comets. These cometary lDPs are rich in preserved interstellar organic compounds II]. In addition, abundant interstellar silicates have recently been discovered in cluster lDPs [2]. In some of these IDPs, the presolar silicate abundance reaches 1 wt %, exceeding the total presolar grain abundance in meteorites by three orders of magnitude, where presolar silicates are still notably absent. The results to date support the idea that comets are rich in presolar materials, but are at odds with the common perception that they are 'pristine aggregates of interstellar grains'. These results underscore the scientific importance of sample return missions to comets. The technology for the analysis of micrometer-sized samples is well advanced. The newest generation of ion probe instruments allow for isotopic analyses at the submicrometer level. The nature of the organic matter is analyzed using Infrared and soft X-ray spectroscopy techniques on synchrotron-based instruments, also at the micrometer-scale and smaller. Electron microscopy and spectroscopy provide details on the mineralogy and chemistry of constituent grains in !DPs at nearly the atomic scale. Novel sample preparation techniques have been developed such that all of these measurements can now be made on the same 10 micrometer diameter particle. Returned comet samples captured in aerogel will pose new challenges in sample analysis, but should provide a major leap in our understanding of the fundamental building blocks of our Solar System.

Keller, L. P.↗

NASA NTRS2012

Predicting the Sources and Formation Mechanisms of Evolved Lunar Crust by Linking K/Ca Ratios of Lunar Granites to Analogous Terrestrial Igneous Rocks

Although silicic rocks (i.e. granites and rhyolites) comprise a minor component of the sampled portion of the lunar crust, recent remote sensing studies [e.g., 1-4] indicate that several un-sampled regions of the Moon have significantly higher concentrations of silicic material (also high in [K], [U], and [Th]) than sampled regions. Within these areas are morphological features that are best explained by the existence of chemically evolved volcanic rocks. Observations of silicic domes [e.g., 1-5] suggest that sizable networks of silicic melt were present during crust formation. Isotopic data indicate that silicic melts were generated over a prolonged timespan from 4.3 to 3.9 Ga [e.g., 6-8]. The protracted age range and broad distribution of silicic rocks on the Moon indicate that their petrogenesis was an important mechanism for secondary crust formation. Understanding the origin and evolution of such silicic magmas is critical to determining the composition of the lunar crustal highlands and will help to distinguish between opposing ideas for the Moon's bulk composition and differentiation. The two main hypotheses for generating silicic melts on Earth are fractional crystallization or partial melting. On the Moon silicic melts are thought to have been generated during extreme fractional crystallization involving end-stage silicate liquid immiscibility (SLI) [e.g. 9, 10]. However, SLI cannot account for the production of significant volumes of silicic melt and its wide distribution, as reported by the remote global surveys [1, 2, 3]. In addition, experimental and natural products of SLI show that U and Th, which are abundant in the lunar granites and seen in the remote sensing data of the domes, are preferentially partitioned into the depolymerized ferrobasaltic magma and not the silicic portion [11, 12]. If SLI is not the mechanism that generated silicic magmas on the Moon then alternative processes such as fractional crystallization (only crystal-liquid separation) or partial melting should be considered as viable possibilities to be tested.

Mills, R. D.↗

NASA NTRSDate not supplied

Am-241 Powered Dynamic Radioisotope Power System (DRPS) for Long Duration Lunar Rovers

For more than half a century most deep space and planetary missions have utilised Pu-238 as the isotope of choice for fuelling radioisotope thermoelectric generators and radioisotope heater units. In Europe, Am-241 based fuel has been selected and developed as part of the European Space Agency funded radioisotope power system program to provide technology solutions in the form of radioisotope thermoelectric generators and radioisotope heater units. A concurrent design study, in collaboration with NASA Glenn Research Centre, has been undertaken to design and develop a dynamic radioisotope power conversion concept that uses the European Large Heat Source. This is a 200 Wth Am-241 based heat source being developed for ESA and is an essential building block for the University of Leicester led radioisotope thermoelectric generator programme. This study aims to expand on the applications of the Am-241 based heat source within and outside Europe. The advancement in Am-241 power technologies could give rise to a suitable and sustainable addition to current Pu-238 based technologies, making the solar system and beyond more accessible for science and exploration mission.

Dynamic Radioisotope Power System↗

NASA NTRS2010

Experimental Study of Abiotic Organic Synthesis at High Temperature and Pressure Conditions: Carbon Isotope and Mineral Surface Characterizations

Abiotic organic synthesis processes have been proposed as potential mechanisms for methane generation in subseafloor hydrothermal systems on Earth, and on other planets. To better understand the detailed reaction pathways and carbon isotope fractionations in this process under a wide range of physical and chemical conditions, hydrothermal experiments at high temperature (750 C) and pressure (0.55 GPa) were performed using piston cylinder apparatus. Formic acid was used as the source of CO2 and H2, and magnetite was the mineral catalyst. The chemical and carbon isotopic compositions of dissolved organic products were determined by GC-C-MS-IRMS, while organic intermediaries on the mineral catalyst were characterized by Pyrolysis-GC-MS. Among experimental products, dissolved CO2 was the dominant carbon species with a relative abundance of 88 mol%. Dissolved CH4 and C2H6 were also identified with a mole ratio of CH4 over C2H6 of 15:1. No dissolved CO was detected in the experiment, which might be attributable to the loss of H2 through the Au capsule used in the experiments at high temperature and pressure conditions and corresponding conversion of CO to CO2 by the water-gas shift reaction. Carbon isotope results showed that the 13C values of CH4 and C2H6 were -50.3% and -39.3% (V-PDB), respectively. CO2 derived from decarboxylation of formic acid had a (sigma)C-13 value of -19.2%, which was 3.2% heavier than its source, formic acid. The (sigma)C-13 difference between CO2 and CH4 was 31.1%, which was higher than the value of 9.4% calculated from theoretical isotopic equilibrium predictions at experimental conditions, suggesting the presence of a kinetic isotope effect. This number was also higher than the values (4.6 to 27.1%) observed in similar experiments previously performed at 400 C and 50 MPa with longer reaction times. CH4 is 11.0% less enriched in C-13 than C2H6. Alcohols were observed as carbon compounds on magnetite surfaces by Pyrolysis-GC-MS, which confirms the hypothesis regarding the reaction pathways of hydrothermal abiotic organic synthesis proposed by Fu et al. (2007, 2008). In this proposed pathway, hydroxymethylene (-CHOH) groups serve as organic intermediaries on mineral surfaces while dissolved H2 serves as a chain terminator/breaker to generate short chain hydrocarbons and oxygenated compounds. This pathway is different from the carbide polymerization theory of Fischer- Tropsch-type (FTT) synthesis in a gas phase. The observed increase of (sigma)C-13 values of C1 and C2 alkanes with carbon number in our hydrothermal experiments can be readily interpreted by hydroxymethylene pathway, and might be used to differentiate between hydroxymethylene and carbide polymerization pathways. Carbon isotope analysis of alcohols on mineral catalyst surfaces is under way to provide further constraints on formation of organic compounds by FTT in hydrothermal systems.

Fu, Qi↗