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Diamond thin films were deposited on copper substrate by the Vapor Solid (VS) deposition method using a mixture of fullerene C(sub 60) and graphite as the source material. The deposition took place only when the substrate was kept in a narrow temperature range of approximately 550-650 C. Temperatures below and above this range results in the deposition of fullerenes and other carbon compounds, respectively.
Solid evidence of liquid water in primitive meteorites is given by the ordinary chondrites H5 Monahans (1998) and H3-6 Zag. Aqueous fluid inclusion-bearing halite (NaCl) crystals were shown to be common in Zag. These striking blue/purple crystals (Figure 1), which gained the coloration from electron-trapping in the Cl-vacancies through exposure to ionizing radiation, were determined to be over 4.0-4.7 billion years old by I-Xe dating. The halite grains are present as discrete grains within an H-chondrite matrix with no evidence for aqueous alteration that indicates a xenogenic source, possibly ancient cryovolcanism. They were proposed to be formed from the cryovolcanic plumes on icy C-type asteroids (possibly Ceres), and were transferred and incorporated into the H chondrite parent asteroid following the eruption event(s). A unique aspect of these halites is that they contain abundant solid inclusions hosted within the halites alongside the water inclusions. The solid inclusions were suggested to be entrained within the fluid erupted from the cryovolcanic event(s), and were shown to be comprised of abundant organics. Spectrofluorometric study and Raman imaging of the halites have identified macromolecular carbon and aliphatic carbon compounds. In order to investigate the type of organics present in Zag and in particular within the fluid-bearing halites, we studied for the first time the amino acid contents of a selected mineral (halite) phase in a meteorite sample.
Ozone is an important air pollutant at the surface, and the third most important anthropogenic greenhouse gas in the troposphere. Since 1980, anthropogenic emissions of ozone precursors methane, non-methane volatile organic compounds, carbon monoxide and nitrogen oxides (NOx) have shifted from developed to developing regions. Emissions have thereby been redistributed equatorwards, where they are expected to have a stronger effect on the tropospheric ozone burden due to greater convection, reaction rates and NOx sensitivity. Here we use a global chemical transport model to simulate changes in tropospheric ozone concentrations from 1980 to 2010, and to separate the influences of changes in the spatial distribution of global anthropogenic emissions of short-lived pollutants, the magnitude of these emissions, and the global atmospheric methane concentration. We estimate that the increase in ozone burden due to the spatial distribution change slightly exceeds the combined influences of the increased emission magnitude and global methane. Emission increases in Southeast, East and South Asia may be most important for the ozone change, supported by an analysis of statistically significant increases in observed ozone above these regions. The spatial distribution of emissions dominates global tropospheric ozone, suggesting that the future ozone burden will be determined mainly by emissions from low latitudes.
To dramatically reduce the cost and risk of CO2 management systems in future extended missions, we have conducted preliminary studies on the materials and device development for advanced "artificial photosynthesis" reaction systems termed the High Tortuosity PhotoElectroChemical (HTPEC) system. Our Phase I studies have demonstrated that HTPEC operates in much the same way a tree would function, namely directly contacting the cabin air with a photocatalyst in the presence of light and water (as humidity) to immediately conduct the process of CO2 reduction to O2 and useful, "tunable" carbon products. This eliminates many of the inefficiencies associated with current ISS CO2 management systems. We have laid the solid foundation for Phase II work to employ novel and efficient reactor geometries, lighting approaches, 3D manufacturing methods and in-house grown novel catalytic materials.The primary objective of the proposed work is to demonstrate the scientific and engineering foundation for light-activated, compact devices capable of converting CO2 to O2 and mission-relevant carbon compounds. The proposed HTPEC CO2 management system will demonstrate a novel pathway with high efficiency and reliability in a compact, lightweight reactor architecture. The proposed HTPEC air processing concept can be developed in multiple architectures, such as centralized processing as well as "artificial leaves" distributed throughout the cabin that utilize pre-existing cabin ventilation (wind). Additionally, HTPEC can be deployed with spectrally tunable collection channels for selectable product generation. HTPEC employs light as its only energy source to remove and convert waste CO2 using a non-toxic composite catalyst.We have demonstrated in the Phase I studies the production, tunability and robustness of the novel composite catalysts following the preliminary work in the Chen laboratory. Additionally, we have designed, fabricated and tested all components of HTPEC device with active materials, including flow modeling to optimize flow mixing and pressure drop as well as the production of ethylene and other larger hydrocarbons. To best determine how this technology could be implemented, we also performed system integration optimization and trade studies. This includes parameters such as mass, volume, power in relation to selected mission configurations, CO2 delivery methods and light source/delivery approaches.
Missions to search for evidence of life on Mars, including Mars Science Laboratory(MSL)are using drilling systems to get beneath the high oxidized and radiated surface where biomolecules may be preserved. MSL drill holes show that even at shallow depth the subsurface is more reduced and therefor more likely to preserve biosignatures. Analysis of these reduced materials yielded the first detection of organic carbon compounds on Mars[1].While MSL was capable of drilling only 10 cm, the ExoMars mission now planned for a 2022 launch will feature a rover carrying a 2 m drill, motivated by desire to penetrate beneath the irradiated surface. The Atacama Rover Astrobiology Drilling Studies(ARADS)was a PSTAR project that used flight prototype technologies in a highly relevant Mars analog site, together with related scientific studies, to better understand how to best search for life on Mars. ARADS field work was performed in Atacama Chile and featured a rover-mounted 1.2m auguring drill to acquire subsurface samples that were analyzed with flight prototype instruments designed to search for chemical signatures of life.
Satellite retrievals of tropospheric-column formaldehyde (HCHO) and nitrogen dioxide (NO 2 ) are frequently used to investigate the sensitivity of ozone (O 3 ) production to emissions of nitrogen oxides and volatile organic carbon compounds. This study inter-compared the systematic biases and uncertainties in retrievals of NO 2 and HCHO, as well as resulting HCHO–NO 2 ratios (FNRs), from two commonly applied satellite sensors to investigate O 3 production sensitivities (Ozone Monitoring Instrument, OMI, and TROPOspheric Monitoring Instrument, TROPOMI) using airborne remote-sensing data taken during the Long Island Sound Tropospheric Ozone Study 2018 between 25 June and 6 September 2018. Compared to aircraft-based HCHO and NO 2 observations, the accuracy of OMI and TROPOMI were magnitude-dependent with high biases in clean environments and a tendency towards more accurate comparisons to even low biases in moderately polluted to polluted regions. OMI and TROPOMI NO 2 systematic biases were similar in magnitude (normalized median bias, NMB = 5 %–6 %; linear regression slope ≈ 0.5–0.6), with OMI having a high median bias and TROPOMI resulting in small low biases. Campaign-averaged uncertainties in the three satellite retrievals (NASA OMI; Quality Assurance for Essential Climate Variables, QA4ECV OMI; and TROPOMI) of NO 2 were generally similar, with TROPOMI retrievals having slightly less spread in the data compared to OMI. The three satellite products differed more when evaluating HCHO retrievals. Campaign-averaged tropospheric HCHO retrievals all had linear regression slopes ∼0.5 and NMBs of 39 %, 17 %, 13 %, and 23 % for NASA OMI, QA4ECV OMI, and TROPOMI at finer (0.05° x 0.05°) and coarser (0.15° x 0.15°) spatial resolution, respectively. Campaign-averaged uncertainty values (root mean square error, RMSE) in NASA and QA4ECV OMI HCHO retrievals were ~9.0 x 10 15 molecules cm –2 (∼ 50 %–55 % of mean column abundance), and the higher-spatial-resolution retrievals from TROPOMI resulted in RMSE values ∼30 % lower. Spatially averaging TROPOMI tropospheric-column HCHO, along with NO 2 and FNRs, to resolutions similar to the OMI reduced the uncertainty in these retrievals. Systematic biases in OMI and TROPOMI NO 2 and HCHO retrievals tended to cancel out, resulting in all three satellite products comparing well to observed FNRs. However, while satellite-derived FNRs had minimal campaign-averaged median biases, unresolved errors in the indicator species did not cancel out in FNR calculations, resulting in large RMSE values compared to observations. Uncertainties in HCHO retrievals were determined to drive the unresolved biases in FNR retrievals.
Determination of carbon content of lunar samples from Apollo 11 flight
Solid amine compounds were examined as possible absorbents for removal of carbon dioxide in life support systems of type which may be employed in high altitude aircraft, spacecraft, or submarines. Many solid amine compounds release absorbed carbon dioxide when heated in vacuum, therefore, when properly packaged spent amine compounds can be readily regenerated and put back into service.
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Thermodynamic properties of compounds of carbon, hydrogen, nitrogen, oxygen, phosphorus, and sulfur
An experimental program on the catalytic oxidation of iso-octane demonstrated the feasibility of the two-stage combustion system for reducing particulate emissions. With a fuel-rich (phi = 4.8 to 7.8) catalytic combustion preburner as the first stage the combustion process was soot free at reactor outlet temperatures of 1200 K or less. Although soot was not measured directly, its absence was indicated. Reaction products collected at two positions downstream of the catalyst bed were analyzed on a gas chromatograph. Comparison of these products indicated that pyrolysis of the larger molecules continued along the drift tube and that benzene formation was a gas-phase reaction. The effective hydrogen-carbon ratio calculated from the reaction products increased by 20 to 68 percent over the range of equivalence ratios tested. The catalytic partial oxidation process also yielded a large number of smaller-containing molecules. The fraction of fuel carbon in compounds having two or fewer carbon atoms ranged from 30 percent at 1100 K to 80 percent at 1200 K.
Carbon dioxide solid matrix study of carbon trioxide production, IR spectrum and molecular structure
The transport and exchange of material between bodies in the outer solar system is often facilitated by their exposure to ionizing radiation. With this in mind we review the effects of energetic ions, electrons and UV photons on materials present in the outer solar system. We consider radiolysis, photolysis, and sputtering of low temperature solids. Radiolysis and photolysis are the chemistry that follows the bond breaking and ionization produced by incident radiation, producing, e.g., O2 and H2 from irradiated H2O ice. Sputtering is the ejection of molecules by incident radiation. Both processes are particularly effective on ices in the outer solar system. Materials reviewed include H2O ice, sulfur-containing compounds (such as S02 and S8), carbon~contajning compounds (such as CH4), nitrogen-containing compounds (such as NH3 and N2), and mixtures of those compounds. We also review the effects of ionizing radiation on a mixture of N2 and CH4 gases, as appropriate to Titan's upper atmosphere, where radiolysis and photolysis produce complex organic compounds (tholins).
Carbonization of binary mixtures of anthracene biphenyl and penanthrene biphenyl
Introduction: The Ion Neutral Mass Spectrometer (INMS) aboard the Cassini orbiter has obtained the first in situ composition measurements of the neutral densities of molecular nitrogen, methane, argon, and a host of stable carbon-nitrile compounds in its first flyby of Titan. The bulk composition and thermal structure of the moon s upper atmosphere do not appear to be changed since the Voyager flyby in 1979. However, the more sensitive techniques provided by modern in-situ mass spectrometry also give evidence for large-spatial-scale large-amplitude atmospheric waves in the upper atmosphere and for a plethora of stable carbon-nitrile compounds above 1174 km. Furthermore, they allow the first direct measurements of isotopes of nitrogen, carbon, and argon, which provide interesting clues about the evolution of the atmosphere. The atmosphere was first accreted as ammonia and ammonia ices from the Saturn sub-nebula. Subsequent photochemistry likely converted the atmosphere into molecular nitrogen. The early atmosphere was 1.5 to 5 times more substantial and was lost via escape over the intervening 4.5 billion years due to the reduced gravity associated with the relatively small mass of Titan. Carbon in the form of methane has continued to outgas over time from the interior with much of it being deposited in the form of complex hydrocarbons on the surface and some of it also being lost to space.
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.
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.