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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Post-synthetic modulation of the charge distribution in a metal–organic framework for optimal binding of carbon dioxide and sulfur dioxide

Modulation of pore environment is an effective strategy to optimize guest binding in porous materials. We report the post-synthetic modification of the charge distribution in a charged metal–organic framework, MFM-305-CH3, [Al(OH)(L)]Cl, [(H2L)Cl ¼ 3,5-dicarboxy-1-methylpyridinium chloride] and its effect on guest binding. MFM-305-CH3 shows a distribution of cationic (methylpyridinium) and anionic (chloride) centers and can be modified to release free pyridyl N-centres by thermal demethylation of the 1- methylpyridinium moiety to give the neutral isostructural MFM-305. This leads simultaneously to enhanced adsorption capacities and selectivities (two parameters that often change in opposite directions) for CO2 and SO2 in MFM-305. The host–guest binding has been comprehensively investigated by in situ synchrotron X-ray and neutron powder diffraction, inelastic neutron scattering, synchrotron infrared and 2 H NMR spectroscopy and theoretical modelling to reveal the binding domains of CO2 and SO2 in these materials. CO2 and SO2 binding in MFM-305-CH3 is shown to occur via hydrogen bonding to the methyl and aromatic-CH groups, with a long range interaction to chloride for CO2. In MFM-305 the hydroxyl, pyridyl and aromatic C–H groups bind CO2 and SO2 more effectively via hydrogen bonds and dipole interactions. Post-synthetic modification via dealkylation of the as-synthesised metal–organic framework is a powerful route to the synthesis of materials incorporating active polar groups that cannot be prepared directly.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Computationally Guided Design of Multiple Impurities Tolerant Electrode (Final Report)

The current project was based on a combined experimental and computational approach, which can help recommend better cathode materials under multiple impurities conditions. The PI will mainly take in charge of experimental and computational thermodynamics of the selected cathode materials for the SOFC applications under multiple impurities. While the co-PI will run the electrochemical tests of the cathodes recommended and eventually the long-term degradation tests. At the end of the project, a multiple tolerant cathode material based on the combined experimental and computational approach will be recommended and the reliability of the commonly used accelerated testing will be evaluated. It will address multiple impurities poisoning effect of SO2, CO2, Cr and H2O on the LSM, LSCF and LNO cathodes by identifying the formation of the detrimental secondary phases by XRD, SEM and TEM techniques. And further recommended cathode material will be subjected to electrochemical testing and the most promising ones will be applied to long-term tests. The hybrid approach the PI proposed will not only be applied to the design of multiple impurities tolerant cathodes but will also be considered in the future oxygen electrode applications in SOECs or reversible SOCs. This hybrid computational and experimental approach includes four sections: 1) Investigation of single impurity poisoning on LSM, LSCF and LNO cathodes in the presence of SO2, CO2, Cr. In this section, LSM, LSCF cathodes from FuelCellMaterials and LNO cathodes from Sol-Gel synthesis will be heat-treated in the above single impurity. And the formation of the secondary phases as well as the corresponding simulations will be cross compared, which shows good agreement between each other. Meanwhile, the accelerated testing approach will be evaluated in these systems compared with the previous published work to understand the reliability of the approach. 2) Investigation of multiple impurities poisoning on LSM, LSCF and LNO cathodes in the presence of Cr+H2O, SO2+Cr and SO2+Cr+H2O conditions. We have also applied these 3 candidate cathodes under these multiple impurities’ conditions and the long-term degradation mechanism of the multiple impurities will be understood with the help of the combined experimental and computational approach. Meanwhile, the synergistic effect of those impurities will be compared with the individual ones in the same cathode system to further reveal the actual operating conditions. 3) Electrochemical testing and polarization of the recommended cathode. We have demonstrated very low polarization resistance in LSCF (core)-LSM (shell) electrodes using MSD process and analyzed impedance spectra using DRT analysis and confirming that the low polarization resistance in LSM infiltrated MSD cells is due to reduction in polarization resistance associated with O2-adsorption process. 4). Long-term degradation testing. We have developed a versatile MSD-based process to deposit various continuous coatings onto porous scaffolds and established baseline for longer term Cr-impurity testing in future projects.

36 MATERIALS SCIENCE↗
DOE OSTI2022

An approach to sulfate geoengineering with surface emissions of carbonyl sulfide

Sulfate geoengineering (SG) methods based on lower stratospheric tropical injection of sulfur dioxide (SO 2 ) have been widely discussed in recent years, focusing on the direct and indirect effects they would have on the climate system. Here a potential alternative method is discussed, where sulfur emissions are located at the surface or in the troposphere in the form of carbonyl sulfide (COS) gas. There are two time-dependent chemistry–climate model experiments designed from the years 2021 to 2055, assuming a 40 Tg-Syr -1 artificial global flux of COS, which is geographically distributed following the present-day anthropogenic COS surface emissions (SG-COS-SRF) or a 6 Tg-Syr -1 injection of COS in the tropical upper troposphere (SG-COS-TTL). The budget of COS and sulfur species is discussed, as are the effects of both SG-COS strategies on the stratospheric sulfate aerosol optical depth (~Δτ=0.080 in the years 2046–2055), aerosol effective radius (0.46 µm), surface SO x deposition (+8.9 % for SG-COS-SRF; +3.3 % for SG-COS-TTL), and tropopause radiative forcing (RF; ~-1.5 W m –2 in all-sky conditions in both SG-COS experiments). Indirect effects on ozone, methane and stratospheric water vapour are also considered, along with the COS direct contribution. According to our model results, the resulting net RF is –1.3 W m –2 , for SG-COS-SRF, and –1.5 W m –2 , for SG-COS-TTL, and it is comparable to the corresponding RF of –1.7 W m –2 obtained with a sustained injection of 4 Tg-Syr -1 in the tropical lower stratosphere in the form of SO 2 (SG-SO2, which is able to produce a comparable increase of the sulfate aerosol optical depth). Significant changes in the stratospheric ozone response are found in both SG-COS experiments with respect to SG-SO2 (~5 DU versus +1.4 DU globally). According to the model results, the resulting ultraviolet B (UVB) perturbation at the surface accounts for –4.3 % as a global and annual average (versus –2.4 % in the SG-SO2 case), with a springtime Antarctic decrease of –2.7 % (versus a +5.8 % increase in the SG-SO2 experiment). Overall, we find that an increase in COS emissions may be feasible and produce a more latitudinally uniform forcing without the need for the deployment of stratospheric aircraft. However, our assumption that the rate of COS uptake by soils and plants does not vary with increasing COS concentrations will need to be investigated in future work, and more studies are needed on the prolonged exposure effects to higher COS values in humans and ecosystems.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS1977

Quantitative remote measurements of pollutants from stationary sources using Raman lidar

The several advantages of Raman lidar for remote measurements of stationary source emissions were quantitatively evaluated using a calibration tank at a distance of 300 m at night. Measurements of approximately 10 to the 3rd ppm SO2 with a 12% accuracy were demonstrated in an observation time of 15 min using a 1.5-J ruby laser at 30 pulses/min, 6-m range resolution, interference filters, photon counting detection, and a 20-cm receiver. Measurement accuracy was checked by measuring known concentrations of SO2 in the tank, by tuning the interference filters through the SO2 Raman line, and by varying the CO2 concentration to very high levels during the SO2 measurements. Evaluation of the seriousness of induced fluorescence from plume aerosols failed due to the inability to simulate the plume aerosols.

Poultney, S. K.↗
NASA NTRS1981

Thermodynamics and kinetics of the sulfation of porous calcium silicate

The sulfation of plasma sprayed calcium silicate in flowing SO2/air mixtures at 900 and 1000 C was investigated thermogravimetrically. Reaction products were analyzed using electron microprobe and X-ray diffraction analysis techniques, and results were compared with thermodynamic predictions. The percentage, by volume, of SO2 in air was varied between 0.036 and 10 percent. At 10 percent SO2 the weight gain curve displays a concave downward shoulder early in the sulfation process. An analytical model was developed which treats the initial process as one which decays exponentially with increasing time and the subsequent process as one which decays exponentially with increasing weight gain. At lower SO2 levels the initial rate is controlled by the reactant flow rate. At 1100 C and 0.036 percent SO2 there is no reaction, in agreement with thermodynamic predictions.

Miller, R. A.↗
NASA NTRS1982

Erosion of frozen sulfur dioxide by ion bombardment - Applications to Io

The erosion of frozen SO2 due to bombardment by both light and heavy ions (He and F) was measured for bombarding energies of 0.08 to 1.3 MeV/amu. The number of SO2 molecules ejected from the target per incident ion (i.e., the sputtering yield) was 50 for 1.5 MeV He ions and 7300 for 6 MeV F ions. Ion bombardment followed by heating produced an oxygen/sulfur residue which was much more stable against subsequent ion bombardment than the initial frozen SO2. The erosion rate of SO2 frost on Jupiter's moon Io depends strongly on the elemental composition and energy spectra of the magnetospheric ion flux which bombards the surface. The combined effects of ion bombardment and heating which produced residues on the target substrates may also occur on Io from magnetospheric ion bombardment and heating by volcanism. The experimental results compare favorably with a new model of the sputtering process which considers the energy loss of the incident ion to electronic excitation in the target.

Melcher, C. L.↗
NASA NTRS1983

Io's atmosphere - Pressure control by regolith cold trapping and surface venting

A new model for the basal pressure of Io's atmosphere is developed. This model takes into account the previously ignored fact that much of Io's surface has very high porosity, typically about 90 pct. Such porosity allows efficient subsurface cold trapping of atmospheric gases which tends to keep ambient surface pressures very low. SO2 is the only gas identified on Io, and the basal pressures for atmospheric models are usually pegged to local surface temperature via the SO2 vapor pressure equilibrium curve. Near Io's subsolar point the pressure in equilibrium with a surface SO2 frost deposit is about 1/10,000,000th bar. Porous surface models of the type developed invoke equilibrium with the colder, subsurface permafrost (at about 3-cm depth) and yield pressures of about 1/10 to the 12th bar. The subsurface cold trapping model explains many but not all observations relevant to Io's atmosphere. The new subsurface cold trapping model and the earlier surface frost equilibrium model, when taken together, provide lower and upper limits, respectively, on the basal SO2 pressure of Io's atmosphere.

Matson, D. L.↗
NASA NTRS1984

Escape of sulfur and oxygen from Io

Charged particle sputtering is reexamined as a mechanism for escape of sulfur and oxygen from Io. Corotating ions and energetic ions are considered, using the best available determinations of ion fluxes and sputtering yields. It is unclear whether molecular SO2 is the dominant escaping neutral from Io or whether atomic O and S are dominant, but the Voyager detection of SO2(+) in the cold torus implies the presence of molecular SO2 there. Thin atmosphere models encounter serious difficulty in achieving adequate sulfur and oxygen escape rates, but they are not yet ruled out. Ionization and dissociation of SO2 in a sputter corona can dominate direct escape. In thick atmosphere models the neutral escape rates can be much higher, but the oxygen escape rate tends to be too high relative to the sulfur escape rate unless diffusive separation in the atmosphere is limited, perhaps by rapid mixing.

Cheng, A. F.↗
NASA NTRS1989

Estimation of the rate of volcanism on Venus from reaction rate measurements

Laboratory rate data for the reaction between SO2 and calcite to form anhydrite are presented. If this reaction rate represents the SO2 reaction rate on Venus, then all SO2 in the Venusian atmosphere will disappear in 1.9 Myr unless volcanism replenishes the lost SO2. The required volcanism rate, which depends on the sulfur content of the erupted material, is in the range 0.4-11 cu km of magma erupted per year. The Venus surface composition at the Venera 13, 14, and Vega 2 landing sites implies a volcanism rate of about 1 cu km/yr. This geochemically estimated rate can be used to determine if either (or neither) of two discordant geophysically estimated rates is correct. It also suggests that Venus may be less volcanically active than the earth.

Fegley, Bruce, Jr.↗
NASA NTRS1989

Venus volcanism: Rate estimates from laboratory studies of sulfur gas-solid reactions

Thermochemical reactions between sulfur-bearing gases in the atmosphere of Venus and calcium-, iron-, magnesium-, and sulfur-bearing minerals on the surface of Venus are an integral part of a hypothesized cycle of thermochemical and photochemical reactions responsible for the maintenance of the global sulfuric acid cloud cover on Venus. SO2 is continually removed from the Venus atmosphere by reaction with calcium bearing minerals on the planet's surface. The rate of volcanism required to balance SO2 depletion by reactions with calcium bearing minerals on the Venus surface can therefore be deduced from a knowledge of the relevant gas-solid reaction rates combined with reasonable assumptions about the sulfur content of the erupted material (gas + magma). A laboratory program was carried out to measure the rates of reaction between SO2 and possible crustal minerals on Venus. The reaction of CaCO3(calcite) + SO2 yields CaSO4 (anhydrite) + CO was studied. Brief results are given.

Ehlers, K.↗
NASA NTRS1991

Lunar sulfur

Ideas introduced by Vaniman, Pettit and Heiken in their 1988 Uses of Lunar Sulfur are expanded. Particular attention is given to uses of SO2 as a mineral-dressing fluid. Also introduced is the concept of using sulfide-based concrete as an alternative to the sulfur-based concretes proposed by Leonard and Johnson. Sulfur is abundant in high-Ti mare basalts, which range from 0.16 to 0.27 pct. by weight. Terrestrial basalts with 0.15 pct. S are rare. For oxygen recovery, sulfur must be driven off with other volatiles from ilmenite concentrates, before reduction. Troilite (FeS) may be oxidized to magnetite (Fe3O4) and SO2 gas, by burning concentrates in oxygen within a magnetic field, to further oxidize ilmenite before regrinding the magnetic reconcentration. SO2 is liquid at -20 C, the mean temperature underground on the Moon, at a minimum of 0.6 atm pressure. By using liquid SO2 as a mineral dressing fluid, all the techniques of terrestrial mineral separation become available for lunar ores and concentrates. Combination of sulfur and iron in an exothermic reaction, to form iron sulfides, may be used to cement grains of other minerals into an anhydrous iron-sulfide concrete. A sulfur-iron-aggregate mixture may be heated to the ignition temperature of iron with sulfur to make a concrete shape. The best iron, sulfur, and aggregate ratios need to be experimentally established. The iron and sulfur will be by-products of oxygen production from lunar minerals.

Kuck, David L.↗
NASA NTRS1985

Photochemical modelling of Venus clouds using Pioneer Venus data

In order to understand the evolution of water on Venus, we must know the hydrogen escape flux as a function of the tropospheric water abundance. We have studied the connection between total stratospheric hydrogen and exobase hydrogen available to non-thermal escape processes and examined the details of the photochemical trap for water at the Venus cloud tops. Our immediate goal is to calculate the stratospheric water abundance as a function of the tropospheric water abundance. Photochemical production of H2SO4 acts as a sink for both water and sulfur and is capable of keeping stratospheric abundances low if a proper balance exists between the tropospheric abundances. If production of H2SO4 were the only sink for H2O and SO2, the excess in tropospheric abundance of one over the other would reach the stratosphere, and the functional dependence of stratospheric H2O on tropospheric H2O would be linear near the present state. On Venus, however, sulfuric acid condenses at cloud top temperatures and the resulting aerosols can absorb additional water of hydration. This complicates the water budget, increasing the efficiency of sulfur as a sink for water. We have investigated the balance between tropospheric H2O and SO2 and how delicate the balance is. Our major conclusions from this work are the following: (1) H2O and SO2 are mutually limiting if proper tropospheric balance is maintained; (2) changes in tropospheric abundances on the order of 5 ppm are significant; and (3) changes in mixing rates near the cloud tops can cause dramatic changes in SO2 without causing dramatic changes in H2O.

Mcelroy, Michael B.↗
NASA NTRS1995

Stealth Plumes on Io

We suggest that Io's eruptive activity may include a class of previously undetected SO2 geysers. The thermodynamic models for the eruptive plumes discovered by Voyager 'involve low to moderate entropy SO2 eruptions. The resulting plumes are a mixture of solid and gas which emerge from the vent and follow essentially ballistic trajectories. We show that intrusion of silicate magma into buried SO2 deposits can create the required conditions for high entropy eruptions which proceed entirely in the vapor phase. These purely gaseous plumes would have been invisible to Voyager's instruments. Hence, we call them "stealth" plumes. Such eruptions could explain the "patchy" SO2 atmosphere inferred from recent UV and micro-wave spectral observations. The magma intrusion rate required to support the required gas production for these plumes is a negligible fraction of estimated global magma intrusion rates.

Johnson, T. V.↗
NASA NTRS1999

Remote Sensing of Volcanic Clouds: Sulfur Gases and Plume Top Topography

New absorption line parameters for H2S were published and submitted to the Gestion et Etude des Informations Spectroscopiques Atmospheriques (GEISA) and high resolution transmission molecular absorption (HITRAN) databases. These new absorption line parameters will make it possible to use observations from the future Tropospheric Emission Spectrometer (TES) instrument [Earth Observing System (EOS) Chemistry Mission (CHEM) platform] to make more accurate H2S measurements if it observes an H2S-rich volcanic cloud. H2S is the second most abundant volcanic sulfur gas, and like SO2, it also converts to H2SO4 aerosols and can have a climate impact. A paper on the Moderate-resolution Imaging-Spectroradiometer (MODIS) SO2 alert is being revised. New aspects in the revision include verification of the SO2 alert during the EOS mission; factors affecting SO2 detection at thermal infrared, ultraviolet, and microwave wavelengths; radiative transfer tests; more description of satellite instruments; and thermal surface alert installed for MODIS. Her research involves the use of remote sensing to generate maps of plume top altitude. This parameter is important for models of volcanic eruption, aircraft hazards, and climate impact. The topographic shape of the top surface of a volcanic plume can provide information necessary to understand the physics controlling the injection and dispersal of a volcanic plume in the atmosphere. Glaze et al. describe the application of a photoclinometric technique to volcanic plumes. The software algorithm has been improved to account for more general plume and illumination geometries and for easily extracting position information directly from Advanced Very High-Resolution Radiometer (AVHRR) level 1B data. Testing of the algorithm has focused on acquiring AVHRR data for a variety of volcanic plumes in an effort to identify problems with the software as well as model sensitivities. The plumes chosen were erupted from volcanoes at a variety of latitudes, at different times of day, and in different seasons. Another important issue that is being investigated is the importance of plume opacity. A diagram illustrates the method for deriving phi, the angle a wind-blown plume makes with the horizontal, in the direction perpendicular to the remote sensing scan. A figure shows a sample output of the algorithm, a wire mesh map of plume top topography. Additional information is contained in the original.

Crisp, Joy A.↗
NASA NTRS2000

A 3-D Model Analysis of The Impact of Asian Anthropogenic Emissions on the Sulfur Cycle Over the Pacific Ocean

The impact of anthropogenic activities on the SO2 and sulfate aerosol levels over the Pacific region is examined in the Georgia Tech/Goddard Global Ozone Chemistry Aerosol Radiation and Transport (GOCART) model. We focus on the analysis of the data from the NASA Pacific Exploratory Missions (PEM) over the western North Pacific and the tropical Pacific. These missions include PEM-West A in September-October 1991, when the Asian outflow was at the minimum but the upper atmosphere was heavily influenced by the Pinatubo volcanic eruption, and PEM-West B in March-April 1994 when the Asian outflow was at the maximum, and PEM-Tropics A in August-September at a region relatively free of direct anthropogenic influences. Specifically, we will examine the relative importance of anthropogenic, volcanic and biogenic sources to the SO2 and sulfate concentrations over the Pacific, and quantify the processes controlling the distributions of SO2 and sulfate in both the boundary layer and the free troposphere. We will also assess the global impact of SO2 emission in Asia on the sulfate aerosol loading.

Chin, Mian↗
NASA NTRS2003

Distributions of Trace Gases and Aerosols during the Dry Biomass Burning Season in Southern Africa

Vertical profiles in the lower troposphere of temperature, relative humidity, sulfur dioxide (SO2), ozone (O3), condensation nuclei (CN), and carbon monoxide (CO), and horizontal distributions of twenty gaseous and particulate species, are presented for five regions of southern Africa during the dry biomass burning season of 2000. The regions are the semiarid savannas of northeast South Africa and northern Botswana, the savanna-forest mosaic of coastal Mozambique, the humid savanna of southern Zambia, and the desert of western Namibia. The highest average concentrations of carbon dioxide (CO2), CO, methane (CH4), O3, black particulate carbon, and total particulate carbon were in the Botswana and Zambia sectors (388 and 392 ppmv, 369 and 453 ppbv, 1753 and 1758 ppbv, 79 and 88 ppbv, 2.6 and 5.5 micrograms /cubic meter and 13.2 and 14.3 micrograms/cubic meter). This was due to intense biomass burning in Zambia and surrounding regions. The South Africa sector had the highest average concentrations of SO2, sulfate particles, and CN (5.1 ppbv, 8.3 micrograms/cubic meter, and per 6400 cubic meter , respectively), which derived from biomass burning and electric generation plants and mining operations within this sector. Air quality in the Mozambique sector was similar to the neighboring South Africa sector. Over the arid Namibia sector there were polluted layers aloft, in which average SO2, O3, and CO mixing ratios (1.2 ppbv, 76 ppbv, and 3 10 ppbv, respectively) were similar to those measured over the other more polluted sectors. This was due to transport of biomass smoke from regions of widespread savanna burning in southern Angola. Average concentrations over all sectors of CO2 (386 +/- 8 ppmv), CO (261 +/- 81 ppbv), SO2 (2.5 +/- 1.6 ppbv), O3 (64 +/- 13 ppbv), black particulate carbon (2.3 +/- 1.9 microgram/cubic meter), organic particulate carbon (6.2 +/- 5.2 microgram/cubic meter), total particle mass (26.0 +/- 4.7 microgram/cubic meter), and potassium particles (0.4 +- 0.1 microgram/cubic meter) were comparable to those in polluted, urban air. Since the majority of the measurements in this study were obtained in locations well removed from industrial sources of pollution, the high average concentrations of pollutants reflect the effects of widespread biomass burning. On occasions, relatively thin (-0.5 km) layers of remarkably clean air were located at -3 km above mean sea level, sandwiched between heavily polluted air. The data presented here can be used for inputs to and validation of regional and global atmospheric chemical models.

Sinha, Parikhit↗
NASA NTRS2010

Efficient Formation of Stratospheric Aerosol for Climate Engineering by Emission of Condensible Vapor from Aircraft

Recent analysis suggests that the effectiveness of stratospheric aerosol climate engineering through emission of non-condensable vapors such as SO2 is limited because the slow conversion to H2SO4 tends to produce aerosol particles that are too large; SO2 injection may be so inefficient that it is difficult to counteract the radiative forcing due to a CO2 doubling. Here we describe an alternate method in which aerosol is formed rapidly in the plume following injection of H2SO4, a condensable vapor, from an aircraft. This method gives better control of particle size and can produce larger radiative forcing with lower sulfur loadings than SO2 injection. Relative to SO2 injection, it may reduce some of the adverse effects of geoengineering such as radiative heating of the lower stratosphere. This method does not, however, alter the fact that such a geoengineered radiative forcing can, at best, only partially compensate for the climate changes produced by CO2.

Pierce, Jeffrey R.↗
NASA NTRS2012

Thermal Reactions of H2O2 on Icy Satellites and Small Bodies: Descent with Modification?

Magnetospheric radiation drives surface and near-surface chemistry on Europa, but below a few meters Europa's chemistry is hidden from direct observation . As an example, surface radiation chemistry converts H2O and SO2 into H2O2 and (SO4)(sup 2-), respectively, and these species will be transported downward for possible thermally-driven reactions. However, while the infrared spectra and radiation chemistry of H2O2-containing ices are well documented, this molecule's thermally-induced solid-phase chemistry has seldom been studied. Here we report new results on thermal reactions in H2O + H2O2 + SO2 ices at 50 - 130 K. As an example of our results, we find that warming H2O + H2O2 + SO2 ices promotes SO2 oxidation to (SO4)(sup 2-). These results have implications for the survival of H2O2 as it descends, with modification, towards a subsurface ocean on Europa. We suspect that such redox chemistry may explain some of the observations related to the presence and distribution of H2O2 across Europa's surface as well as the lack of H2O2 on Ganymede and Callisto.

Hudson, Reggie L.↗