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At least 307 records · Page 17
All sourcesNASA NTRSDOE OSTI
NASA NTRS1997

Global Troposphere Experiment Project

For the Global Troposphere Experiment project Pacific Exploratory Measurements West B (PEM West B), we made determinations of sulfur dioxide (SO2) and dimethyl sulfide (DMS) using gas chromatography-mass spectrometry with isotopically labelled internal standards. This technique provides measurements with precision of 1 part-per-trillion by volume below 20 pptv and 1% above 20 pptv. Measurement of DMS and SO2 were performed with a time cycle of 5-6 minutes with intermittent zero checks. The detection limits were about 1 pptv for SO2 and 2 pptv for DMS. Over 700 measurements of each compound were made in flight. Volcanic impacts on the upper troposphere were again found as a result of deep convection in the tropics. Extensive emission of SO2 from the Pacific Rim land masses were primarily observed in the lower well-mixed part of the boundary layer but also in the upper part of the boundary layer. Analyses of the SO2 data with aerosol sulfate, beryllium-7, and lead-210 indicated that SO2, contributed to half or more of the observed total oxidized sulfur (SO2 plus aerosol sulfate) in free tropospheric air. Cloud processing and rain appeared to be responsible for lower SO2 levels between 3 and 8.5 km than above or below this region. During both phases of PEM-West, dimethyl sulfide did not appear to be a major source of sulfur dioxide in the upper free troposphere over the western Pacific Ocean. In 1991 the sources Of SO2 at high altitude appeared to be both anthropogenic and volcanic with an estimated 1% being solely from DMS. The primary difference for the increase in the DMS source was the very low concentration of SO2 at high altitude. In the midlatitude region near the Asian land masses, DMS in the mixed layer was lower than in the tropical region of the western Pacific. Convective cloud systems near volcanoes in the tropical convergence in the western Pacific troposphere were a major source of SO2 at high altitudes during PEM-West B. High levels of SO2 were observed in several instances with large number concentrations of ultrafine CN above 9 km in the tropical convergence zone. Conversion of SO2, by OH to SO3 and subsequently to sulfuric acid may have been enhanced by lightning-produced NO levels exceeding 1 part per billion. Coupling of strong convection and volcanic sources of SO2 apparently is an important source of new particle formation at high altitude in the tropical convergence zone.

Bandy, Alan R.↗
DOE OSTI2013

Effect of SO 2 on oxidation of metallic materials in CO 2 /H 2 O-rich gases relevant to oxyfuel environments: Effect of SO 2 on oxidation of metallic materials

In an oxyfuel plant, heat exchanging metallic components will be exposed to a flue gas that contains substantially higher contents of CO2, water vapor, and SO2 than conventionalflue gases. In the present study, the oxidation behavior of the martensitic steel P92 was studied in CO2-and/or H2O-rich gas mixtures with and without addition of SO2. For this purpose, the corrosion of P92 at 550 8C up to 1000 h in Ar–H2O–SO2, Ar–CO2–SO2, Ar–CO2–O2–SO2 and simulated oxyfuel gas (Ar–CO2–H2O–O2–SO2) was compared with the behavior in selected SO2-free gases. The oxidation kinetics were estimated by a number of methods such as optical microscopy, scanning electron microscopy with energy and wave length dispersive X-ray analysis, glow discharge optical emission spectroscopy, X-ray diffraction as well as transmission electron microscopy. The experimental results revealed that the effect of SO2 addition on the materials behavior substantially differed, depending on the prevailing base gas atmosphere. The various types of corrosion attack affected by SO2 could not be explained by solely comparing equilibrium activities of the gas atmospheres with thermodynamic stabilities of possible corrosion products. The results were found to be strongly affected by relative rates of reactions of the various gas species occurring within the frequently porous corrosion scales as well as at the scale/gas-and scale/alloy interfaces.Whereas SO2 addition to Ar–CO2 resulted in formation of an external mixed oxide/sulflde layer, the presence of SO2 in oxyfuel gas and in Ar–H2O–SO2 resulted in Fe-sulflde formation near the interface between inner and outer oxide layer as well as Cr-sulflde formation in the alloy. In the latter gases, the presence of SO2 seemed to have no dramatic effect on oxide scale growth rates.

36 MATERIALS SCIENCE↗
DOE OSTI2023

The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics

Abstract. Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth–atmosphere system, alter the formation of clouds and precipitation, and have a substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and black carbon (BC) particulate emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as particulate phase sulfate (SO4) in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m−2), SO2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to ensure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models.

54 ENVIRONMENTAL SCIENCES↗
NASA NTRS2016

Reactions Involving Calcium and Magnesium Sulfates as Potential Sources of Sulfur Dioxide During MSL SAM Evolved Gas Analyses

The Sample Analysis at Mars (SAM) and Chemistry and Mineralogy (CheMin) instruments on the Mars Science Laboratory (MSL) have analyzed several subsamples of <150 micron fines from ten sites at Gale Crater. Three were in Yellowknife Bay: the Rocknest aeolian bedform (RN) and drilled Sheepbed mudstone from sites John Klein (JK) and Cumberland (CB). One was drilled from the Windjana (WJ) site on a sandstone of the Kimberly formation. Four were drilled from sites Confidence Hills (CH), Mojave (MJ), Telegraph Peak (TP) and Buckskin (BK) of the Murray Formation at the base of Mt. Sharp. Two were drilled from sandstones of the Stimson formation targeting relatively unaltered (Big Sky, BY) and then altered (Greenhorn, GH) material associated with a light colored fracture zone. CheMin analyses provided quantitative sample mineralogy. SAM's evolved gas analysis mass spectrometry (EGA-MS) detected H2O, CO2, O2, H2, SO2, H2S, HCl, NO, and other trace gases. This contribution will focus on evolved SO2. All samples evolved SO2 above 500 C. The shapes of the SO2 evolution traces with temperature vary between samples but most have at least two "peaks' within the wide high temperature evolution, from approx. 500-700 and approx. 700-860 C (Fig. 1). In many cases, the only sulfur minerals detected with CheMin were Ca sulfates (e.g., RN and GH), which should thermally decompose at temperatures above those obtainable by SAM (>860 C). Sulfides or Fe sulfates were detected by CheMin (e.g., CB, MJ, BK) and could contribute to the high temperature SO2 evolution, but in most cases they are not present in enough abundance to account for all of the SO2. This additional SO2 could be largely associated with x-ray amorphous material, which comprises a significant portion of all samples. It can also be attributed to trace S phases present below the CheMin detection limit, or to reactions which lower the temperatures of SO2 evolution from sulfates that are typically expected to thermally decompose at temperatures outside the SAM temperature range (e.g., Ca and Mg sulfates). Here we discuss the results of SAM-like laboratory analyses targeted at understanding this last possibility, focused on understanding if reactions of HCl or an HCl evolving phase (oxychlorine phases, chlorides, etc.) and Ca and Mg sulfates can result in SO2 evolution in the SAM temperature range.

McAdam, A. C.↗
NASA NTRS2022

Trends in sulfur dioxide over the Indian subcontinent during 2003–2019

Sulfur dioxide (SO2) and its oxidation products profoundly impact the air quality and climate. In recent decades, contrasting SO2 trends have been observed over different regions of the globe due to urbanization, energy generation and control measures. In this study, we have investigated the SO2 trends over the rapidly developing Indian subcontinent using model reanalysis, satellite data, and emission inventories during 2003–2019 period. Copernicus Atmosphere Monitoring Service (CAMS) reanalysis shows rapid SO2 growth up to 0.4 ppbv/yr during 2003–2009, particularly significant over the Indo-Gangetic Plain (IGP) and eastern India. However, the growth becomes slower after 2010 and is followed by a stabilization or slight reduction. The CAMS results agree with the satellite-based observations, however, the model underestimates enhancements over eastern India. The analysis of inventory datasets also suggests slower growths in SO2 emissions and coal-fired electricity generation in recent years. Besides the changes in regional emissions, the enhancements in water vapor and OH radical coinciding with SO2 stabilization indicate strengthening of the sink processes. Model simulation (Modern-Era Retrospective analysis for Research and Applications version 2―MERRA-2) with constant emissions shows reduction in SO2 which confirms the stronger chemical losses. Overall, the SO2 trends over the Indian subcontinent are found to be a manifestation of the combined effects of the regional emission change and chemistry. Our findings highlight the need for studies to assess the impacts of changing SO2 trends in India on the regional and global climate.

Lakhima Chutia↗
NASA NTRS2008

Sulfur Dioxide and the Production of Sulfuric Acid on Present-Day and Early Mars: Implications for the Lack of Detected Carbonates on the Surface

In the early history of Mars, volcanic activity associated with the formation of the Tharsis ridge produced a very large amount of atmospheric SO2--on the order of a bar of atmospheric SO2. In the present-day atmosphere of Mars, the lifetime of SO2 is relatively short with a lifetime of less than a day. The short lifetime of SO2 in the present Mars atmosphere makes the production of significant levels of H2SO4 very difficult since the SO2 may be destroyed by various chemical and photochemical processes before the SO2 can be converted to H2SO4. However, photochemical calculations performed and described here, indicate that enhanced atmospheric levels of CO2 in the early atmosphere of Mars resulted in a significantly enhanced atmospheric lifetime for SO2 up to several years. With a significantly enhanced atmospheric lifetime, SO2 could readily form large amounts of H2SO4, which precipitated out of the atmosphere in the form of droplets. The precipitated H2SO4 then reacted with potential surface carbonates, destroying the carbonates and resulting in the abundant and widespread distribution of sulfates on the surface of Mars as detected by recent Mars missions.

Levine, Joel S.↗
NASA NTRS2010

The Other Chemistry of the Jovian Icy Satellites - Low Energy and Sulfurous

Spectra of Jupiter's icy satellites reveal surfaces dominated by H2O-ice with minor amounts of SO2 and other materials. The co-existence of H2O and SO2 in surfaces exposed to jovian magnetospheric radiation suggests that sulfuric acid (H2SO4) also could be present. This was noted by Carlson et al. (1999), who supported this suggestion with assignments of near-IR bands in Europa spectra to hydrated H2SO4. Laboratory experiments since have demonstrated radiolytically-driven syntheses in S- and SO2-containing H2O-Ices (Carlson et al., 2002; Moore et al., 2006). In the Cosmic Ice Laboratory, we recently have investigated the thermal chemistry of SO2 trapped in H2O-ice. IR spectra of H2O + SO2 mixtures recorded at 10 to 230 K were used to follow low-temperature reactions in the absence of radiation effects. No SO2 reactions were found at 10 K, but warming to more-relevant Europa temperatures produced both HSO3(-) and S2O5(2-). Added NH3 shifted the product composition toward SO3(2-) and away from the other ions. We find that H2O and SO2 react to produce sulfur oxyanions, such as bisulfite, that as much as 30% of the SO2 can be consumed through this reaction, and that the products remain in the ice when the temperature is lowered, indicating that these reactions are irreversible. Our results suggest that thermally-induced reactions can alter the chemistry at and below the surfaces of the icy satellites in the jovian system.

Hudson, Reggie L.↗
NASA NTRS2021

Impact of Regional Northern Hemisphere Mid-latitude Anthropogenic Sulfur Dioxide Emissions on Local and Remote Tropospheric Oxidants

The unintended consequences of reductions in regional anthropogenic sulfur dioxide (SO2) emissions implemented to protect human health are poorly understood. SO2 decreases began in the 1970s in the US and Europe and are expected to continue into the future, while recent emissions decreases in China are also projected to continue. In addition to the well-documented climate effects (warming) from reducing aerosols, tropospheric oxidation is impacted via aerosol modification of photolysis rates and radical sinks. Impacts on the hydroxyl radical and other trace constituents directly affect climate and air quality metrics such as surface ozone levels. We use the Geophysical Fluid Dynamics Laboratory Atmospheric Model version 3 nudged towards National Centers for Environmental Prediction (NCEP) reanalysis wind velocities to estimate the impact of SO2 emissions from the US, Europe, and China by differencing a control simulation with an otherwise identical simulation in which 2015 anthropogenic SO2 emissions are set to zero over one of the regions. Springtime sulfate aerosol changes occur both locally to the emission region and also throughout the Northern Hemispheric troposphere, including remote oceanic regions and the Arctic. Hydroperoxy (HO2) radicals are directly removed via heterogeneous chemistry on aerosol surfaces, including sulfate, in the model, and we find that sulfate aerosol produced by SO2 emissions from the three individual northern mid-latitude regions strongly reduces both HO2 and hydroxyl (OH) by up to 10 % year-round throughout most of the troposphere north of 30∘ N latitude. Regional SO2 emissions significantly increase nitrogen oxides (NOx) by about 5 %–8 % throughout most of the free troposphere in the Northern Hemisphere by increasing the NOx lifetime as the heterogeneous sink of HO2 on sulfate aerosol declines. Despite the NOx increases, tropospheric ozone decreases at northern mid-latitudes by 1 %–4 % zonally averaged and by up to 5 ppbv in summertime surface air over China, where the decreases in HO2 and OH suppress O3 production. Since 2015 anthropogenic SO2 emissions in China exceed those in the US or Europe, the oxidative response is greatest for the China perturbation simulation. Chemical effects of aerosols on oxidation (reactive uptake) dominate over radiative effects (photolysis rates), the latter of which are only statistically significant locally for the large perturbation over China. We find that the SO2 emissions decrease in China, which has yet to be fully realized, will have the largest impact on oxidants and related species in the Northern Hemisphere free troposphere compared to future decreases in Europe or the US. Our results bolster previous calls for a multipollutant strategy for air pollution mitigation to avoid the unintended consequence of aerosol removal leading to surface ozone increases that offset or mask surface ozone gains achieved by regulation of other pollutants, especially in countries where current usage of high-sulfur emitting fuels may be phased out in the future.

anthropogenic sulfur dioxide emissions↗
NASA NTRS2014

A Decade of Volcanic Observations from Aura and the A-Train

Aura observations have made many seminal contributions to volcanology. Prior to the Aura launch, satellite observations of volcanic degassing (e.g., from TOMS) were mostly restricted to large eruptions. However, the vast majority of volcanic gases are released during quiescent 'passive' degassing between eruptions. The improved sensitivity of Aura OMI permitted the first daily, space-borne measurements of passive volcanic SO2 degassing, providing improved constraints on the source locations and magnitude of global SO2 emissions for input to atmospheric chemistry and climate models. As a result of this unique sensitivity to volcanic activity, OMI data were also the first satellite SO2 measurements to be routinely used for volcano monitoring at several volcano observatories worldwide. Furthermore, the Aura OMI SO2 data also offer unprecedented sensitivity to volcanic clouds in the UTLS, elucidating the transport, fate and lifetime of volcanic SO2 and providing critical input to aviation hazard mitigation efforts. Another major advance has been the improved vertical resolution of volcanic clouds made possible by synergy between Aura and other A-Train instruments (e.g., AIRS, CALIPSO, CloudSat), advanced UV SO2 altitude retrievals, and inverse trajectory modeling of detailed SO2 cloud maps. This altitude information is crucial for climate models and aviation hazards. We will review some of the highlights of a decade of Aura observations of volcanic activity and look ahead to the future of volcanic observations from space.

Aura↗
DOE OSTI2014

SO 2 Phototriggered Crystalline Nanomechanical Transduction of Aromatic Rotors in Tosylates: Rationalization via Photocrystallography of [Ru(NH 3 ) 4 SO 2 X]tosylate 2 (X = pyridine, 3-Cl-pyridine, 4-Cl-pyridine)

Thermally-reversible solid-state linkage SO2 photoisomers of three complexes in the [Ru(NH3)4SO2X]tosylate2 family are captured in their metastable states using photocrystallography, where X = pyridine (1), 3-Cl-pyridine (2) and 4-Cl-pyridine (3). This photoisomerism only exists in the single-crystal form; accordingly, the nature of the crystalline environment surrounding the photo-active species controls its properties. In particular, the structural role of the tosylate anion needs to be understood against possible chemical influences due to varying the trans ligand, X. The photo-excited geometries, photoconversion levels and thermal stabilities of the photoisomers that form in 1-3 are therefore studied. 1 and 2 yield two photo-isomers at 100 K: the O-bound end-on n1-SO2 Page 1 of 32 ACS Paragon Plus Environment The Journal of Physical Chemistry (MS1) configuration and the side-bound n2-SO2 (MS2), while 3 only exhibits the more thermally stable MS2 geometry. The decay kinetics of the MS2 geometry for 1-3 demonstrate that the greater the free volume of the GS SO2 ligand for a given counterion, the greater the MS2 thermal stability. Furthermore, a rationalization is sought for the SO2 phototriggered molecular rotation of the phenyl ring in the tosylate anion; this is selectively observed in 2, manifesting as nanomechanical molecular transduction. This molecular transduction was not observed in 1, despite the presence of the MS1 geometry due to the close intermolecular interactions between the MS1 SO2 and the neighbouring tosylate ion. The decay of this anionic molecular rotor in 2, however, follows a non-traditional decay pathway, as determined by time-resolved crystallographic analysis; this contrasts with the well-behaved first-order kinetic decay of its MS1 SO2 phototrigger.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1979

Sulfur dioxide in the Venus atmosphere - Distribution and implications

The Pioneer Venus Orbiter ultraviolet spectrometer sees variable disk brightness features similar to the well-known 'UV markings' seen at longer wavelengths. The bright features are consistent with a homogeneous cloud of H2SO4 aerosols. The darker features show the presence of a broad-band absorber, which is at some depth in the cloud layer. Additional contrast arises from SO2 absorption. The observed strength of the SO2 absorption as a function of wavelength rules out a uniform mixing ratio for the SO2. The data are well fitted by an inhomogeneous light scattering model in which the SO2 scale height is one-fifth of the CO2 scale height, and the mixing ratio of SO2 at 40 mb is 10 to the -7th. A model of the oxidation of sulfur dioxide in the upper cloud reproduces the observed vertical distribution of SO2 and indicates that SO2 alone is sufficient to produce the observed amount of H2SO4 in this region.

Esposito, L. W.↗
NASA NTRS1982

Io's surface - Its phase composition and influence on Io's atmosphere and Jupiter's magnetosphere

The evidence and interpretations pertaining to the surface phase composition of Io and the mechanisms by which Io's surface influences its atmosphere are discussed. The mechanism by which Io's surface and/or atmosphere supplies neutral and ionic species to the region around the satellite and ultimately to the Jovian magnetosphere is also discussed. A model is suggested in which the global SO2 gas abundance is primarily controlled by buffering in the brightest, coldest regions. The net SO2 flux across the disk is limited by regional cold trapping on high albedo regions and possibly by the resistance of a tenuous non-SO2 residual atmosphere. The continuing migration of SO2 toward cooler regions and those lacking SO2 sources is opposed by SO2 destruction and planetary ejection processes, including sputtering, thus preventing buildup of thick, ubiquitous SO2 coverage.

Fanale, F. P.↗
NASA NTRS1984

The photochemistry of a remote marine stratiform cloud

The coupled gas- and aqueous-phase photochemistry of a stratiform cloud in a remote region of the marine atmosphere is investigated with a time-dependent box model. Both scavenging of ambient acidic aerosols and gases as well as aqueous-phase chemical reactions within droplets are found to be important sources of acidity to cloud water and can lead to pH levels in cloud water in the remote marine atmosphere well below 5.6. The major sources of acidity via aqueous-phase chemical reactions are the generation of sulfuric acid from dissolved SO2 and the generation of formic acid from dissolved formaldehyde. In both cases, aqueous-phase free radicals can play a significant role either directly by oxidizing dissolved SO2 and HCHO or indirectly by producing the aqueous-phase oxidant H2O2. The rate of SO2 conversion to sulfuric acid is sensitive to a variety of parameters including the accommodation or sticking coefficient for SO2, H2O2, HO2, and OH, the liquid water content, and the ambient levels of SO2, HNO3, and other acidic or basic gases. Because high levels of SO2 tend to deplete cloud water of H2O3, the possibility exists that the pH of precipitation in polluted regions will respond nonlinearly to reduced SO2 emissions.

Chameides, W. L.↗