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NASA NTRS2022

Emission Factors and Evolution of SO2 Measured From Biomass Burning in Wildfires and Agricultural Fires

Fires emit sufficient sulfur to affect local and regional air quality and climate. This study analyzes SO2 emission factors and variability in smoke plumes from US wildfires and agricultural fires, as well as their relationship to sulfate and hydroxymethanesulfonate (HMS) formation. Observed SO2 emission factors for various fuel types show good agreement with the latest reviews of biomass burning emission factors, producing an emission factor range of 0.47–1.2 g SO2 kg^(−1) C. These emission factors vary with geographic location in a way that suggests that deposition of coal burning emissions and application of sulfur-containing fertilizers likely play a role in the larger observed values, which are primarily associated with agricultural burning. A 0-D box model generally reproduces the observed trends of SO2 and total sulfate (inorganic + organic) in aging wildfire plumes. In many cases, modeled HMS is consistent with the observed organosulfur concentrations. However, a comparison of observed organosulfur and modeled HMS suggests that multiple organosulfur compounds are likely responsible for the observations but that the chemistry of these compounds yields similar production and loss rates as that of HMS, resulting in good agreement with the modeled results. We provide suggestions for constraining the organosulfur compounds observed during these flights, and we show that the chemistry of HMS can allow organosulfur to act as an S(IV) reservoir under conditions of pH > 6 and liquid water content >10^(−7) g sm^(−3). This can facilitate long-range transport of sulfur emissions, resulting in increased SO2 and eventually sulfate in transported smoke.

Sulfur↗
NASA NTRS2022

Anoxic photochemical weathering of pyrite on Archean continents

Sulfur is an essential element of life that is assimilated by Earth’s biosphere through the chemical breakdown of pyrite. On the early Earth, pyrite weathering by atmospheric oxygen was severely limited, and low marine sulfate concentrations persisted for much of the Archean eon. Here, we show an anoxic photochemical mechanism of pyrite weathering that could have provided substantial amounts of sulfate to the oceans as continents formed in the late Archean. Pyrite grains suspended in anoxic ferrous iron solutions produced millimolar sulfate concentrations when irradiated with ultraviolet light. The Fe2+(aq) was photooxidized, which, in turn, led to the chemical oxidation of pyritic sulfur. Additional experiments conducted with 2.68 Ga shale demonstrated that photochemically derived ferric iron oxidizes and dissolves sedimentary pyrite during chemical weathering. The results suggest that before the rise of atmospheric oxygen, oxidative pyrite weathering on Archean continents was controlled by the exposure of land to sunlight.

Jihua Hao↗
NASA NTRS2022

Evolved Gas Analyses of Sedimentary Rocks from the Glen Torridon Clay-Bearing Unit, Gale Crater, Mars: Results From the Mars Science Laboratory Sample Analysis at Mars Instrument Suite

Evolved gas analysis (EGA) data from the Sample Analysis at Mars (SAM) instrument suite indicated Fe-rich smectite, carbonate, oxidized organics, Fe/Mg sulfate, and chloride in sedimentary rocks from the Glen Torridon (GT) region of Gale crater that displayed phyllosilicate spectral signatures from orbit. SAM evolved H2O data indicated that the primary phyllosilicate in all GT samples was an Fe-rich dioctahedral smectite (e.g., nontronite) with lesser amounts of a phyllosilicate such as mixed layer talc-serpentine or greenalite-minnesotaite. CO(2) data supported the identification of siderite in several samples, and CO(2) and CO data was also consistent with trace oxidized organic compounds such as oxalate salts. SO(2) data indicated trace and/or amorphous Fe sulfates in all samples and one sample may contain Fe sulfides. SO(2) data points to significant Mg sulfates in two samples, and lesser amounts in several other samples. A lack of evolved O(2) indicated the absence of oxychlorine salts and Mn3+/Mn4+ oxides. The lack of, or very minor, evolved NO revealed absent or very trace nitrate/nitrite salts. HCl data suggested chloride salts in GT samples. Constraints from EGA data on mineralogy and chemistry indicated that the environmental history of GT involved alteration with fluids of variable redox potential, chemistry and pH under a range of fluid-to-rock ratio conditions. Several of the fluid episodes could have provided habitable environmental conditions and carbon would have been available to any past microbes though the lack of significant N could have been a limiting factor for microbial habitability in the GT region.

A. C. McAdam↗
NASA NTRSDate not supplied

Using Mineralogy to Interpret Martian Geologic History

The surface mineralogy of Mars is key to interpreting the planet’s geologic history and constraining when and where Mars may have been habitable to microbial life. Orbital mineralogical data from infrared spectrometers collected over the last two decades have demonstrated that Mars is more than a basaltic planet. Thermal infrared (TIR) emission spectrometers have identified regional variations in igneous minerals, iron oxides, and chloride salts, showing evidence for magmatic evolution and aqueous alteration. Orbital visible/shortwave infrared reflectance spectra provide detailed information about the aqueous history of Mars through the identification of clay minerals, sulfates, carbonates, zeolites, and amorphous materials in ancient ~3-4-billion-year-old terrains. Mineralogical data from rovers allow us to better characterize mineral formation mechanisms by identifying mineral assemblages and placing them in geologic context using outcrop- to grain-scale images. TIR and Mössbauer data from the Mars Exploration Rovers helped identify an ancient dune-interdune playa environment with multiple episodes of groundwater at Meridiani Planum and volcanism-induced hydrothermalism at Gusev crater. The CheMin X-ray diffractometer on the Mars Science Laboratory Curiosity rover in Gale crater is the first fully quantitative mineralogical instrument sent to another planetary surface. CheMin data allow the quantification of minerals and X-ray amorphous materials with a mineral detection limit of <1 wt.% and provide crystal chemistry of major phases from refined unit-cell parameters. CheMin has revealed local mineralogical changes in ancient sedimentary rocks not seen from orbit and helped identify habitable environments. Throughout the 600+ m of vertical stratigraphy studied so far, changes in clay mineralogy, Fe-oxides/oxyhydroxides, sulfates, and carbonates demonstrate a long history of surface and groundwater at Gale crater with variable salinity, pH, Eh, and temperature. Recent CheMin data document a decrease in clay minerals and an increase in sulfate minerals in younger strata that corresponds with a change from fluvio-lacustrine to eolian depositional environments, potentially documenting a change to a drier climate across the planet.

E. B. Rampe↗
NASA NTRSDate not supplied

Acid Alteration of Clay Minerals With Implication for Mars’ Surface Processes

The co-occurrence of phyllosilicates (clays) and sulfate stratigraphies at many locations on Mars are associated with a sharp change in surface conditions from neutral/alkaline pH during the Noachian (4.1-3.7 Ga) which favored the formation of clays to acidic conditions during the Hesperian (3.7-2.9 Ga) which favored the formation of sulfates. Yet, if these two contrasting geosystems were temporarily sequential, it is unknown how the Hesperian acidic conditions altered the previously formed clay units. We performed laboratory batch experiments to fingerprint the diagnostic features produced during interactions of Mars-analog clays and acidic solutions. Two clays, and silicon (IV) oxide, were reacted with solution of either sulfuric acid or filtered natural acid rock drainage (ARD) in plastic bottles. The solutions were adjusted at four pH values (1, 3, 5, and 7) and reacted at 4, 30, and 80°C for 3, 7, and 14 days. At the end of the experiments, the filtered supernatants were analyzed by ICP-MS while the solids were characterized by X-Ray Diffraction; Energy-Dispersive X-Ray Fluorescence analyses; Raman and Short-Wave Infrared spectroscopies and Scanning Electron Microscopy. Results show that the solution chemistry played a key role in the evolution of the clay-solution systems. In H2SO4 systems, the solution pH steadily increased due to partial clay dissolution with no secondary phase formation detected. Contrary, in the ARD systems, the pH decreased due to the ample presence of Fe which controlled both the reactivity of clays by the growth of protecting surface coatings and the solution pH by the precipitation of Fe nanophases; secondary phase detected included goethite, jarosite, gypsum, and siderite. These results indicate that, on Mars, the chemical interaction between clays and acidic solutions was complex and dependent on the solution chemistry. Acidic, sulfate-rich solutions have a high dissolution capacity and could have induced widespread clay disintegration. Notably, if Fe-rich ARD was involved, the clays on Mars could have remained stable during acidic Hesperian period due to formation of protective coatings. Comparison of our results with martian observations will be performed to determine how acidic conditions could potentially affect clays in sedimentary settings, including the Gale crater.

L. Lefticariu↗
NASA NTRS2023

The Emissions Model Intercomparison Project (Emissions-MIP): Quantifying Model Sensitivity to Emission Characteristics

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 SO 2 injection, seasonality of SO 2 and black carbon (BC) particulate emissions, and the assumed fraction of SO 2 emissions that is injected into the atmosphere as particulate phase sulfate (SO 4 ) 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 SO 2 , SO 4 , and BC, with a particularly large relative variation for SO 2 , which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO 2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of −0.35 W m −2 ), SO 2 lifetime over Northern Hemisphere land (maximum difference of 0.8 d), surface SO 2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO 2 at height consistently increased SO 2 and SO 4 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 SO 4 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 SO 4 emission fraction are accurately and consistently represented in global models.

Emissions Model Intercomparison Project↗
NASA NTRSDate not supplied

Observing and Projecting the Lasting Fate of the Hunga Eruption on Atmospheric Water Vapor and Hydroxyl Radical

On 15th Jan. 2022 the submarine Hunga volcano erupted injecting approximately 0.5 Tg of sulfur dioxide into the stratosphere, but more significantly added 150-170 Tg of water vapor to the stratospheric background (over a 10% perturbation) in a matter of several hours. The sulfur dioxide rapidly converted to sulfate aerosol and along with water vapor, was transported around the Southern Hemisphere sub-tropics into midlatitudes and beyond with some transport into the Northern Hemisphere. With a much longer lifetime than sulfate aerosol, measurable water vapor mass anomalies have persisted with only small losses over more than 2 years since the eruption and are likely to continue above background for the remainder of the decade. Satellite measurements from limb and nadir viewing observing instruments provide the information needed to reasonably initialize the Hunga eruption in the Goddard Earth Observing System (GEOS) model using the “replay” framework coupled to the Global Modeling Initiative (GMI) stratosphere-troposphere chemical mechanism for the recent past and have continued the simulations into the future with the free running chemistry climate model (CCM). Using a number of model ensemble members together with the satellite observations, we quantify how the Hunga eruption is perturbing atmospheric composition and climate and projecting the influences to come as the enhanced water vapor continues in the stratosphere with only very slow removal mechanisms. Modeling suggests that the water rich eruption enhanced stratospheric hydroxyl radiacal (OH) and is supported by the speed of the observed conversion of SO2 into sulfate aerosol. These simulations also suggest a significant reduction in tropospheric OH over the mid-high latitude Southern Hemisphere, which has implications for numerous species that are impacted by this radical. The Hunga eruption provides a useful test of chemistry climate models and an opportunity for observation-based process understanding and in making new connections.

Hunga volcano↗
NASA NTRS2024

Inverse Modeling of the Initial Stage of the 1991 Pinatubo Volcanic Cloud Accounting for Radiative Feedback of Volcanic Ash

The way volcanic clouds evolve is very sensitive to the initial spatial 3D distributions of volcanic materials, which are often unknown. In this study, we conducted inverse modeling of the Mt. Pinatubo cloud using TOMS 2D mapping of Aerosol Index and SO 2 loading during the first three post-eruption days to estimate the time-dependent emissions profiles and initial 3D spatial distributions of volcanic ash and SO 2 . We account for aerosol radiative feedback and dynamic lofting of volcanic ash in the inversion calculations for the first time. This resulted in a lower ash injection height (by 1.5 km for ash) than without ash radiative feedback. The Pinatubo eruption ejected ≈77% of fine ash at 12 to 23 km, ≈65% of SO 2 at 18–25 km. In contrast with previous studies, which suggested that all volcanic materials were emitted above the tropopause, a significant fraction of SO 2 (5.1 of 15.5 Mt) and fine ash (37.2 of 66.5 Mt) were ejected in the troposphere, where SO 2 quickly oxidized into sulfate aerosol that is short-lived in the troposphere. This explains the early presence of sulfate aerosols in the plume and why the models can reproduce the observed volcanic aerosols' optical depth (AOD), assuming lower-than-observed SO 2 emission in the stratosphere. Despite the quicker than in observations build-up of sulfate AOD, in a month after the eruption, the evolution of the Pinatubo AOD simulated using the obtained ash and SO 2 initial distributions converges with the available stratospheric aerosol and gas experiment (SAGE) observations.

Pinatubo volcanic ash and SO2 emissions↗
NASA NTRS1999

Crystallization and preliminary X-ray diffraction analysis of restriction endonuclease EcoRII

Crystals of the restriction endonuclease EcoRII have been obtained by the vapor-diffusion technique in the presence of ammonium sulfate or polyethylene glycol. The best crystals were grown with ammonium sulfate as a precipitant. Crystals with dimensions of up to 0.6 x 0. 6 x 0.6 mm have been observed. The crystals diffract to about 4.0 A resolution at a cryo-temperature of 100 K using a rotating-anode X-ray source and a Rigaku R-AXIS IV imaging-plate detector. The space group has been determined to be either I23 or I2(1)3, with unit-cell parameters a = b = c = 160.3 A, alpha = beta = gamma = 90 degrees. The crystal asymmetric unit contains two protein molecules, and self-rotation function analysis shows a pseudo-twofold symmetry relating the two monomers. Attempts to improve the resolution of crystal diffraction and to search for heavy-atom derivatives are under way.

Deoxyribonucleases, Type II Site-Specific/chemistr↗
NASA NTRS2004

In situ evidence for an ancient aqueous environment at Meridiani Planum, Mars

Sedimentary rocks at Eagle crater in Meridiani Planum are composed of fine-grained siliciclastic materials derived from weathering of basaltic rocks, sulfate minerals (including magnesium sulfate and jarosite) that constitute several tens of percent of the rock by weight, and hematite. Cross-stratification observed in rock outcrops indicates eolian and aqueous transport. Diagenetic features include hematite-rich concretions and crystal-mold vugs. We interpret the rocks to be a mixture of chemical and siliciclastic sediments with a complex diagenetic history. The environmental conditions that they record include episodic inundation by shallow surface water, evaporation, and desiccation. The geologic record at Meridiani Planum suggests that conditions were suitable for biological activity for a period of time in martian history.

Water↗
NASA NTRS2004

Development of a thermal gradient cloud condensation nucleus spectrometer

Droplet clouds are one of the most important factors controlling the albedo and hence the temperature of out planet. Anthropogenic aerosols, such as black carbon (BC) organic carbon (OC) and sulfate, have a strong influence on cloud albedo. IPCC (2001) has estimated the global mean forcing from aerosols to be potentially as large as that of green house gases but opposite in sign. However, the uncertainties associated with the indirect aerosol forcing preclude a quantitative estimate. An additional impact on the indirect aerosol forcing, not quantified by IPCC, arises from recently identified chemical factors, for examples, interactions of atmospheric soluble gases, slightly soluble solutes, and organic substance with aerosols, which may influence the formation of cloud droplets. Recent studies suggest that inclusion of chemical effects on aerosol droplets. We plan to conduct several critical laboratory experiments that will reduce the uncertainty associated with indirect radiative forcing due to chemical modification of sulfate and BC aerosols by ambient gases.

organic carbon↗
NASA NTRS2016

Evaluating Secondary Inorganic Aerosols in Three Dimensions

The spatial distribution of aerosols and their chemical composition dictates whether aerosols have a cooling or a warming effect on the climate system. Hence, properly modeling the three-dimensional distribution of aerosols is a crucial step for coherent climate simulations. Since surface measurement networks only give 2-D data, and most satellites supply integrated column information, it is thus important to integrate aircraft measurements in climate model evaluations. In this study, the vertical distribution of secondary inorganic aerosol (i.e., sulfate, ammonium, and nitrate) is evaluated against a collection of 14 AMS flight campaigns and surface measurements from 2000 to 2010 in the USA and Europe. GISS ModelE2 is used with multiple aerosol microphysics (MATRIX, OMA) and thermodynamic (ISORROPIA II, EQSAM) configurations. Our results show that the MATRIX microphysical scheme improves the model performance for sulfate, but that there is a systematic underestimation of ammonium and nitrate over the USA and Europe in all model configurations. In terms of gaseous precursors, nitric acid concentrations are largely underestimated at the surface while overestimated in the higher levels of the model. Heterogeneous reactions on dust surfaces are an important sink for nitric acid, even high in the troposphere. At high altitudes, nitrate formation is calculated to be ammonia limited. The underestimation of ammonium and nitrate in polluted regions is most likely caused by a too simplified treatment of the NH3/NH4(+) partitioning which affects the HNO3/NO3(-) partitioning.

aerosols↗
NASA NTRS2021

Rapid Cloud Removal of Dimethyl Sulfide Oxidation Products Limits SO 2 and Cloud Condensation Nuclei Production in the Marine Atmosphere

Oceans emit large quantities of dimethyl sulfide (DMS) to the marine atmosphere. The oxidation of 60 DMS leads to the formation and growth of cloud condensation nuclei (CCN) with consequent effects on Earth’s radiation balance and climate. Quantitative assessment of the impact of DMS emissions on CCN concentrations necessitates a detailed description of the oxidation of DMS in the presence of existing aerosol particles and clouds. In the unpolluted marine atmosphere, DMS is efficiently oxidized to hydroperoxymethyl thioformate (HPMTF), a stable intermediate in the chemical trajectory towards sulfur dioxide (SO 2 ) and ultimately sulfate aerosol (Veres et al. 2020). Using direct airborne flux measurements, we demonstrate that irreversible loss of HPMTF to clouds in the marine boundary layer determines the HPMTF lifetime (τ HPMTF < 2 hours) and terminates DMS oxidation to SO 2 in the cloudy marine boundary layer. When accounting for HPMTF cloud loss in a global chemical transport model, we show that SO 2 production from DMS is reduced by 35% globally and near surface (0-3km) SO 2 concentrations over the ocean are lowered by 24%. This large, previously unconsidered loss process for volatile sulfur accelerates the timescale for conversion of DMS to sulfate, while limiting new particle formation in the marine atmosphere and changing the dynamics of aerosol growth. This loss process potentially reduces the spatial scale over which DMS emissions contribute to aerosol production and growth and weakens the link between DMS emission and marine CCN production with subsequent implications for cloud formation, radiative forcing, and climate.

dimethyl sulfide↗
NASA NTRS1975

Improved ion exchange membrane

Membrane, made from commercially-available hollow fibers, is used in reverse osmosis, or dialysis. Fiber has skin layers which pass only small molecules. Macromolecules cannot penetrate skin. Fibers can also be used to remove other undesirable anions, such as phosphate, sulfate, carbonate, and uranium in form of uranium-sulfate complex.

Rembaum, A.↗
NASA NTRS1975

Electrochemical generation of oxygen. 1: The effects of anions and cations on hydrogen chemisorption and anodic oxide film formation on platinum electrode. 2: The effects of anions and cations on oxygen generation on platinum electrode

The effects were studied of anions and cations on hydrogen chemisorption and anodic oxide film formation on Pt by linear sweep voltammetry, and on oxygen generation on Pt by potentiostatic overpotential measurement. The hydrogen chemisorption and anodic oxide film formation regions are greatly influenced by anion adsorption. In acids, the strongly bound hydrogen occurs at more cathodic potential when chloride and sulfate are present. Sulfate affects the initial phase of oxide film formation by produced fine structure while chloride retards the oxide-film formation. In alkaline solutions, both strongly and weakly bound hydrogen are influenced by iodide, cyanide, and barium and calcium cations. These ions also influence the oxide film formation. Factors considered to explain these effects are discussed. The Tafel slope for oxygen generation was found to be independent on the oxide thickness and the presence of cations or anions. The catalytic activity indicated by the exchange current density was observed decreasing with increasing oxide layer thickness, only a minor dependence on the addition of certain cations and anions was found.

Huang, C. J.↗
NASA NTRS1976

A global average model of atmospheric aerosols for radiative transfer calculations

A global average model is proposed for the size distribution, chemical composition, and optical thickness of stratospheric and tropospheric aerosols. This aerosol model is designed to specify the input parameters to global average radiative transfer calculations which assume the atmosphere is horizontally homogeneous. The model subdivides the atmosphere at multiples of 3 km, where the surface layer extends from the ground to 3 km, the upper troposphere from 3 to 12 km, and the stratosphere from 12 to 45 km. A list of assumptions made in construction of the model is presented and discussed along with major model uncertainties. The stratospheric aerosol is modeled as a liquid mixture of 75% H2SO4 and 25% H2O, while the tropospheric aerosol consists of 60% sulfate and 40% soil particles above 3 km and of 50% sulfate, 35% soil particles, and 15% sea salt below 3 km. Implications and consistency of the model are discussed.

Toon, O. B.↗
NASA NTRS1977

Low-temperature coal desulfurization

Economical, low-temperature chlorinolysis converts sulfur to water-soluble sulfates. Sulfates are removed by washing. Subsequent steps dry coal and remove chlorine. Chlorine and solvents can be reused.

Ganguli, P. S.↗
NASA NTRS1977

Evaluation of a new antinauseant drug for the prevention of motion sickness

The new drug, AHR 5645B, together with other drugs was evaluated in tests, conducted with eight male subjects, concerning its ability to prevent motion sickness. It was found that AHR 5645B, used in doses of 20, 50, and 100 mg, was not efficacious in preventing experimental motion sickness. A combination of 50 mg meclizine and 25 mg ephedrine sulfate produced the best results. Favorable results were also obtained with a combination of 12.5 mg promethazine hydrochloride and 12.5 mg ephedrine sulfate. The findings in the reported experiment point to the difficulty of identifying a highly efficacious antimotion sickness drug for everyone.

Graybiel, A.↗