Reactions of SO2 on hydrated cement particle system for atmospheric pollution reduction: A DRIFTS and XANES study
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Ramakrishnan, Girish↗
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Molecular interactions of SO2 with carbonate minerals under co-sequestration conditions: a combined experimental and theoretical study
We present a combined experimental and theoretical study investigating the reactivity between selected and morphologically important surfaces of carbonate minerals with supercritical CO2 with co-existing H2O and SO2. Trace amounts of SO2 cause formation of CaSO3 in the form of hannebachite in the initial stages of SO2 adsorption and transformation. Atomistic simulations of these initial steps indicate a somewhat catalytic activity of water, which is enhanced by the presence of Magnesium atoms in the mineral surface. Under co-sequestration conditions, traces of water are not likely to cause carbonate dissolution, however the presence of SO2 greatly stabilizes the sulfite product.
58 GEOSCIENCES↗
Ionic-Based Electrochemical Gas Sensors for Low-Cost, High-Sensitivity SO2 Detection
Sulfur dioxide (SO2) is a toxic gas associated with adverse health and environmental effects that necessitate reliable monitoring techniques. Here, we report the development of an all-solid-state electrochemical sensor utilizing a lithium borate (Li3BO3) solid electrolyte capable of subppm of SO2 detection. While subppm of SO2 sensing has been previously demonstrated in other solid-state electrolyte systems─such as stabilized zirconia, natrium super ionic conductors (NASICON) under mixed-potential conditions─here we establish Li3BO3 as an alternative solid electrolyte enabling equilibrium potentiometric sensing in an all-solid architecture. This sensor demonstrates a detection limit of at least 0.25 ppm, surpassing the human-olfactory threshold and meeting the rigorous requirements for industrial and personal monitoring applications. The sensing mechanism relies on the formation of Li2SO4 on the electrode surface, as evidenced by multimodal characterization techniques, including Raman spectroscopy, scanning electron microscopy (SEM), and scanning transmission electron microscopy (STEM). The strong linear correlation between the open-circuit potential (OCV) and the logarithm of SO2 concentration between 0.25 and 2 ppm indicates that the response is Nernstian in nature.
Lagunas, Francisco (ORCID:000000026377683X)↗
Photochemistry of SO2 in Venus' upper cloud layers
The photochemical and transport processes that occur in the Venusian atmosphere in and above the upper cloud region are characterized with attention to the correlation with the Pioneer Venus spectrometer results for the cloud top SO2 distribution. The model uses upward-flowing SO2 and H2O to replace the sulfur and hydrogen lost through the lower boundary by the settling of sulfuric acid aerosols. Oxygen for the oxidation of SO2 to SO3 prior to hydration to H2SO4 is supplied by the photolysis of CO2. A model with SO2 as the major sulfur-bearing gas is consistent with the Pioneer data.
Winick, J. R.↗
The microwave absorption of SO2 in the Venus atmosphere
Sulfur dioxide has a strong and complex rotational spectrum in the microwave and far infrared regions. The microwave absorption due to SO2 in a CO2 mixture is calculated for conditions applicable to the Venus atmosphere. It is shown that at the concentrations detected by Pioneer-Venus in situ measurements, SO2 may be expected to contribute significantly to the microwave opacity of the Venus atmosphere. In particular, SO2 might provide the major source of opacity in the atmospheric region immediately below the main sulfuric acid cloud deck. The spectrum is largely nonresonant at the pressures where SO2 is expected to occur, however.
Janssen, M. A.↗
Photochemistry of SO2 in the atmosphere of Io and implications on atmospheric escape
Photochemical models of Io's atmosphere are presented with the assumption that SO2 is the major gas and that the SO2 surface pressure is controlled by vapor-pressure equilibrium at the surface. Photolysis of SO2 leads to efficient production of SO, O2, S, and O. Of these products, O and S are likely to be the dominant constituents in the upper atmosphere, and the atmospheric escape is expected to be in atomic form. Nonthermal escape processes are necessary to populate the plasma torus. SO2 surface densities greater than 100-billion per cu cm are needed on the dayside to supply the required amounts of S and O to maintain the torus. Surface chemistry presents an interesting possibility, namely, the conversion of O to O2, in which case O2 will be the dominant constituent throughout the nightside and over the polar caps with a surface O2 density of 10-billion per cu cm.
Kumar, S.↗
Laboratory studies of charged particle erosion of SO2 ice and applications to the frosts of Io
The removal and/or redistribution of SO2 frosts on the surface of the first Galilean satellite, Io, can occur through the erosion of these frosts by the magnetosphere particle environment of the satellite. The energy, species, and temperature dependence of the erosion rates of SO2 ice films by charged particles have been studied in laboratory experiments. Rutherford backscattering and thin film techniques are used in the experiments. The ice temperature is varied between about 10 K and the sublimation temperature. The erosion rates are found to have a temperature-independent and a temperature-dependent regime and to be much greater, for 10-2000 keV ions, than those predicted by the usual sputtering process. The laboratory results are used together with measured magnetosphere particle fluxes in the vicinity of Io to estimate the erosion rates of SO2 ice films from the satellite and implications therefrom on an SO2 atmosphere on Io.
Lanzerotti, L. J.↗
An interpretation of the near-ultraviolet absorption spectrum of SO2 - Implications for Venus, Io, and laboratory measurements
Line characteristics of remotely sensed SO2 spectra near the UV are discussed, noting the implications for the interpretation of data gathered by the IUE of Io and ground-based and Pioneer spectra of Venus. It is shown that the ratio of mean line spacing to linewidth is greater than unity, and that fully resolved lines have features consistent with concepts of temperature and pressure broadening. The application of Beer's approximation for the absorption spectra of Venus and Io atmospheres is found to be incorrect. Further, the spectroscopic limit on the SO2 line data from Io observations by the IUE are interpreted as establishing a lower bound on the SO2 in the Io atmosphere. A greater concentration of SO2 in vapor equilibrium may be present in the lower atmosphere. Laboratory measurements to resolve the uncertainties regarding the UV spectroscopic data from Io and Venus are suggested.
Belton, M. J. S.↗
Io's 4-micron band and the role of adsorbed SO2
The role of adsorbed SO2 on Io's surface particles in producing the observed spectral absorption band near 4 microns in Io's reflectance spectrum is explored. Calculations show that a modest 50 percent monolayer coating of adsorbed So2 molecules on submicron grains of sulfur or alkali sulfide, assumed to make up Io's uppermost optical surface ('radialith'), will result in a nu 1 + nu 3 absorption band near 4 microns with depth about 30 percent below the adjacent continuum, consistent with the observed strength of the Io band. The precise wavelength position of the nu 1 + nu 3 band of SO2 in different phase states such as frost, ice, adsorbate, and gas are summarized from the experimental literature and compared with the available telescopic measurements of the Io band position. The results suggest that the 4-micron band in Io's full disk spectrum can best be explained by the presence on Io's surface of widespread SO2 in the form of adsorbate rather than ice or frost.
Nash, D. B.↗
Mass spectrometric determination of partial and total electron impact ionization cross sections of SO2 from threshold up to 200 eV
The partial and total ionization cross section for the formation of O(+), S(+), SO(+) and SO2(+) from the impact ionization of SO2 are reported, extending the electron impact energies to 200 eV. The relative flow technique is used to determine the cross section values. The threshold potentials for the products are 23.5 eV for O(+), 16.5 eV for S(+), 16.5 eV for SO(+), and 12.5 eV for SO2(+). Good agreement with the literature is found for SO(+) and SO2(+).
Orient, O. J.↗
Study of the sulphur-containing molecules in the EUV region. IV - The dissociation processes of SO2 in the 760 A region
The fluoresence throughout the VUV and violet regions has been observed from photoexcitation of SO2, and the absolute fluorescence cross sections of the VUV emissions have been measured at selected atomic emission lines and in the synchrotron radiation continuum from 550 to 760 A. Emissions from the O I 1304 A and several S I lines account for the fluorescence observed in the VUV region, while the fluorescence observed in the UV and violet regions is due to excited SO and, also, possibly to excited SO2(+) and SO(+). Structure in the VUV fluorescence excitation function is attributed to predissociation of Rydberg states. The VUV fluorescence resulting from an O2 elimination process, SO2 + h times nu yielding metastable S + O2, has been observed in the present work although the threshold for this process has not been determined. The threshold corresponding to the total dissociation process, SO2 + h times nu yielding metastable S + 2O, has been measured and found to agree reasonably with the expected value calculated from thermochemical data. The processes for the formation of S(+) are also discussed.
Wu, C. Y. R.↗
Oxidation of SO2 by NO2 and O3 on carbon - Implications to tropospheric chemistry
The oxidation of SO2 to sulfate in air at 65 percent relative humidity on carbon particles was investigated gravimetrically in the presence of NO2 and O3. Approximately 1 mg samples of carbon black were exposed to continuously flowing ppbv mixtures of SO2, SO2 + NO2 and SO2 + O3 for prescribed periods of time before desorption into dry N2. Wet chemical analysis of the particles followed desorption. NO2 and O3 were found to have little, if any, effect relative to air on sulfate yields at the concentrations studied.
Cofer, W. R., III↗
Adsorption of O2, SO2, and SO3 on nickel oxide. Mechanism for sulfate formation
Calculations based on the atom superposition and electron delocalization molecular orbital (ASED-MO) technique suggest that O2 will adsorb perferentially end-on at an angle 45 deg from normal on a nickel cation site on the (100) surface of NiO. SO2 adsorption is also stronger on the nickel site; SO2 bonds through the sulfur atom is a plane perpendicular to the surface. Adsorption energies for SO3 on the nickel and oxygen sites are comparable in the perferred orientation in which the SO3 plane is parallel to the surface. On activation, SO3 adsorbed to an O2(-) site forms a trigonal pyramidal SO4 species which yields, with a low barrier, a tetrahedral sulfate anion. Subsequently the anion reorients on the surface. Possibilities for alternative mechanisms which require the formation of Ni3(+) or O2(-) are discussed. NiSO4 thus formed leads to the corrosion of Ni at high temperatures in the SO2+O2/SO3 The SO2+O2/SO3 atmosphere, as discussed in the experimental literature.
Mehandru, S. P.↗
Adsorption of O2, SO2, and SO3, on nickel oxide - Mechanism for sulfate formation
Calculations based on the atom superposition and electron delocalization molecular orbital technique suggest that O2 will adsorb preferentially end-on at an angle 45 deg from normal on a nickel cation site on the (100) surface of NiO. SO2 adsorption is also stronger on the nickel site; SO2 bonds through the sulfur atom in a plane perpendicular to the surface. Adsorption energies for SO3 on the nickel and oxygen sites are comparable in the preferred orientation in which the SO3 plane is parallel to the surface. The calculations suggest that the strength of adsorption varies as O2 greater than SO2 greater than SO3. On activation, SO3 adsorbed to an O(2-) site forms a trigonal pyramidal SO4 species which yields, with a low barrier, a tetrahedral sulfate anion. Subsequently the anion reorients on the surface. Alternative mechanisms which require the formation of Ni(3+) or O(-) are discussed. NiSO4 thus formed may play a passivating role for the corrosion of Ni at low temperatures in the SO2 + O2 + SO3 atmospheres and an active role at high temperatures, as discussed in the experimental literature.
Mehandru, S. P.↗
The global distribution, abundance, and stability of SO2 on Io
Voyager multispectral mosaics, earth-observed spectra, and photometric characterizations have been used to model and globally map the SO2 distribution and abundances, the bolometric hemispheric albedos, and the passive surface temperatures on Io. The SO2 is noted to be concentrated in the bright equatorial band, while being deficient in the region defined by Pele-type volcanic eruptions and the polar regions. The brightest, locally coldest areas correspond to SO2-rich regions, although many small patches occur elsewhere. These results are found to support the regional cold-trapping model for the surface and atmospheric SO2 of Fanale et al. (1982).
Mcewen, Alfred S.↗
The atmospheric abundance of SO2 on Io
The IUE satellite has obtained near-UV spectra of Io with sufficient resolution to ascertain the east, or leading and west, or trailing hemispheres' dayside atmosphere SO2 abundance. The derived geometric albedos are compared with various model albedos that might result from proposed SO2 atmospheres, as well as from localized, sublimation- or volcanism-generated atmospheres. A homogeneous-layer alternative atmosphere is introduced whose upper limit on the average SO2 column density for both hemispheres implies that a collisionally thick SO2 atmosphere of intermediate density may have been present on Io's dayside during the present observations.
Ballester, Gilda E.↗
The role of SO2 on Mars and on the primordial oxygen isotope composition of water on Earth and Mars
We stress the importance of SO2 on Mars. In the case that water should have been supplied in sufficient quantities to the Martian surface by a late veneer and stored in the near surface layers in form of ice, temporary greenhouse warming by SO2 after large SO2 discharges may have been responsible for melting of ice and break-out of water in areas not directly connected to volcanic activity. Aside from water, liquid SO2 could explain at least some of the erosion features on the Martian surface.
Waenke, H.↗
Thermally driven diffusion of SO2 within the surface of Io
The presence of sulfur dioxide (SO2) on Io, together with the fact that the surface layer of Io has extremely high porosity, suggests the possibility of diffusion of this volatile within the surface, as well as exchange between the surface and an atmosphere. The former possibility is investigated through the development of a surface layer thermal model and subsequent calculations of the thermally driven diffusion flux of SO2 within the layer. The major factors affecting the diffusion process are the temperature and temperature gradient in the surface layer throughout the day, and the porosity and grain size in the surface layer. The results indicate that the net transport of SO2 in the near-surface region is downward into the subsurface, causing near-surface depletion of SO2. Near-surface depletion would result in a layer of reduced thermal inertia overlying the bulk of the surface, consistent with thermal eclipse observations of Io. For the present nominal model with 10-micron grains and a porosity of 85 percent, the peak net diurnal downward flux reaches nearly 0.008 g/sq cm per period.
Meade, Paul E.↗