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Dipartimento CFTA, Universita` di Palermo
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- PublicationRestrictedEmission of bromine and iodine from Mount Etna volcano(2005-08-25)
; ; ; ; ; ; ; ; ; ;Aiuppa, A.; Dipartimento CFTA, Universita` di Palermo ;Federico, C.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;Franco, A.; Dipartimento CFTA, Universita` di Palermo ;Giudice, G.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;Gurrieri, S.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;Inguaggiato, S.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;Liuzzo, M.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;McGonigle, A. J. S.; Department of Geography, University of Cambridge, Downing Place, CB2 3EN Cambridge, UK ;Valenza, M.; Dipartimento CFTA, Universita` di Palermo; ; ; ; ; ; ; ; Constraining fluxes of volcanic bromine and iodine to the atmosphere is important given the significant role these species play in ozone depletion. However, very few such measurements have been made hitherto, such that global volcanic fluxes are poorly constrained. Here we extend the data set of volcanic Br and I degassing by reporting the first measurements of bromine and iodine emissions from Mount Etna. These data were obtained using filter packs and contemporaneous ultraviolet spectroscopic SO2 flux measurements, resulting in time-averaged emission rates of 0.7 kt yr 1 and 0.01 kt yr 1 for Br and I, respectively, from April to October 2004, from which we estimate global Br and I fluxes of order 13 (range, 3â 40) and 0.11 (range, 0.04â 6.6) kt yr 1. Observed changes in plume composition highlight the coherent geochemical behavior of HCl, HF, HBr, and HI during magmatic degassing, and strong fractionation of these species with respect to SO2.301 118 - PublicationOpen AccessThe tropospheric processing of acidic gases and hydrogen sulphide in volcanic gas plumes as inferred from field and model investigations(2007-03-13)
; ; ; ; ; ; ; ; ;Aiuppa, A.; Università di Palermo, Dipartimento CFTA ;Franco, A.; Università di Palermo, Dipartimento CFTA ;von Glasow, R.; Institut für Umweltphysik, University of Heidelberg, Germany ;Allen, A. G.; School of Geography, Earth and Environmental Sciences, University of Birmingham, UK ;D'Alessandro, W.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Palermo, Palermo, Italia ;Mather, T. A.; Earth Science Department, University of Oxford, UK ;Pyle, D. M.; Earth Science Department, University of Oxford, UK ;Valenza, M.; Università di Palermo, Dipartimento CFTA; ; ; ; ; ; ; Improving the constraints on the atmospheric fate and depletion rates of acidic compounds persistently emitted by non-erupting (quiescent) volcanoes is important for quantitatively predicting the environmental impact of volcanic gas plumes. Here, we present new experimental data coupled with modelling studies to investigate the chemical processing of acidic volcanogenic species during tropospheric dispersion. Diffusive tube samplers were deployed at Mount Etna, a very active open-conduit basaltic volcano in eastern Sicily, and Vulcano Island, a closed-conduit quiescent volcano in the Aeolian Islands (northern Sicily). Sulphur dioxide (SO2), hydrogen sulphide (H2S), hydrogen chloride (HCl) and hydrogen fluoride (HF) concentrations in the volcanic plumes (typically several minutes to a few hours old) were repeatedly determined at distances from the summit vents ranging from 0.1 to ~10 km, and under different environmental conditions. At both volcanoes, acidic gas concentrations were found to decrease exponentially with distance from the summit vents (e.g., SO2 decreases from ~10,000 μg/m3 at 0.1 km from Etna’s vents down to ~7 _μg/m3 at ~10km distance), reflecting the atmospheric dilution of the plume within the acid gas-free background troposphere. Conversely, SO2/HCl, SO2/HF, and SO2/H2S ratios in the plume showed no systematic changes with plume aging, and fit source compositions within analytical error. Assuming that SO2 losses by reaction are small during short-range atmospheric transport within quiescent (ash-free) volcanic plumes, our observations suggest that, for these short transport distances, atmospheric reactions for H2S and halogens are also negligible. The one-dimensional model MISTRA was used to simulate quantitatively the evolution of halogen and sulphur compounds in the plume of Mt. Etna. Model predictions support the hypothesis of minor HCl chemical processing during plume transport, at least in cloud-free conditions. Larger variations in the modelled SO2/HCl ratios were predicted under cloudy conditions, due to heterogeneous chlorine cycling in the aerosol phase. The modelled evolution of the SO2/H2S ratios is found to be substantially dependent on whether or not the interactions of H2S with halogens are included in the model. In the former case, H2S is assumed to be oxidized in the atmosphere mainly by OH, which results in minor chemical loss for H2S during plume aging and produces a fair match between modelled and measured SO2/H2S ratios. In the latter case, fast oxidation of H2S by Cl leads to H2S chemical lifetimes in the early plume of a few seconds, and thus SO2 to H2S ratios that increase sharply during plume transport. This disagreement between modelled and observed plume compositions suggests that more in-detail kinetic investigations are required for a proper evaluation of H2S chemical processing in volcanic plumes.167 92 - PublicationOpen AccessThe tropospheric processing of acidic gases and hydrogen sulphide in volcanic gas plumes as inferred from field and model investigations(2006)
; ; ; ; ; ; ; ; ;Aiuppa, A.; Dipartimento CFTA, Universit `a di Palermo, Palermo, Italy ;Franco, A.; Dipartimento CFTA, Universit `a di Palermo, Palermo, Italy ;von Glasow, R.; Institut f ¨ ur Umweltphysik, University of Heidelberg, Germany ;Allen, A. G.; School of Geography, Earth and Environmental Sciences, University of Birmingham, UK ;D'Alessandro, W.; Istituto Nazionale di Geofisica e Vulcanologia, Sezione Pisa, Pisa, Italia ;Mather, T. A.; Earth Science Department, University of Oxford, UK ;Pyle, D. M.; Earth Science Department, University of Oxford, UK ;Valenza, M.; Dipartimento CFTA, Universit `a di Palermo, Palermo, Italy; ; ; ; ; ; ; Improving the constraints on the atmospheric fate and depletion rates of acidic compounds persistently emitted by non-erupting (quiescent) volcanoes is important for quantitatively predicting the environmental impact of volcanic gas plumes. Here, we present new experimental data coupled with modelling studies to investigate the chemical processing of acidic volcanogenic species during tropospheric dispersion. Diffusive tube samplers were deployed at Mount Etna, a very active open-conduit basaltic volcano in eastern Sicily, and Vulcano Island, a closed-conduit quiescent volcano in the Aeolian Islands (northern Sicily). Sulphur dioxide (SO2), hydrogen sulphide (H2S), hydrogen chloride (HCl) and hydrogen fluoride (HF) concentrations in the volcanic plumes (typically several minutes to a few hours old) were repeatedly determined at distances from the summit vents ranging from 0.1 to 10 km, and under different environmental conditions. At both volcanoes, acidic gas concentrations were found to decrease exponentially with distance from the summit vents (e.g., SO2 decreases from 10 000 μg/m3 at 0.1 km from Etna’s vents down to 7 μg/m3 at 10 km distance), reflecting the atmospheric dilution of the plume within the acid gas-free background troposphere. Conversely, SO2/HCl, SO2/HF, and SO2/H2S ratios in the plume showed no systematic changes with plume aging, and fit source compositions within analytical error. Assuming that SO2 losses by reaction are small during short-range atmospheric transport within quiescent (ash-free) volcanic plumes, our observations suggest that, for these short transport distances, atmospheric reactions for H2S and halogens are also negligible. The one-dimensional model MISTRA was used to simulate quantitatively the evolution of halogen and sulphur compounds in the plume of Mt. Etna. Model predictions support the hypothesis of minor HCl chemical processing during plume transport, at least in cloud-free conditions. Larger variations in the modelled SO2/HCl ratios were predicted under cloudy conditions, due to heterogeneous chlorine cycling in the aerosol phase. The modelled evolution of the SO2/H2S ratios is found to be substantially dependent on whether or not the interactions of H2S with halogens are included in the model. In the former case, H2S is assumed to be oxidized in the atmosphere mainly by OH, which results in minor chemical loss for H2S during plume aging and produces a fair match between modelled and measured SO2/H2S ratios. In the latter case, fast oxidation of H2S by Cl leads to H2S chemical lifetimes in the early plume of a few seconds, and thus SO2 to H2S ratios that increase sharply during plume transport. This disagreement between modelled and observed plume compositions suggests that more in-detail kinetic investigations are required for a proper evaluation of H2S chemical processing in volcanic plumes.222 116