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dc.contributor.authorAlexander, Becky
dc.contributor.authorPark, Rokjin J.
dc.contributor.authorJacob, Daniel J.
dc.contributor.authorGong, Sunling
dc.date.accessioned2014-03-17T18:31:47Z
dash.embargo.terms2009-06-01
dc.date.issued2009
dc.identifier.citationAlexander, Becky, Rokjin J. Park, Daniel J. Jacob, and Sunling Gong. 2009. “Transition Metal-Catalyzed Oxidation of Atmospheric Sulfur: Global Implications for the Sulfur Budget.” Journal of Geophysical Research: Atmospheres 114 (D2): D02309. doi:10.1029/2008jd010486. http://dx.doi.org/10.1029/2008JD010486.en_US
dc.identifier.issn2169-897Xen_US
dc.identifier.issn2169-8996en_US
dc.identifier.urihttp://nrs.harvard.edu/urn-3:HUL.InstRepos:11923057
dc.description.abstractWe use observations of the oxygen-17 excess \((Δ^{17}O)\) of sulfate in the Arctic to quantify the sulfate source from aqueous \(SO_2 (S(IV))\) oxidation by \(O_2\) catalyzed by transition metals. Due to the lack of photochemically produced OH and \(H_2O_2\) in high latitudes during winter, combined with high anthropogenic \(SO_2\) emissions in the Northern Hemisphere, oxidation by \(O_3\) is predicted to dominate sulfate formation during winter in this region. However, \(Δ^{17}O\) measurements of sulfate aerosol collected in Alert, Canada, are not consistent with \(O_3\) as the dominant oxidant and indicate that a S(IV) oxidant with near-zero \(Δ^{17}O\) values \((O_2)\) is important during winter. We use a global chemical transport model to interpret quantitatively the Alert observations and assess the global importance of sulfate production by Fe(III)- and Mn(II)-catalyzed oxidation of S(IV) by \(O_2\). We scale anthropogenic and natural atmospheric metal concentrations to primary anthropogenic sulfate and dust concentrations, respectively. The solubility and oxidation state of these metals is determined by cloud liquid water content, source, and sunlight. By including metal-catalyzed S(IV) oxidation, the model is consistent with the \(Δ^{17}O\) magnitudes in the Alert data during winter. Globally, we find that this mechanism contributes 9–17% to sulfate production. The inclusion of metal-catalyzed oxidation does not resolve model discrepancies with surface SO2 and sulfate observations in Europe. Oxygen isotope measurements of sulfate aerosols collected near anthropogenic and dust sources of metals would help to verify the importance of this sulfur oxidation pathway.en_US
dc.description.sponsorshipEngineering and Applied Sciencesen_US
dc.language.isoen_USen_US
dc.publisherWiley-Blackwellen_US
dc.relation.isversionofdoi:10.1029/2008jd010486en_US
dash.licenseLAA
dc.subjectsulfate aerosolen_US
dc.subjecttropospheric chemistryen_US
dc.subjectoxygen isotopesen_US
dc.titleTransition Metal-Catalyzed Oxidation of Atmospheric Sulfur: Global Implications for the Sulfur Budgeten_US
dc.typeJournal Articleen_US
dc.description.versionVersion of Recorden_US
dc.relation.journalJournal of Geophysical Research: Atmospheresen_US
dash.depositing.authorJacob, Daniel J.
dc.date.available2014-03-18T07:30:53Z
dc.identifier.doi10.1029/2008jd010486*
dash.contributor.affiliatedJacob, Daniel


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