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Titel |
An isotopic analysis of ionising radiation as a source of sulphuric acid |
VerfasserIn |
M. B. Enghoff, N. Bork, S. Hattori, C. Meusinger, M. Nakagawa, J. O. P. Pedersen, S. Danielache, Y. Ueno, M. S. Johnson, N. Yoshida, H. Svensmark |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 12, no. 12 ; Nr. 12, no. 12 (2012-06-19), S.5319-5327 |
Datensatznummer |
250011271
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Publikation (Nr.) |
copernicus.org/acp-12-5319-2012.pdf |
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Zusammenfassung |
Sulphuric acid is an important factor in aerosol nucleation and growth. It
has been shown that ions enhance the formation of sulphuric acid aerosols,
but the exact mechanism has remained undetermined. Furthermore some studies
have found a deficiency in the sulphuric acid budget, suggesting a missing
source. In this study the production of sulphuric acid from SO2 through a
number of different pathways is investigated. The production methods are
standard gas phase oxidation by OH radicals produced by ozone photolysis with
UV light, liquid phase oxidation by ozone, and gas phase oxidation initiated
by gamma rays. The distributions of stable sulphur isotopes in the products
and substrate were measured using isotope ratio mass spectrometry. All
methods produced sulphate enriched in 34S and we find an enrichment factor (δ34S)
of 8.7 ± 0.4‰ (1 standard deviation) for the
UV-initiated OH reaction. Only UV light (Hg emission at 253.65 nm) produced a
clear non-mass-dependent excess of 33S. The pattern of isotopic
enrichment produced by gamma rays is similar, but not equal, to that produced
by aqueous oxidation of SO2 by ozone. This, combined with the relative
yields of the experiments, suggests a mechanism in which ionising radiation
may lead to hydrated ion clusters that serve as nanoreactors for S(IV) to
S(VI) conversion. |
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