An isotopic analysis of ionising radiation as a source of sulphuric acid
| Autor: | Jens Olaf Pepke Pedersen, Naohiro Yoshida, Henrik Svensmark, Nicolai Bork, Mayuko Nakagawa, Sebastian O. Danielache, Shohei Hattori, Carl Meusinger, Martin Andreas Bødker Enghoff, Matthew S. Johnson, Yuichiro Ueno |
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| Rok vydání: | 2012 |
| Předmět: |
Atmospheric Science
Ozone Aqueous solution 010504 meteorology & atmospheric sciences Isotope Radical Radiochemistry Photodissociation chemistry.chemical_element 010502 geochemistry & geophysics 01 natural sciences Sulfur lcsh:QC1-999 Ion lcsh:Chemistry chemistry.chemical_compound lcsh:QD1-999 chemistry Isotope-ratio mass spectrometry lcsh:Physics 0105 earth and related environmental sciences |
| Zdroj: | Enghoff, M A B, Bork, N C, Hattori, S, Meusinger, C, Nakagawa, M, Pedersen, J O P, Danielache, S, Ueno, Y, Johnson, M S, Yoshida, N & Svensmark, H 2012, ' An isotopic analysis of ionising radiation as a source of sulphuric acid ', Atmospheric Chemistry and Physics, vol. 12, no. 12, pp. 5319-5327 . https://doi.org/10.5194/acp-12-5319-2012 Atmospheric Chemistry and Physics, Vol 12, Iss 12, Pp 5319-5327 (2012) |
| ISSN: | 1680-7324 |
| DOI: | 10.5194/acp-12-5319-2012 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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