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Titel |
SOA from limonene: role of NO3 in its generation and degradation |
VerfasserIn |
J. L. Fry, A. Kiendler-Scharr, A. W. Rollins, T. Brauers, S. S. Brown, H.-P. Dorn, W. P. Dubé, H. Fuchs, A. Mensah, F. Rohrer, R. Tillmann, A. Wahner, P. J. Wooldridge, R. C. Cohen |
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 ; 11, no. 8 ; Nr. 11, no. 8 (2011-04-28), S.3879-3894 |
Datensatznummer |
250009656
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Publikation (Nr.) |
copernicus.org/acp-11-3879-2011.pdf |
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Zusammenfassung |
The formation of organic nitrates and secondary organic aerosol (SOA) were
monitored during the NO3 + limonene reaction in the atmosphere
simulation chamber SAPHIR at Research Center Jülich. The 24-h run began
in a purged, dry, particle-free chamber and comprised two injections of
limonene and oxidants, such that the first experiment measured SOA yield in
the absence of seed aerosol, and the second experiment yields in the presence
of 10 μg m−3 seed organic aerosol. After each injection,
two separate increases in aerosol mass were observed, corresponding to
sequential oxidation of the two limonene double bonds. Analysis of the
measured NO3, limonene, product nitrate concentrations, and aerosol
properties provides mechanistic insight and constrains rate constants,
branching ratios and vapor pressures of the products. The organic nitrate
yield from NO3 + limonene is ≈30%. The SOA mass yield was observed
to be 25–40%. The first injection is reproduced by a kinetic model. PMF
analysis of the aerosol composition suggests that much of the aerosol mass
results from combined oxidation by both O3 and NO3, e.g., oxidation of
NO3 + limonene products by O3. Further, later aerosol nitrate mass seems
to derive from heterogeneous uptake of NO3 onto unreacted aerosol alkene. |
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