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Titel |
Global modelling of secondary organic aerosol in the troposphere: a sensitivity analysis |
VerfasserIn |
K. Tsigaridis, M. Kanakidou |
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 ; 3, no. 5 ; Nr. 3, no. 5 (2003-10-31), S.1849-1869 |
Datensatznummer |
250001281
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Publikation (Nr.) |
copernicus.org/acp-3-1849-2003.pdf |
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Zusammenfassung |
A global 3-dimensional chemistry/transport model able to describe
O3, NOx, Volatile Organic Compounds (VOC), sulphur and
NH3 chemistry has been extended to simulate the temporal and spatial distribution of primary and secondary carbonaceous aerosols in the troposphere
focusing on Secondary Organic Aerosol (SOA) formation. A number of global simulations
have been performed to determine a possible range of annual global SOA production and
investigate uncertainties associated with the model results. The studied uncertainties in the
SOA budget have been evaluated to be in decreasing importance: the potentially irreversible
sticking of the semi-volatile compounds on aerosols, the enthalpy of vaporization of these
compounds, the partitioning of SOA on non-carbonaceous aerosols, the conversion of
aerosols from hydrophobic to hydrophilic, the emissions of primary carbonaceous aerosols,
the chemical fate of the first generation products and finally the activity coefficient of the
condensable species. The large uncertainties associated with the emissions of VOC and the
adopted simplification of chemistry have not been investigated in this study. Although not all
sources of uncertainties have been investigated, according to our calculations, the above
factors within the experimental range of variations could result to an overall uncertainty of
about a factor of 20 in the global SOA budget. The global annual SOA production from
biogenic VOC might range from 2.5 to 44.5 Tg of organic matter per year, whereas that from
anthropogenic VOC ranges from 0.05 to 2.62 Tg of organic matter per year. These estimates
can be considered as a lower limit, since partitioning on coarse particles like nitrate, dust or
sea-salt, together with the partitioning and the dissociation of the semi-volatile products in
aerosol water has been neglected. Comparison of model results to observations, where
available, shows a better agreement for the upper budget estimates than for the lower ones. |
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