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Titel |
Simulating ultrafine particle formation in Europe using a regional CTM: contribution of primary emissions versus secondary formation to aerosol number concentrations |
VerfasserIn |
C. Fountoukis, I. Riipinen, H. A. C. Denier van der Gon, P. E. Charalampidis, C. Pilinis, A. Wiedensohler, C. O'Dowd, J. P. Putaud, M. Moerman, S. N. Pandis |
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. 18 ; Nr. 12, no. 18 (2012-09-26), S.8663-8677 |
Datensatznummer |
250011471
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Publikation (Nr.) |
copernicus.org/acp-12-8663-2012.pdf |
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Zusammenfassung |
A three-dimensional regional chemical transport model (CTM) with detailed
aerosol microphysics, PMCAMx-UF, was applied to the European domain to
simulate the contribution of direct emissions and secondary formation to
total particle number concentrations during May 2008. PMCAMx-UF uses the
Dynamic Model for Aerosol Nucleation and the Two-Moment Aerosol Sectional
(TOMAS) algorithm to track both aerosol number and mass concentration using
a sectional approach. The model predicts nucleation events that occur over
scales of hundreds up to thousands of kilometers especially over the Balkans
and Southeast Europe. The model predictions were compared against
measurements from 7 sites across Europe. The model reproduces more than
70% of the hourly concentrations of particles larger than 10 nm
(N10) within a factor of 2. About half of these particles are predicted
to originate from nucleation in the lower troposphere. Regional nucleation
is predicted to increase the total particle number concentration by
approximately a factor of 3. For particles larger than 100 nm the effect
varies from an increase of 20% in the eastern Mediterranean to a decrease
of 20% in southern Spain and Portugal resulting in a small average
increase of around 1% over the whole domain. Nucleation has a significant
effect in the predicted N50 levels (up to a factor of 2 increase) mainly
in areas where there are condensable vapors to grow the particles to larger
sizes. A semi-empirical ternary sulfuric acid-ammonia-water parameterization
performs better than the activation or the kinetic parameterizations in
reproducing the observations. Reducing emissions of ammonia and sulfur
dioxide affects certain parts of the number size distribution. |
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