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Titel |
Development of a parallel sampling and analysis method for the elucidation of gas/particle partitioning of oxygenated semi-volatile organics: a limonene ozonolysis study |
VerfasserIn |
S. Rossignol, L. Chiappini, E. Perraudin, C. Rio, S. Fable, R. Valorso, J. F. Doussin |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1867-1381
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Measurement Techniques ; 5, no. 6 ; Nr. 5, no. 6 (2012-06-27), S.1459-1489 |
Datensatznummer |
250002977
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Publikation (Nr.) |
copernicus.org/amt-5-1459-2012.pdf |
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Zusammenfassung |
The gas/particle partitioning behaviour of the semi-volatile fraction of
secondary organic matter and the associated multiphase chemistry are key
features to accurately evaluate climate and health impacts of secondary
organic aerosol (SOA). However, today, the partitioning of oxygenated
secondary species is rarely assessed in experimental SOA studies and SOA
modelling is still largely based on estimated partitioning data. This paper
describes a new analytical approach, solvent-free and easy to use, to
explore the chemical composition of the secondary organic matter at a
molecular scale in both gas and particulate phases. The method is based on
thermal desorption (TD) of gas and particulate samples, coupled with gas
chromatography (GC) and mass spectrometry (MS), with derivatisation on
sampling supports. Gaseous compounds were trapped on Tenax TA adsorbent
tubes pre-coated with pentafluorobenzylhydroxylamine (PFBHA) or
N-Methyl-N-(t-butyldimethylsilyl)trifluoroacetamide (MTBSTFA). Particulate
samples were collected onto quartz or Teflon-quartz filters and subsequently
subjected to derivatisation with PFBHA or MTBSTFA before TD-GC/MS analysis.
Method development and validation are presented for an atmospherically
relevant range of organic acids and carbonyl and hydroxyl compounds.
Application of the method to a limonene ozonolysis experiment conducted in
the EUPHORE simulation chamber under simulated atmospheric conditions of low
concentrations of limonene precursor and relative humidity, provides an
overview of the method capabilities. Twenty-five compounds were positively
or tentatively identified, nine being in both gaseous and particulate
phases; and twelve, among them tricarboxylic acids, hydroxyl dicarboxylic
acids and oxodicarboxylic acids, being detected for the first time. |
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