phase, composition, and growth mechanism for secondary organic aerosol from the ozonolysis of α-cedrene
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2016
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Abstract
Sesquiterpenes are an important class of biogenic volatile organic compounds
(BVOCs) and have a high secondary organic aerosol (SOA) forming potential.
However, SOA formation from sesquiterpene oxidation has received less
attention compared to other BVOCs such as monoterpenes, and the underlying
mechanisms remain poorly understood. In this work, we present a comprehensive
experimental investigation of the ozonolysis of α-cedrene both in a
glass flow reactor (27–44 s reaction times) and in static Teflon chambers
(30–60 min reaction times). The SOA was collected by impaction or filters,
followed by analysis using attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy and electrospray ionization mass
spectrometry (ESI-MS), or measured online using direct analysis in
real-time mass spectrometry (DART-MS) and aerosol mass spectrometry (AMS). The slow evaporation of
2-ethylhexyl nitrate that was incorporated into the SOA during its formation
and growth gives an estimated diffusion coefficient of
3 × 10−15 cm2 s−1 and shows that SOA is a highly
viscous semisolid. Possible structures of four newly observed low molecular
weight (MW ≤ 300 Da) reaction products with higher oxygen content
than those previously reported were identified. High molecular weight (HMW)
products formed in the early stages of the oxidation have structures
consistent with aldol condensation products, peroxyhemiacetals, and esters.
The size-dependent distributions of HMW products in the SOA, as well as the
effects of stabilized Criegee intermediate (SCI) scavengers on HMW products
and particle formation, confirm that HMW products and reactions of SCI play a crucial role in early stages of particle formation. Our
studies provide new insights into mechanisms of SOA formation and growth in
α-cedrene ozonolysis and the important role of sesquiterpenes in new
particle formation as suggested by field measurements.
| Reference Key |
zhao2016atmosphericphase,
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|---|---|
| Authors | ;Y. Zhao;L. M. Wingen;V. Perraud;B. J. Finlayson-Pitts |
| Journal | Journal of agricultural and food chemistry |
| Year | 2016 |
| DOI |
10.5194/acp-16-3245-2016
|
| URL | |
| Keywords |
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