Role of the reaction of stabilized Criegee intermediates with peroxy radicals in particle formation and growth in air

Physical Chemistry Chemical Physics : PCCP
Yue ZhaoBarbara J Finlayson-Pitts

Abstract

Ozonolysis of alkenes is an important source of secondary organic aerosol (SOA) in the atmosphere. However, the mechanisms by which stabilized Criegee intermediates (SCI) react to form and grow the particles, and in particular the contributions from oligomers, are not well understood. In this study, ozonolysis of trans-3-hexene (C6H12), as a proxy for small alkenes, was investigated with an emphasis on the mechanisms of particle formation and growth. Ozonolysis experiments were carried out both in static Teflon chambers (18-20 min reaction times) and in a glass flow reactor (24 s reaction time) in the absence and presence of OH or SCI scavengers, and under different relative humidity (RH) conditions. The chemical composition of polydisperse and size-selected SOA particles was probed using different mass spectrometric techniques and infrared spectroscopy. Oligomers having SCI as the chain unit are found to be the dominant components of such SOA particles. The formation mechanism for these oligomers suggested by our results follows the sequential addition of SCI to organic peroxy (RO2) radicals, in agreement with previous studies by Moortgat and coworkers. Smaller particles are shown to have a relatively greater contribution from...Continue Reading

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Citations

Jan 16, 2016·The Journal of Physical Chemistry. a·Nanna MyllysHanna Vehkamaki
Jun 17, 2016·Physical Chemistry Chemical Physics : PCCP·Josep M Anglada, Albert Solé
Jan 14, 2017·Physical Chemistry Chemical Physics : PCCP·Yosuke SakamotoJun Hirokawa
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Aug 5, 2018·Proceedings of the National Academy of Sciences of the United States of America·Christopher M KensethJohn H Seinfeld
Jul 28, 2021·The Journal of Physical Chemistry. a·Mei-Tsan KuoKaito Takahashi

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