OligomerizationReaction of the Criegee Intermediate Leads to Secondary Organic AerosolFormation in Ethylene Ozonolysis.
In: Journal of Physical Chemistry A, Jg. 117 (2013-12-05), Heft 48, S. 12912-12921
academicJournal
Zugriff:
Ethylene ozonolysis was investigatedin laboratory experiments using a Teflon bag reactor. A negative ionchemical ionization mass spectrometer (NI-CIMS) using SO2Cl–and Cl–as reagent ions wasused for product analysis. In addition to the expected gas-phase products,such as formic acid and hydroperoxymethyl formate, oligomeric hydroperoxidescomposed of the Criegee intermediate (CH2OO) as a chainunit were observed. Furthermore, we observed secondary organic aerosol(SOA) formation from the ethylene ozonolysis, and the particle-phaseproducts were also analyzed by NI-CIMS. The CH2OO oligomerswere also observed as particle-phase components, suggesting that theoligomeric hydroperoxides formed in the gas phase partition into theparticle phase. By adding methanol as a stabilized Criegee intermediatescavenger, both the gas-phase oligomer formation and SOA formationwere strongly suppressed. This indicates that CH2OO playsa critical role in the formation of oligomeric hydroperoxides followedby SOA formation in ethylene ozonolysis. A new formation mechanismfor the oligomeric hydroperoxides, which includes sequential additionof CH2OO to hydroperoxides, is proposed. [ABSTRACT FROM AUTHOR]
Titel: |
OligomerizationReaction of the Criegee Intermediate Leads to Secondary Organic AerosolFormation in Ethylene Ozonolysis.
|
---|---|
Autor/in / Beteiligte Person: | Sakamoto, Yosuke ; Inomata, Satoshi ; Hirokawa, Jun |
Link: | |
Zeitschrift: | Journal of Physical Chemistry A, Jg. 117 (2013-12-05), Heft 48, S. 12912-12921 |
Veröffentlichung: | 2013 |
Medientyp: | academicJournal |
ISSN: | 1089-5639 (print) |
DOI: | 10.1021/jp408672m |
Schlagwort: |
|
Sonstiges: |
|