期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 16, 期 17, 页码 11001-11018出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-16-11001-2016
关键词
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资金
- Camille and Henry Dreyfus Postdoctoral Fellowship Program in Environmental Chemistry
- CAPES Foundation
- Ministry of Education of Brazil [99999.000542/2015-06]
- National Oceanic and Atmospheric Administration (NOAA) Climate Program Office's AC4 program [NA13OAR4310064]
- Pakistani Higher Education Commission
- United States Agency for International Development (US-AID)
We report the formation of aliphatic organosulfates (OSs) in secondary organic aerosol (SOA) from the photooxidation of C-10-C-12 alkanes. The results complement those from our laboratories reporting the formation of OSs and sulfonates from gas-phase oxidation of polycyclic aromatic hydrocarbons (PAHs). Both studies strongly support the formation of OSs from the gas-phase oxidation of anthropogenic precursors, as hypothesized on the basis of recent field studies in which aromatic and aliphatic OSs were detected in fine aerosol collected from several major urban locations. In this study, dodecane, cyclodecane and decalin, considered to be important SOA precursors in urban areas, were photochemically oxidized in an outdoor smog chamber in the presence of either non-acidified or acidified ammonium sulfate seed aerosol. Effects of acidity and relative humidity on OS formation were examined. Aerosols collected from all experiments were characterized by ultra performance liquid chromatography coupled to electrospray ionization high-resolution quadrupole time-of-flight mass spectrometry (UPLC/ESI-HR-QTOFMS). Most of the OSs identified could be explained by formation of gaseous epoxide precursors with subsequent acid-catalyzed reactive uptake onto sulfate aerosol and/or heterogeneous reactions of hydroperoxides. The OSs identified here were also observed and quantified in fine urban aerosol samples collected in Lahore, Pakistan, and Pasadena, CA, USA. Several OSs identified from the photooxidation of decalin and cyclodecane are isobars of known monoterpene organosulfates, and thus care must be taken in the analysis of alkane-derived organosulfates in urban aerosol.
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