Transitions from functionalization to fragmentation reactions of laboratory Secondary Organic Aerosol (SOA) generated from the OH oxidation of alkane precursors

Andrew T. Lambe, Timothy B. Onasch, David R. Croasdale, Justin P. Wright, Alexander T. Martin, Jonathan P. Franklin, Paola Massoli, Jesse H. Kroll, Manjula R. Canagaratna, William H. Brune, Douglas R. Worsnop, Paul Davidovits

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Abstract

Functionalization (oxygen addition) and fragmentation (carbon loss) reactions governing secondary organic aerosol (SOA) formation from the OH oxidation of alkane precursors were studied in a flow reactor in the absence of NOx. SOA precursors were n-decane (n-C10), n-pentadecane (n-C15), n-heptadecane (n-C17), tricyclo[5.2.1.0 2,6]decane (JP-10), and vapors of diesel fuel and Southern Louisiana crude oil. Aerosol mass spectra were measured with a high-resolution time-of-flight aerosol mass spectrometer, from which normalized SOA yields, hydrogen-to-carbon (H/C) and oxygen-to-carbon (O/C) ratios, and C xHy+, CxHyO+, and C xHyO2+ ion abundances were extracted as a function of OH exposure. Normalized SOA yield curves exhibited an increase followed by a decrease as a function of OH exposure, with maximum yields at O/C ratios ranging from 0.29 to 0.74. The decrease in SOA yield correlates with an increase in oxygen content and decrease in carbon content, consistent with transitions from functionalization to fragmentation. For a subset of alkane precursors (n-C10, n-C15, and JP-10), maximum SOA yields were estimated to be 0.39, 0.69, and 1.1. In addition, maximum SOA yields correspond with a maximum in the CxHyO+ relative abundance. Measured correlations between OH exposure, O/C ratio, and H/C ratio may enable identification of alkane precursor contributions to ambient SOA.

Original languageEnglish (US)
Pages (from-to)5430-5437
Number of pages8
JournalEnvironmental Science and Technology
Volume46
Issue number10
DOIs
StatePublished - May 15 2012

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Environmental Chemistry

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    Lambe, A. T., Onasch, T. B., Croasdale, D. R., Wright, J. P., Martin, A. T., Franklin, J. P., Massoli, P., Kroll, J. H., Canagaratna, M. R., Brune, W. H., Worsnop, D. R., & Davidovits, P. (2012). Transitions from functionalization to fragmentation reactions of laboratory Secondary Organic Aerosol (SOA) generated from the OH oxidation of alkane precursors. Environmental Science and Technology, 46(10), 5430-5437. https://doi.org/10.1021/es300274t