Transitions from Functionalization to Fragmentation Reactions of Laboratory Secondary Organic Aerosol (SOA) Generated from the OH Oxidation of Alkane Precursors. 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. Environmental Science & Technology, 46(10):5430-5437, 5, 2012.
Paper
Website abstract bibtex 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 NO. SOA precursors were n-decane (n-C-10), n-pentadecane (n-C-15), n-heptadecane (n-C-17), tricyclo[5.2.1.0(2,6)]clecane (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-tocarbon (H/C) and oxygen-to-carbon (O/C) ratios, and CxHy+, CxHyO+, and CxHyO2+ 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-C-10, n-C-15, 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, 0/C ratio, and H/C ratio may enable identification of alkane precursor contributions to ambient SOA.
@article{
title = {Transitions from Functionalization to Fragmentation Reactions of Laboratory Secondary Organic Aerosol (SOA) Generated from the OH Oxidation of Alkane Precursors},
type = {article},
year = {2012},
identifiers = {[object Object]},
keywords = {Aerosols,Aerosols: analysis,Alkanes,Alkanes: chemistry,Carbon,Carbon: analysis,Hydroxyl Radical,Hydroxyl Radical: chemistry,Laboratories,Mass Spectrometry,Mexico,Organic Chemicals,Organic Chemicals: analysis,Oxidation-Reduction,Oxygen,Oxygen: analysis,Petroleum Pollution,Petroleum Pollution: analysis,Time Factors,air-pollution sources,emissions,evolution,high-resolution,mass-spectrometry,molecular-structure,n-alkanes,nox,photooxidation,smog-chamber},
pages = {5430-5437},
volume = {46},
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month = {5},
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notes = {<b>From Duplicate 2 (<i>Transitions from Functionalization to Fragmentation Reactions of Laboratory Secondary Organic Aerosol (SOA) Generated from the OH Oxidation of Alkane Precursors</i> - Lambe, Andrew T; Onasch, Timothy B; Croasdale, David R; Wright, Justin P; Martin, Alexander T; Franklin, Jonathan P; Massoli, Paola; Kroll, Jesse H; Canagaratna, Manjula R; Brune, William H; Worsnop, Douglas R; Davidovits, Paul)<br/></b><br/><b>From Duplicate 2 (<i>Transitions from Functionalization to Fragmentation Reactions of Laboratory Secondary Organic Aerosol (SOA) Generated from the OH Oxidation of Alkane Precursors</i> - Lambe, Andrew T; Onasch, Timothy B; Croasdale, David R; Wright, Justin P; Martin, Alexander T; Franklin, Jonathan P; Massoli, Paola; Kroll, Jesse H; Canagaratna, Manjula R; Brune, William H; Worsnop, Douglas R; Davidovits, Paul)<br/></b><br/>941LM<br/>Times Cited:8<br/>Cited References Count:50},
folder_uuids = {bab84624-6274-432e-ab41-d62bfeb363da,a5042800-0ea9-4d06-b074-9eaaca092a07},
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 NO. SOA precursors were n-decane (n-C-10), n-pentadecane (n-C-15), n-heptadecane (n-C-17), tricyclo[5.2.1.0(2,6)]clecane (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-tocarbon (H/C) and oxygen-to-carbon (O/C) ratios, and CxHy+, CxHyO+, and CxHyO2+ 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-C-10, n-C-15, 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, 0/C ratio, and H/C ratio may enable identification of alkane precursor contributions to ambient SOA.},
bibtype = {article},
author = {Lambe, Andrew T and Onasch, Timothy B and Croasdale, David R and Wright, Justin P and Martin, Alexander T and Franklin, Jonathan P and Massoli, Paola and Kroll, Jesse H and Canagaratna, Manjula R and Brune, William H and Worsnop, Douglas R and Davidovits, Paul},
journal = {Environmental Science & Technology},
number = {10}
}
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