期刊
ATMOSPHERIC ENVIRONMENT
卷 119, 期 -, 页码 144-155出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.atmosenv.2015.08.010
关键词
Aromatic hydrocarbon; NOx; Secondary organic aerosol; Kinetic modeling; Radicals
资金
- National Science Foundation [ATM 0901282]
- W. M. Keck Foundation
Secondary organic aerosol (SOA) formation from aromatic hydrocarbon photooxidation is highly sensitive to NO concentration. The instantaneous effect of NO on SOA formation from m-xylene photooxidation is investigated in this work by data mining 10 years of aromatic hydrocarbon chamber experiments conducted in the UC Riverside/CE-CERT chamber. First, the effect of sub-ppb NO concentrations on SOA formation is explored. The relationship of SOA growth rate to 1) NO2/NO ratio; 2) instantaneous HC/NO; 3) absolute NO concentration; 4) peroxy radical reaction branching ratio and 5) hydroxyl radical concentration are illustrated. Second, continuous and stepwise NO, NO2 and HONO injection are applied to m-xylene photooxidation experiments to simulate continuous NO sources in an urban area. The influence of these reaction scenarios on radical concentrations and SOA formation is explored. [HO2 center dot]/[RO2 center dot.] shows a strong correlation with SOA yields in addition to [(OH)-O-center dot]/[HO2 center dot], [(OH)-O-center dot], [HO2 center dot] and [RO2 center dot]. Enhanced SOA formation is observed when low NO levels (<1 ppb) are artificially maintained by continuous or step-wise injection; consistent with earlier research, SOA formation is observed to be suppressed by large initial NO injections. It is proposed that NO at sub-ppb level enhances (OH)-O-center dot formation increasing HO2 center dot and RO2 center dot and therefore promoting SOA formation. Further, two NO pathways (one promoting and one suppressing SOA formation) and one extremely low NO phase (NO free) are used to demonstrate the evolution of NO impact on SOA formation during photooxidation. This study implies that SOA yields from aromatic hydrocarbon and low NO photooxidation is previously underestimated due to differences between traditional environmental chamber experiments and atmospheric reactivity. (C) 2015 Published by Elsevier Ltd.
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