期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 14, 期 24, 页码 13801-13816出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-14-13801-2014
关键词
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资金
- US National Science Foundation [AGS-1036675]
- California Agricultural Experiment Station [CA-D-ETX-2102-H, CA-D*-LAW-6403-RR]
- Office of Biological and Environmental Research of the US PNNL
- US DOE [DE-AC06-76RL0 1830]
- Jastro Shields Graduate Research Award (UC Davis)
- Atmospheric Aerosols and Health (AAH) program at UCDavis
- Div Atmospheric & Geospace Sciences
- Directorate For Geosciences [1036675] Funding Source: National Science Foundation
Phenolic compounds, which are emitted in significant amounts from biomass burning, can undergo fast reactions in atmospheric aqueous phases to form secondary organic aerosol (aqSOA). In this study, we investigate the reactions of phenol (compound with formula C6H5OH)), guaiacol (2-methoxyphenol), and syringol (2,6-dimethoxyphenol) with two major aqueous-phase oxidants - the triplet excited states of an aromatic carbonyl (C-3*) and hydroxyl radical (center dot OH). We thoroughly characterize the low-volatility species produced from these reactions and interpret their formation mechanisms using aerosol mass spectrometry (AMS), nanospray desorption electrospray ionization mass spectrometry (nano-DESI MS), and ion chromatography (IC). A large number of oxygenated molecules are identified, including oligomers containing up to six monomer units, functionalized monomer and oligomers with carbonyl, carboxyl, and hydroxyl groups, and small organic acid anions (e.g., formate, acetate, oxalate, and malate). The average atomic oxygen-to-carbon (O / C) ratios of phenolic aqSOA are in the range of 0.85-1.23, similar to those of low-volatility oxygenated organic aerosol (LV-OOA) observed in ambient air. The aqSOA compositions are overall similar for the same precursor, but the reactions mediated by C-3* are faster than center dot OH-mediated reactions and produce more oligomers and hydroxylated species at the point when 50% of the phenolic compound has reacted. Profiles determined using a thermodenuder indicate that the volatility of phenolic aqSOA is influenced by both oligomer content and O / C ratio. In addition, the aqSOA shows enhanced light absorption in the UV-visible region, suggesting that aqueous-phase reactions of phenols may contribute to formation of secondary brown carbon in the atmosphere, especially in regions influenced by biomass burning.
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