Dynamic Oxidative Potential of Atmospheric Organic Aerosol under Ambient Sunlight

摘要

The atmospheric process dynamically changes the chemical compositions of organic aerosol (OA), thereby complicating the interpretation of its health effects. In this study, the dynamic evolution of the oxidative potential of various OA was studied, including wood combustion particles and secondary organic aerosols (SOA) generated from different hydrocarbons (i.e., gasoline, toluene, isoprene, and alpha-pinene). The oxidative potential of OA at different aging stages was subsequently measured by the dithiothreitol consumption (DTTm, mass normalized). We hypothesized that DTT consumptions by OA were modulated by catalytic particulate oxidizers (e.g., quinones), noncatalytic particulate oxidizers (e.g., organic hydroperoxides and peroxyacyl nitrates) and electron-deficient alkenes. The results of this study showed that the oxidative potential of OA decreased after an extended period of aging due to the decomposition of particulate oxidizers and electron-deficient alkenes. Quinones (GC-MS data) partially attributed to the DTIm. of fresh wood smoke particles but rapidly dropped with aging. In biogenic SOA, organic hydroperoxides (4-nitrophenyl boronic acid assay) exclusively accounted for DTTm and decreased with aging. The DTTm of aromatic SOA, mainly comprising organic hydroperoxides and electron-deficient alkenes (FTIR data), was shortly elevated during the early atmospheric process; however, it showed a noticeable decrease (32-75%) for a long period of aging. We concluded that fresh or moderately aged OA are more reactive to a sulfhydryl group than highly aged OA.