{"content"=>"Parameterized Yields of Semivolatile Products from Isoprene Oxidation under Different NO Levels: Impacts of Chemical Aging and Wall-Loss of Reactive Gases.", "sub"=>{"content"=>"x"}} (original) (raw)

2018, Environmental science & technology

We developed a parametrizable box model to empirically derive the yields of semivolatile products from VOC oxidation using chamber measurements, while explicitly accounting for the multigenerational chemical aging processes (such as the gas-phase fragmentation and functionalization and aerosol-phase oligomerization and photolysis) under different NO levels and the loss of particles and gases to chamber walls. Using the oxidation of isoprene as an example, we showed that the assumptions regarding the NO -sensitive, multigenerational aging processes of VOC oxidation products have large impacts on the parametrized product yields and SOA formation. We derived sets of semivolatile product yields from isoprene oxidation under different NO levels. However, we stress that these product yields must be used in conjunction with the corresponding multigenerational aging schemes in chemical transport models. As more mechanistic insights regarding SOA formation from VOC oxidation emerge, our box ...

Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low and high NOx conditions

Atmospheric Chemistry and Physics Discussions, 2016

We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation formed in an environmental simulation chamber using dry neutral seed particles, thereby suppressing the role of acid catalyzed multiphase chemistry, at a variety of oxidant conditions. A high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and AEROsols (FIGAERO) allowed for the simultaneous online sampling of the gas and particle composition. Under high HO<sub>2</sub> and low NO conditions, highly oxygenated (O : C ≥ 1) C<sub>5</sub> compounds were major components (~ 50 %) of the SOA. The overall composition of the SOA evolved both as a function of time and as a function of input NO concentrations. As the level of input NO increased, organic nitrates increased in both the gas- and particle-phases, but the domina...

Relative contributions of selected multigeneration products to chamber SOA formed from photooxidation of a range (C10–C17) of n-alkanes under high NO conditions

Atmospheric Environment, 2021

A series of chamber experiments was conducted to investigate the composition of secondary organic aerosol (SOA) following oxidation of a range of parent n-alkanes (C10–C17) in the presence of NOx. The relative contribution of selected species representing first, second, and higher generation products to SOA mass was measured using a high-resolution aerosol mass spectrometer. Gas chromatography was also used for a limited set of amenable species. Relative contributions varied substantially across the range of investigated alkanes reflecting slight changes in SOA composition. The contribution of first-generation cyclic hemiacetal is minimal toward the small end of the investigated range and gradually increase with n-alkane size. The relative contribution of second generation and higher nitrate-containing species, in contrast, decrease with an increased alkane size. A similar trend is observed for relative contribution of organonitrates to SOA. Finally, SOA yield and composition are sensitive to water vapor concentrations. This sensitivity is limited to a narrow range (dry to ~15% RH) with little, if any, impact above 15% suggesting that this impact may be negligible under ambient conditions. The impact of water vapor also appears to decrease with increasing alkane carbon number.

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