Secondary organic aerosol (SOA) contributes a significant fraction to aerosol mass and toxicity.Low-volatility organic vapors are critical intermediates connecting the oxidation of volatile organic compounds (VOCs) to SOA formation. However, the direct measurement of intermediate vapors poses a great challenge, further compounded by the difficulty of linking them to specific precursors from a cocktail of complex emission sources in the vast urbanized areas. Here, we present coordinated measurements of low-volatility oxidation products, termed oxygenated organic molecules (OOMs) in three most urbanized regions in China. With a newly-developed analysis methodology, we are able to assign these OOMs to their likely precursors and ultimately connect SOA formation to various VOCs. At all measurement locations, we find similar OOM
Reducing the amount of organic aerosol
(OA) is crucial to mitigation
of particulate pollution in China. We present time and air-origin
dependent variations of OA markers and source contributions at a regionally
urban background site in South China. The continental air contained
primary OA markers indicative of source categories, such as levoglucosan,
fatty acids, and oleic acid. Secondary OA (SOA) markers derived from
isoprene and monoterpenes also exhibited higher concentrations in
continental air, due to more emissions of their precursors from terrestrial
ecosystems and facilitation of anthropogenic sulfate for monoterpenes
SOA. The marine air and continental–marine mixed air had more
abundant hydroxyl dicarboxylic acids (OHDCA), with anthropogenic unsaturated
organics as potential precursors. However, OHDCA formation in continental
air was likely attributable to both biogenic and anthropogenic precursors.
The production efficiency of OHDCA was highest in marine air, related
to the presence of sulfur dioxide and/or organic precursors in ship
emissions. Regional biomass burning (BB) was identified as the largest
contributor of OA in continental air, with contributions fluctuating
from 8% to 74%. In contrast, anthropogenic SOA accounted for the highest
fraction of OA in marine (37 ± 4%) and mixed air (31 ± 3%),
overriding the contributions from BB. This study demonstrates the
utility of molecular markers for discerning OA pollution sources in
the offshore marine atmosphere, where continental and marine air pollutants
interact and atmospheric oxidative capacity may be enhanced.
Motor vehicle emissions are an important but poorly constrained source of secondary organic aerosol (SOA). Here, we investigated in situ SOA formation from urban roadside air in Hong Kong during winter time using an oxidation flow reactor (OFR), with equivalent atmospheric oxidation ranging from several hours to several days. The campaign-average mass enhancement of OA, nitrate, sulfate, and ammonium upon OFR aging was 7.0, 7.2, 0.8, and 2.6 μg m −3 , respectively. To investigate the sources of SOA formation potential, we performed multilinear regression analysis between measured peak SOA concentrations from OFR and the concentrations of toluene that represent motor vehicle emissions and cooking OA from positive matrix factorization (PMF) analysis of ambient OA. Trafficrelated SOA precursors contributed 92.3%, 92.4%, and 83.1% to the total SOA formation potential during morning rush hours, noon and early afternoon, and evening meal time, respectively. The SOA production factor (PF) was approximately 5.2 times of primary OA (POA) emission factor (EF) and the secondary particulate matter (PM) PF was approximately 2.6 times of primary particles EF. This study highlights the potential benefit of reducing secondary PM production from motor vehicle emissions in mitigating PM pollutions.
Due to the high health risks associated with indoor air pollutants and long‐term exposure, indoor air quality has received increasing attention. In this study, we put emphasis on the molecular composition, source emissions, and chemical aging of air pollutants in a residence with designed activities mimicking ordinary Hong Kong homes. More than 150 air pollutants were detected at molecular level, 87 of which were quantified at a time resolution of not less than 1 hour. The indoor‐to‐outdoor ratios were higher than 1 for most of the primary air pollutants, due to emissions of indoor activities and indoor backgrounds (especially for aldehydes). In contrast, many secondary air pollutants exhibited higher concentrations in outdoor air. Painting ranked first in aldehyde emissions, which also caused great enhancement of aromatics. Incense burning had the highest emissions of particle‐phase organics, with vanillic acid and syringic acid as markers. The other noteworthy fingerprints enabled by online measurements included linoleic acid, cholesterol, and oleic acid for cooking, 2,5‐dimethylfuran, stigmasterol, iso‐/anteiso‐alkanes, and fructose isomers for smoking, C28‐C34 even n‐alkanes for candle burning, and monoterpenes for the use of air freshener, cleaning agents, and camphor oil. We showed clear evidence of chemical aging of cooking emissions, giving a hint of indoor heterogeneous chemistry. This study highlights the value of organic molecules measured at high time resolutions in enhancing our knowledge on indoor air quality.
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