Dataset Information

Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models.

ABSTRACT: The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts of using different methods to estimate compound vapour pressures as well as simulating the formation of highly oxygenated organic molecules (HOM) via auto-oxidation on SOA formation indoors. Estimation of vapour pressures for 136 ?-pinene oxidation species by six investigated methods led to standard deviations of 28-216%. Inclusion of HOM formation improved model performance across three of the six assessed vapour pressure estimation methods when comparing against experimental data, particularly when the NO₂ concentration was relatively high. We also explored the predicted SOA composition using two product classification methods, the first assuming the molecule is dominated by one functionality according to its name, and the second accounting for the fractional weighting of each functional group within a molecule. The SOA composition was dominated by the HOM species when the NO₂-to-?-terpineol ratio was high for both product classification methods, as these conditions promoted formation of the nitrate radical and hence formation of HOM monomers. As the NO₂-to-?-terpineol ratio decreased, peroxides and acids dominated the simple classification, whereas for the fractional classification, carbonyl and alcohol groups became more important.

SUBMITTER: Kruza M

PROVIDER: S-EPMC7884095 | biostudies-literature | 2020 Nov

REPOSITORIES: biostudies-literature

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Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models.

Kruza M M McFiggans G G Waring M S MS Wells J R JR Carslaw N N

Atmospheric Environment: X 20201101

The formation of secondary organic aerosol (SOA) indoors is one of the many consequences of the rich and complex chemistry that occurs therein. Given particulate matter has well documented health effects, we need to understand the mechanism for SOA formation indoors and its resulting composition. This study evaluates some uncertainties that exist in quantifying gas-to-particle partitioning of SOA-forming compounds using an indoor detailed chemical model. In particular, we investigate the impacts ...[more]

PMID: 33594348

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Project description:To eliminate the spread of a novel coronavirus breaking out in the end of 2019 (COVID-19), the Chinese government has implemented a nationwide lockdown policy after the Chinese lunar New Year of 2020, resulting in a sharp reduction in air pollutant emissions. To investigate the impact of the lockdown on aerosol chemistry, the number fraction, size distribution and formation process of oxalic acid (C2) containing particles and its precursors were studied using a single particle aerosol mass spectrometer (SPAMS) at the urban site of Liaocheng in the North China Plain (NCP). Our results showed that five air pollutants (i.e., PM2.5, PM10, SO2, NO2, and CO) decreased by 30.0-59.8% during the lockdown compared to those before the lockdown, while O3 increased by 63.9% during the lockdown mainly due to the inefficient titration effect of O3 via NO reduction. The increased O3 concentration can boost the atmospheric oxidizing capacity and further enhance the formation of secondary organic aerosols, thereby significantly enhancing the C2 particles and its precursors as observed during the lockdown. Before the lockdown, C2 particles were significantly originated from biomass burning emissions and their subsequent aqueous-phase oxidation. The hourly variation patterns and correlation analysis before the lockdown suggested that relative humidity (RH) and aerosol liquid water content (ALWC) played a key role in the formation of C2 particles and the increased aerosol acidity can promote the conversion of precursors such as glyoxal (Gly) and methyglyoxal (mGly) into C2 particles in the aqueous phase. RH and ALWC decreased sharply but O3 concentration and solar radiation increased remarkably during the lockdown, the O3-dominated photochemical pathways played an important role in the formation of C2 particles in which aerosol acidity was ineffective. Our study indicated that air pollution treatment sponges on a joint-control and balanced strategy for controlling numerous pollutants.

Project description:The molecular characteristics and formation mechanism of biogenic secondary organic aerosols (BSOAs) in the forested atmosphere are poorly known. Here, we report the temporal variations in and formation processes of BSOA tracers derived from isoprene, monoterpenes, and β caryophyllene in PM2.5 samples collected at the foot of Mt. Huang (483 m a. s. l) in East China during the summer of 2019 with a 3 h time resolution. The concentrations of nearly all of the detected species, including organic carbon (OC), elemental carbon (EC), levoglucosan, and SIA (sum of SO42-, NO3-, and NH4+), were higher at night (19:00-7:00 of the next day) than in the daytime (7:00-19:00). In addition, air pollutants that accumulated by the dynamic transport of the mountain breeze at night were also a crucial reason for the higher BSOA tracers. Most of the BSOA tracers exhibited higher concentrations at night than in the daytime and peaked at 1:00 to 4:00 or 4:00 to 7:00. Those BSOA tracers presented strong correlations with O3 in the daytime rather than at night, indicating that BSOAs in the daytime were primarily derived from the photo-oxidation of BVOCs with O3. The close correlations of BSOA tracers with SO42- and particle acidity (pHis) suggest that BSOAs were primarily derived from the acid-catalyzed aqueous-phase oxidation. Considering the higher relative humidity and LWC concentration at night, the promoted aqueous oxidation was the essential reason for the higher concentrations of BSOA tracers at night. Moreover, levoglucosan exhibited a robust correlation with BSOA tracers, especially β-caryophyllinic acid, suggesting that biomass burning from long-distance transport exerted a significant impact on BSOA formation. Based on a tracer-based method, the estimated concentrations of secondary organic carbon (SOC) derived from isoprene, monoterpenes, and β caryophyllene at night (0.90 ± 0.57 µgC m-3) were higher than those (0.53 ± 0.34 µgC m-3) in the daytime, accounting for 14.5 ± 8.5% and 12.2 ± 5.0% of OC, respectively. Our results reveal that the BSOA formation at the foot of Mt. Huang was promoted by the mountain-valley breezes and anthropogenic pollutants from long-range transport.

Dataset Information

Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models.

Publications

Indoor secondary organic aerosols: Towards an improved representation of their formation and composition in models.

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