In:
Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 12 ( 2020-06-24), p. 7291-7306
Kurzfassung:
Abstract. Secondary organic aerosol (SOA) is an important component of fine particular matter (PM2.5). Most air quality models use an equilibrium partitioning method along with the saturation vapor pressure (SVP) of semivolatile organic compounds (SVOCs) to predict SOA formation. However, the models typically assume that the organic particulate matter (OPM) is an ideal mixture and ignore the partitioning of water vapor to OPM. In this study, the Community Multiscale Air Quality model (CMAQ) is updated to investigate the impacts of water vapor partitioning and nonideality of the
organic–water mixture on SOA formation during winter (January) and summer
(July) of 2013 over eastern China. The updated model treats the partitioning of water vapor molecules into OPM and uses the universal functional activity coefficient (UNIFAC) model to estimate the activity coefficients of species in the organic–water mixture. The modified model can generally capture the observed surface organic carbon (OC) with a correlation coefficient R of 0.7 and the surface organic aerosol (OA) with the mean fractional bias (MFB) and mean fractional error (MFE) of −0.28 and 0.54, respectively. SOA concentration shows significant seasonal and spatial variations, with high concentrations in the North China Plain (NCP), central China, and the Sichuan Basin (SCB) regions during winter (up to 25 µg m−3) and in the Yangtze River Delta (YRD) during summer (up to 16 µg m−3). In winter, SOA decreases slightly in the updated model, with a monthly averaged relative change of 10 %–20 % in the highly concentrated areas, mainly due to organic–water interactions. The monthly averaged concentration of SOA increases greatly in summer, by 20 %–50 % at the surface and 30 %–60 % in the whole column. The increase in SOA is mainly due
to the increase in biogenic SOA in inland areas and anthropogenic SOA in
coastal areas. As a result, the averaged aerosol optical depth (AOD) is
increased by up to 10 %, and the cooling effect of aerosol radiative
forcing (ARF) is enhanced by up to 15 % over the YRD in summer. The aerosol
liquid water content associated with OPM (ALWorg) at the surface is relatively high in inland areas in winter and over the ocean in summer, with a monthly averaged concentration of 0.5–3.0 and 5–7 µg m−3, respectively. The hygroscopicity parameter κ of OA based on the κ–Köhler theory is determined using the modeled ALWorg. The correlation of κ with the O:C ratio varies significantly across
different cities and seasons. Analysis of two representative cities, Jinan
(in the NCP) and Nanjing (in the YRD), shows that the impacts of water partitioning
and nonideality of the organic–water mixture on SOA are sensitive to
temperature, relative humidity (RH), and the SVP of SVOCs. The two processes exhibit opposite impacts on SOA in eastern China. Water uptake increases SOA by up to 80 % in the organic phase, while including nonunity activity coefficients decreases SOA by up to 50 %. Our results indicate that both water partitioning into OPM and the activity coefficients of the condensed organics should be considered in simulating SOA formation from gas–particle partitioning, especially in hot and humid environments.
Materialart:
Online-Ressource
ISSN:
1680-7324
DOI:
10.5194/acp-20-7291-2020
DOI:
10.5194/acp-20-7291-2020-supplement
Sprache:
Englisch
Verlag:
Copernicus GmbH
Publikationsdatum:
2020
ZDB Id:
2092549-9
ZDB Id:
2069847-1
