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Sources of secondary organic aerosols in the Pearl River Delta region in fall: Contributions from the aqueous reactive uptake of dicarbonyls
Li, N (Li, Nan)[ 1,2 ]; Fu, TM (Fu, Tzung-May)[ 3,4 ]; Cao, JJ (Cao, Junji)[ 1,5 ]; Lee, SC (Lee, Shuncheng)[ 6 ]; Huang, XF (Huang, Xiao-Feng)[ 7 ]; He, LY (He, Ling-Yan)[ 7 ]; Ho, KF (Ho, Kin-Fai)[ 8 ]; Fu, JS (Fu, Joshua S.)[ 9 ]; Lam, YF (Lam, Yun-Fat)[ 10 ]
2013-09-30
Source PublicationATMOSPHERIC ENVIRONMENT
Volume76Issue:SIPages:200-207
Subtype期刊论文
Abstract

We used the regional air quality model CMAQ to simulate organic aerosol (OA) concentrations over the Pearl River Delta region (PRO) and compared model results to measurements. Our goals were (1) to evaluate the potential contribution of the aqueous reactive uptake of dicarbonyls (glyoxal and methylglyoxal) as a source of secondary organic aerosol (SOA) in an urban environment, and (2) to quantify the sources of SOA in the PRO in fall. We improved the representation of dicarbonyl gas phase chemistry in CMAQ as well as added SOA formation via the irreversible uptake of dicarbonyls by aqueous aerosols and cloud droplets, characterized by a reactive uptake coefficient gamma = 2.9 x 10(-3) based on laboratory studies. Our model results were compared to aerosol mass spectrometry (AMS) measurements in Shenzhen during a photochemical smog event in fall 2009. Including the new dicarbonyl SOA source in CMAQ led to an increase in the simulated mean SOA concentration at the sampling site from 4.1 mu g m(-3) to 9.0 mu g m(-3) during the smog event, in better agreement with the mean observed oxygenated OA (OOA) concentration (8.0 mu z m(-3)). The simulated SOA reproduced the variability of observed OOA (r = 0.89). Moreover, simulated dicarbonyl SOA was highly correlated with simulated sulfate (r = 0.72), consistent with the observed high correlation between OOA and sulfate (r = 0.84). Including the dicarbonyl SOA source also increased the mean simulated concentrations of total OA from 8.2 mu g m(-3) to 13.1 mu g m(-3) closer to the mean observed OA concentration (16.5 mu g m(-3)). The remaining difference between the observed and simulated OA was largely due to impacts from episodic biomass burning emissions, but the model did not capture this variability. We concluded that, for the PRD in fall and outside of major biomass burning events, 75% of the total SOA was biogenic. Isoprene was the most important precursor, accounting for 41% of the total SOA. Aromatics accounted for 13% of the total SOA. Our results show that the aqueous chemistry of dicarbonyls can be an important SOA source, potentially accounting for 53% of the total surface SOA in the PRD in fall.

KeywordSecondary Organic Aerosol Glyoxal Methylglyoxal Cmaq Pearl River Delta (Prd)
DOI10.1016/j.atmosenv.2012.12.005
Indexed BySCI ; EI
Language英语
Citation statistics
Cited Times:23[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.ieecas.cn/handle/361006/9938
Collection粉尘与环境研究室
Corresponding AuthorFu, TM (Fu, Tzung-May)[ 3,4 ]
Affiliation1.Key Lab of Aerosol Science & Technology, SKLLQG, Institute of Earth Environment, Chinese Academy of Sciences, Xi’an, China;
2.Graduate University of Chinese Academy of Science, Beijing, China;
3.Department of Atmospheric and Oceanic Sciences and Laboratory for Climate and Ocean-Atmosphere Studies, School of Physics,Peking University, Beijing, China;
4.Institute of Global Environmental Change, Xi’an Jiaotong University, Xi’an, China;
5.Department of Civil and Structural Engineering, Research Center for Environmental Technology and Management,The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China;
6.Key Laboratory for Urban Habitat Environmental Science and Technology, School of Environment and Energy, Peking University ShenzhenGraduate School, Shenzhen, China;
7.School of Public Health and Primary Care, The Chinese University of Hong Kong, Sha Tin, Hong Kong, China;
8.Department of Civil and Environmental Engineering, University of Tennessee, Knoxville, TN 37996, USA;
9.School of Energy and Environment, City University of Hong Kong, Hong Kong, China
Recommended Citation
GB/T 7714
Li, N ,Fu, TM ,Cao, JJ ,et al. Sources of secondary organic aerosols in the Pearl River Delta region in fall: Contributions from the aqueous reactive uptake of dicarbonyls[J]. ATMOSPHERIC ENVIRONMENT,2013,76(SI):200-207.
APA Li, N .,Fu, TM .,Cao, JJ .,Lee, SC .,Huang, XF .,...&Lam, YF .(2013).Sources of secondary organic aerosols in the Pearl River Delta region in fall: Contributions from the aqueous reactive uptake of dicarbonyls.ATMOSPHERIC ENVIRONMENT,76(SI),200-207.
MLA Li, N ,et al."Sources of secondary organic aerosols in the Pearl River Delta region in fall: Contributions from the aqueous reactive uptake of dicarbonyls".ATMOSPHERIC ENVIRONMENT 76.SI(2013):200-207.
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