1State Key Joint Laboratory of Environmental Simulation and Pollution Control, College of Environmental Sciences and Engineering, Peking University, Beijing, China
2Research Center for Advanced Science and Technology, University of Tokyo, Tokyo, Japan
3Institute of Low Temperature Science, Hokkaido University, Sapporo, Japan
4Research Institute of Chemical Defence, Beijing, China
5Air Quality Research Center, University of California, Davis, California, USA
Received: 19 Dec 2010 – Published in Atmos. Chem. Phys. Discuss.: 19 Jan 2011
Abstract. Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m−3 and 13.5 ± 8.7 μg m−3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300–700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and oxygenated aerosol. The origin of HOA and OOA (the sum of LV-OOA and SV-OOA) has been further confirmed by the statistics that primary organic carbon (POC) and secondary organic carbon (SOC), estimated by the EC tracer method, were closely correlated with HOA and OOA, respectively. The results of the EC tracer method and of the PMF model revealed that primary organic aerosol (POA) constituted ~34–47 % of OA mass and secondary organic aerosol (SOA) constituted ~53–66 % of regional organic aerosol in PRD during summer season. The presence of abundant SOA was consistent with water soluble organic carbon (WSOC) results (accounting for ~60 % of OC on average) by Miyazaki et al. (2009) for the same campaign. OOA correlated well with WSOC at the BG site, indicating that most OOA were water soluble. More specifically, approximately 86 % of LV-OOA and 61 % of SV-OOA were estimated as water soluble species on the basis of carbon content comparison.
Revised: 08 Jun 2011 – Accepted: 20 Jun 2011 – Published: 18 Jul 2011
Citation: Xiao, R., Takegawa, N., Zheng, M., Kondo, Y., Miyazaki, Y., Miyakawa, T., Hu, M., Shao, M., Zeng, L., Gong, Y., Lu, K., Deng, Z., Zhao, Y., and Zhang, Y. H.: Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign, Atmos. Chem. Phys., 11, 6911-6929, doi:10.5194/acp-11-6911-2011, 2011.