Abstract

Abstract. Severe air pollution in Asia is often the consequence of a combination of large anthropogenic emissions and adverse synoptic conditions. However, limited studies on aerosols have been conducted under high emission intensity and under unique geographical and meteorological conditions. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) and other state-of-the-art instruments were utilized at a suburban site, Ziyang, in the Sichuan Basin during December 2012 to January 2013. The chemical compositions of atmospheric submicron aerosols (PM1) were determined, the sources of organic aerosols (OA) were apportioned, and the aerosol secondary formation and aging process were explored as well. Due to high humidity and static air, PM1 maintained a relatively stable level during the whole campaign, with the mean concentration of 59.7 ± 24.1 µg m−3. OA was the most abundant component (36 %) in PM1, characterized by a relatively high oxidation state. Positive matrix factorization analysis was applied to the high-resolution organic mass spectral matrix, which deconvolved OA mass spectra into four factors: low-volatility (LV-OOA) and semivolatile oxygenated OA (SV-OOA), biomass burning (BBOA) and hydrocarbon-like OA (HOA). OOA (sum of LV-OOA and SV-OOA) dominated OA as high as 71 %. In total, secondary inorganic and organic formation contributed 76 % of PM1. Secondary inorganic species correlated well (Pearson r = 0.415–0.555, p < 0.01) with relative humidity (RH), suggesting the humid air can favor the formation of secondary inorganic aerosols. As the photochemical age of OA increased with higher oxidation state, secondary organic aerosol formation contributed more to OA. The slope of OOA against Ox( = O3+NO2) steepened with the increase of RH, implying that, besides the photochemical transformation, the aqueous-phase oxidation was also an important pathway of the OOA formation. Primary emissions, especially biomass burning, resulted in high concentration and proportion of black carbon (BC) in PM1. During the episode obviously influenced by primary emissions, the contributions of BBOA to OA (26 %) and PM1 (11 %) were much higher than those (10–17 %, 4–7 %) in the clean and other polluted episodes, highlighting the significant influence of biomass burning.

Highlights

  • With its dense population and rapid economic development in the past decades, the Sichuan Basin suffers from serious fine particle pollution and has become one of the most polluted regions in China (Chen and Xie, 2012)

  • The mass spectrum (MS) of BBOA resolved in this study showed good correlation with the average MS of BBOA in previous studies (Table S2)

  • We investigated the chemical compositions of atmospheric submicron aerosols with a HR-ToF-AMS at a suburban site, Ziyang, located in the Sichuan Basin, China, during the wintertime from December 2012 to January 2013

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Summary

Introduction

With its dense population and rapid economic development in the past decades, the Sichuan Basin suffers from serious fine particle pollution and has become one of the most polluted regions in China (Chen and Xie, 2012). High emissions of gaseous and particulate pollutants, such as volatile organic compounds (VOCs), SO2, organic carbon (OC), black carbon (BC) and fine particles (PM2.5), are found in the Sichuan Basin over China (He, 2012). Influenced by the particular topographic condition, the Sichuan Basin is within the region of the lowest wind speed and relatively high humidity over China all year round (Chen and Xie, 2013; Yang et al, 2011). The unique geographical and meteorological conditions in the region favor the accumulation of local and regional atmospheric pollutants (Yang et al, 2011), making environmental threats in Sichuan more severe

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