Abstract

Abstract. A revised Community Multi-scale Air Quality (CMAQ) model with updated secondary organic aerosol (SOA) yields and a more detailed description of SOA formation from isoprene oxidation was applied to study the spatial and temporal distribution of SOA in China in the entire year of 2013. Predicted organic carbon (OC), elemental carbon and volatile organic compounds agreed favorably with observations at several urban areas, although the high OC concentrations in wintertime in Beijing were under-predicted. Predicted summer SOA was generally higher (10–15 µg m−3) due to large contributions of isoprene (country average, 61 %), although the relative importance varies in different regions. Winter SOA was slightly lower and was mostly due to emissions of alkane and aromatic compounds (51 %). Contributions of monoterpene SOA was relatively constant (8–10 %). Overall, biogenic SOA accounted for approximately 75 % of total SOA in summer, 50–60 % in autumn and spring, and 24 % in winter. The Sichuan Basin had the highest predicted SOA concentrations in the country in all seasons, with hourly concentrations up to 50 µg m−3. Approximately half of the SOA in all seasons was due to the traditional equilibrium partitioning of semivolatile components followed by oligomerization, while the remaining SOA was mainly due to reactive surface uptake of isoprene epoxide (5–14 %), glyoxal (14–25 %) and methylglyoxal (23–28 %). Sensitivity analyses showed that formation of SOA from biogenic emissions was significantly enhanced due to anthropogenic emissions. Removing all anthropogenic emissions while keeping the biogenic emissions unchanged led to total SOA concentrations of less than 1 µg m−3, which suggests that manmade emissions facilitated biogenic SOA formation and controlling anthropogenic emissions would result in reduction of both anthropogenic and biogenic SOA.

Highlights

  • Fast economic development and rapid industrialization and urbanization in the past several decades significantly increased the level of air pollution in China and lead to higher aerosol loadings in the downwind regions

  • As ozone and a significant portion of the PM2.5 mass are formed from photochemical reactions of the precursors, the general capability of the model to reproduce these species suggests that the oxidation capability of the atmosphere and precursor concentrations essential for secondary organic aerosol (SOA) predictions were reasonably predicted – even though the SOA formation processes are much more complex and less understood

  • 5 Conclusions In China, predicted SOA concentrations are generally higher in summer (10–15 μg m−3) due to large contributions of isoprene and lower in wintertime due to emissions of alkane and aromatic compounds (51 %)

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Summary

Introduction

Fast economic development and rapid industrialization and urbanization in the past several decades significantly increased the level of air pollution in China and lead to higher aerosol loadings in the downwind regions. In order to determine the contributions of SOA to total organic carbon (OC) burden in China, receptororiented analysis with specific SOA tracers (Akagi et al, 2011), or statistical analysis with minimal elemental-carbonto-OC (EC / OC) ratio (Peng et al, 2013; Wang et al, 2015), have been attempted. Advanced techniques such as the positive matrix factorization analysis of organic aerosol data from aerosol mass spectrometers have been applied to determine the amount of SOA and its precursors (Huang et al, 2014b; Sun et al, 2014; Wang et al, 2016)

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