Abstract

Abstract. To mitigate haze pollution in China, a better understanding of the sources of carbonaceous aerosols is required due to the complexity in multiple emissions and atmospheric processes. Here we combined the analysis of radiocarbon and the stable isotope 13C to investigate the sources and formation of carbonaceous aerosols collected in two Chinese megacities (Beijing and Xi'an) during severe haze events of a “red alarm” level from December 2016 to January 2017. The haze periods with daily PM2.5 concentrations as high as ∼ 400 µg m−3 were compared to subsequent clean periods (i.e., PM2.5 less than median concentrations during the winter 2016/2017) with PM2.5 concentrations below 100 µg m−3 in Xi'an and below 20 µg m−3 in Beijing. In Xi'an, liquid fossil fuel combustion was the dominant source of elemental carbon (EC; 44 %–57 %), followed by biomass burning (25 %–29 %) and coal combustion (17 %–29 %). In Beijing, coal combustion contributed 45 %–61 % of EC, and biomass burning (17 %–24 %) and liquid fossil fuel combustion (22 %–33 %) contributed less. Non-fossil sources contributed 51 %–56 % of organic carbon (OC) in Xi'an, and fossil sources contributed 63 %–69 % of OC in Beijing. Secondary OC (SOC) was largely contributed by non-fossil sources in Xi'an (56±6 %) and by fossil sources in Beijing (75±10 %), especially during haze periods. The fossil vs. non-fossil contributions to OC and EC did not change drastically during haze events in both Xi'an and Beijing. However, compared to clean periods, the contribution of coal combustion to EC during haze periods increased in Xi'an and decreased in Beijing. During clean periods, primary OC from biomass burning and fossil sources constituted ∼ 70 % of OC in Xi'an and ∼ 53 % of OC in Beijing. From clean to haze periods, the contribution of SOC to total OC increased in Xi'an but decreased in Beijing, suggesting that the contribution of secondary organic aerosol formation to increased OC during haze periods was more efficient in Xi'an than in Beijing. In Beijing, the high SOC fraction in total OC during clean periods was mainly due to an elevated contribution from non-fossil SOC. In Xi'an, a slight day–night difference was observed during the clean period with enhanced fossil contributions to OC and EC during the day. This day–night difference was negligible during severe haze periods, likely due to the enhanced accumulation of pollutants under stagnant weather conditions.

Highlights

  • Severe haze pollution with high PM2.5 concentrations and reduced visibility occurs frequently during winter in China (An et al, 2019)

  • We investigated the sources of carbonaceous aerosols in PM2.5 in both cities during several haze periods and compared them to clean periods with PM2.5 concentrations below 100 μg m−3 in Xi’an and below 20 μg m−3 in Beijing

  • In Xi’an, even during the clean periods that we defined here, daily PM2.5 concentrations were higher than the Chinese pollution standard of 75 μg m−3, reflecting severe air quality problems

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Summary

Introduction

Severe haze pollution with high PM2.5 (i.e., particulate matter with aerodynamic diameter ≤ 2.5 μm) concentrations and reduced visibility occurs frequently during winter in China (An et al, 2019). Field measurements show that carbonaceous aerosol contributes a significant fraction of PM2.5 load-. H. Ni et al.: Different sources of carbonaceous aerosol in Beijing and Xi’an ing during severe haze events in China (Huang et al, 2014; Elser et al, 2016; Liu et al, 2016). A better understanding of the sources and atmospheric processes of carbonaceous aerosols is needed for mitigating haze pollution. Many previous studies focus solely on Beijing, the capital of China. Studies on other megacities are needed for comparison, as well as for a more comprehensive understanding of haze pollution in China

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