Secondary aerosol formation drives atmospheric particulate matter pollution over megacities (Beijing and Seoul) in East Asia

Abstract

Atmospheric particulate matter (PM) pollution in Beijing and Seoul is an urgent concern because of the dense population and the role of the capital city. This study aimed to understand haze formation over East Asia during winter by simultaneously measuring the in situ aerosol chemical composition in the two megacities. During the sampling period, a similar pollution situation characterized by extremely low SO2 (approximately 1 ppbv) and high NOx (approximately 20 ppbv) concentrations and secondary inorganic aerosol (SIA)-dominated PM was found in both cities. Nitrate dominated the inorganic components in the submicron particles in both cities and was more pronounced in Seoul than in Beijing. The enhanced SIA mass concentrations during pollution episodes were observed to be associated with an increased local atmospheric oxidation capacity (indicated by O3+NO2=Ox concentration) and ambient relative humidity under similar stagnant weather conditions. Regarding the thermodynamic equilibrium, abundant aerosol liquid water promoted the partitioning of gaseous HNO3 into its particle phase when pollution events occurred. This result emphasized the importance of local secondary aerosol formation for atmospheric PM pollution in East Asian megacities. The box model simulation of nitrate formation indicated that the homogeneous oxidation of NO2 by OH radicals was the major nitrate formation pathway in both megacities. The downward transport of nitrate from the residual layer also significantly contributed to nitrate concentrations. NOx and volatile organic compounds (VOCs) exhibited a non-linear relationship with nitrate formation. Reducing VOCs concentrations was an efficient approach to mitigate nitrate in both megacities. A reduction of more than 50% in NOx concentrations was required for the effective reduction of nitrate. This study highlighted that Beijing and Seoul were experiencing similar PM pollution situations, and nitrate reduction should be considered to improve their air quality. © 2023 Elsevier Ltd