Insights into the chemistry of aerosol growth in Beijing: Implication of fine particle episode formation during wintertime

摘要

Nucleation particle growth plays a major role in the occurrence of fine particles, yet the mechanism of new particle formation (NPF) remains ambiguous in the complex atmosphere of megacities and hinders the development of measures to mitigate PM2.5 pollution. In this study, the chemistry of ultrafine particles during the growth phase of nucleation events was investigated in urban Beijing from Nov. 15, 2018 to Jan. 15, 2019, using two scanning mobility particle spectrometers (SMPS) systems and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). During this intense campaign, 11 NPF events were observed and the growth rate (GR) of nanoparticles ranged from 12.5 to 24.5 nm h(-1). Four periodic cycles of PM2.5 episodes that included aerosol particle growth to particulate matter pollution were identified. Based on the Q(GR) - Q(AMS) theoretical frame that exploring the balance between the source rate of condensable vapors and the observed growth rate of nanoparticles, we clearly showed the physical and chemical evolution of nano-particle during the growth processes to ambient-atmosphere sizes (100 nm). Generally, the modal diameter of aerosol particles grew by more than 100 nm (7 out of 11 NPF events) when the nitrate concentration and less-oxidized oxygenated organic aerosol (LO-OOA) were high; however, another class of aerosol particle growth was limited to 50-100 nm (3 out of 11 NPF events) when sulfate was high. Note that the remaining one NPF event could not be identified if it can grow up to 100 nm or not due to the unavailable of observation data during the late growth stage. By linking the aerosol growth with chemical compositions, sulfate and organics were found to be the main contributors during the initial stage of the aerosol growth, while cooking-related OA (COA) enhanced the transition stage, and nitrate and more-oxidized OOA (MO-OOA) dominated the subsequent growth of aerosol to ambient-atmosphere sizes. An important portion of aerosol growth in PM2.5 was controlled by semi-volatile organic vapors, which can partition into the externally condensed phase of the accumulation mode and coarse mode via the physical process of adsorption. Through quantifying the physical and chemical properties of aerosol particle growth, the detail processes of nucleation initiated PM2.5 pollution episodes were evaluated and provided observational evidence on the formation mechanism of winter haze pollution in the megacity of Beijing. (C) 2021 Elsevier Ltd. All rights reserved.