Abstract

Secondary organic aerosol (SOA) plays a key role in air pollution and global climate change. However, the understanding and modelling of SOA properties and evolution are still limited. In this paper, we developed a novel kinetic Core-Shell box model for Viscosity dependent SOA simulation (CSVA), which includes explicit gas-phase reactions (MCM), homogeneous nucleation by H2SO4-NH3-H2O, viscosity dependent mass transfer between gas and particle phases (organic and aqueous phases) and particle-phase reactions. The gas-particle mass transfer is represented by chainlike reactions analogizing to electrical resistance. The CSVA model is verified and applied to chamber experiments of toluene oxidation systems. The monomers and dimers of SOA are determined by coupling the high-resolution Orbitrap mass spectra and MCM mechanism. The majority of dimers are confirmed to be peroxyhemiacetals formed by reactions of hydroperoxides with aldehydes in the particle phase. The results show that CSVA can well capture the following processes: (1) relative humidity (RH) dependent nucleation of the H2SO4-NH3-H2O system, (2) particle size-dependent hygroscopic growth of inorganics (e.g., NaCl and (NH4)2SO4) and organics (levoglucosan and SOA), (3) NOx dependent SOA formation, (4) viscosity-induced evolution of particle size distribution, and (5) effect of RH on SOA formation. In particular, our model reproduces the phenomenon that the evolution of SOA particle size distribution from a one-peak mode into a two-peak mode is due to viscosity.

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