A comprehensive observation-based multiphase chemical model analysis of sulfur dioxide oxidations in both summer and winter

Abstract

Sulfate is one of the main components of haze fine particles, and its formation mechanism remains controversial. A lack of detailed and comprehensive field data hinders the accurate evaluation of relative roles of prevailing sulfate formation pathways. Here, we analyzed the sulfate production rates using a state-of-the-art multiphase model constrained to the observed concentrations of transition metal, nitrogen dioxide, ozone, hydrogen peroxide and other important parameters in winter and summer in the North China Plain. Our results showed that aqueous transition metal ion (TMI)-catalyzed oxidation was the most important pathway followed by the surface oxidation of Mn in both winter and summer while the hydroxyl and Criegee radical oxidations contribute significantly in summer. In addition, we also modeled the published cases for the fog and cloud conditions. It is found that nitrogen dioxide oxidation is the dominant pathway for the fog in a higher pH range while hydroperoxide and ozone oxidations dominated for the cloud.