A review on the heterogeneous oxidation of SO2 on solid atmospheric particles: Implications for sulfate formation in haze chemistry

Abstract

The oxidation of sulfur dioxide (SO2) to sulfate in the atmosphere is an important concern in regional air quality, global climate change, and human health. While gas-phase and liquid-phase oxidation of SO2 are widely regarded as important sources of sulfate, the contribution of the heterogeneous oxidation process on particle surfaces is controversial. Recently, this heterogeneous chemistry has been considered to be an important mechanism that is missing in current models to explain sulfate concentrations observed in haze episodes in East Asia. Therefore, the heterogeneous oxidation of SO2 on particles under the conditions of complex air pollution needs to be reassessed. This review summarizes the fundamental understanding of the heterogeneous reactions of SO2 on solid particles such as mineral dust, black carbon, sea salts, organic aerosol, and so on. The factors affecting the mechanism and kinetics of the heterogeneous reactions of SO2, including coexisting components (O3, NO2, H2O2, NH3, and VOCs), reactive sites, surface properties, relative humidity, and illumination, are reviewed. Reactive oxygen species involved in the heterogeneous oxidation of SO2 on particles are discussed. To our knowledge, while previous reviews have appeared on the oxidation of SO2 in the aqueous-phase, this is the first review on the atmospheric heterogeneous reactions of SO2 on the surface of solid particles, which can be of help in understanding the sulfur cycle in the atmosphere and its environmental impacts. A number of recommendations for future research are also presented.