Hydrogen peroxide serves as pivotal fountainhead for aerosol aqueous sulfate formation from a global perspective
Jie Gao, Haoqi Wang, Wenqi Liu, Xu Han, Yuting Wei, Xiao Tian, Yinchang Feng, Shaojie Song, Guoliang Shi
Abstract
Abstract Traditional atmospheric chemistry posits that sulfur dioxide (SO 2 ) can be oxidized to sulfate (SO 4 2– ) through aqueous-phase reactions in clouds and gas-phase oxidation. Despite adequate knowledge of traditional mechanisms, several studies have highlighted the potential for SO 2 oxidation within aerosol water. Given the widespread presence of tropospheric aerosols, SO 4 2− production through aqueous-phase oxidation in aerosol water could have a pervasive global impact. Here, we quantify the potential contributions of aerosol aqueous pathways to global sulfate formation based on the GEOS-Chem simulations and subsequent theoretical calculations. Hydrogen peroxide (H 2 O 2 ) oxidation significantly influences continental regions both horizontally and vertically. Over the past two decades, shifts in the formation pathways within typical cities reveal an intriguing trend: despite reductions in SO 2 emissions, the increased atmospheric oxidation capacities, like rising H 2 O 2 levels, prevent a steady decline in SO 4 2− concentrations. Abating oxidants would facilitate the benefit of SO 2 reduction and the positive feedback in sulfate mitigation.