Gas-Phase Molecular Halogen Formation from NaCl and NaBr Aerosols:When Are Interface Reactions Important?

摘要

Unique interface reactions at the surface of sea-salt particles have been suggested as an important source of photolyzable gas-phase halogen species in the troposphere.Many factors influence the relative importance of interface chemistry compared to aqueous-phase chemistry.The Model of Aerosol,Gas,and Interfacial Chemistry(MAGIC 2.0)is used to study the influence of interface reactions on gas-phase molecular halogen production from pure NaCl and NaBr aerosols.The main focus is to identify the relative importance of bulk compared to interface chemistry and to determine when interface chemistry dominates.Results show that the interface process involving Cl_(surf)~-and OH_(g)is the main source of Cl_(2(g)).For the analogous oxidation of bromide by OH,gaseous Br_2 is formed mainly in the bulk aqueous phase and transferred across the interface.However,the reaction of Br_(surf)~-with O_(3(g))at the interface is the primary source of Br_(2(g))under dark conditions.The effect of aerosol size is also studied.Potential atmospheric implications and effects of interface processes on aerosol pH are discussed.