Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles

Atmospheric sulfate aerosols have important impacts on air quality, climate, and human and ecosystem health. However, current air-quality models generally underestimate the rate of conversion of sulfur dioxide (SO₂) to sulfate during severe haze pollution events, indicating that our understanding of sulfate formation chemistry is incomplete. This may arise because the air-quality models rely upon kinetics studies of SO₂ oxidation conducted in dilute aqueous solutions, and not at the high solute strengths of atmospheric aerosol particles. Here, we utilize an aerosol flow reactor to perform direct investigation on the kinetics of aqueous oxidation of dissolved SO₂ by hydrogen peroxide (H₂O₂) using pH-buffered, submicrometer, deliquesced aerosol particles at relative humidity of 73 to 90%. We find that the high solute strength of the aerosol particles significantly enhances the sulfate formation rate for the H₂O₂ oxidation pathway compared to the dilute solution. By taking these effects into account, our results indicate that the oxidation of SO₂ by H₂O₂ in the liquid water present in atmospheric aerosol particles can contribute to the missing sulfate source during severe haze episodes.