Surface distribution of sulfites and sulfates on natural volcanic and desert dusts: impact of humidity and chemical composition.
Résumé
The heterogeneous interaction of gas-phase species with solid surfaces is a crucial research field to understand
the chemical evolution of the atmosphere of Earth. SO2 gas is an important widely encountered gas. It was
recently evidenced that the interaction of SO2 gas with mineral dust is reactive in nature and that as a result
sulfites and sulfates are formed on the surface. However, the distribution of sulfites and sulfates on natural dust
samples and their dependence on various parameters has never been addressed.
In this work formation and loss of sulfites and sulfates as a function of time and stability of the formed species
on the surface of five Icelandic volcanic dusts and three desert dusts were investigated. In addition, the role of
surface composition and relative humidity in the formation of sulfites and sulfates was evaluated. Controlled
processing of volcanic and desert dusts with SO2 was achieved in a custom-made atmospheric pressure reactor
at the temperature of 298 K at different relative humidity (RH) values ranging from 0% to 83%. Using a
recently developed HPLC method kinetics of formation and loss of sulfur species formed on the surface of five
Icelandic volcanic dusts and three desert dusts were investigated. Our results suggest that surface composition
influences the amount of sulfites and sulfates formed on the surface under low humidity conditions (RH below
30%). Higher amounts of sulfites are positively correlated with (Fe+Ti)/Si parameter, while higher amounts of
sulfates are positively correlated to the amount of Na on the surface of dust. However, a dominant role in both
formation and distribution of sulfites and sulfates on the surface was attributed to water, as it increases the rate
of transformation of sulfites to sulfates.
This information can be used in atmospheric modeling to better evaluate the impact of dust on various
atmospheric processes such as the ability of dusts to remove SO2 gas and thus better evaluate air quality.