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Reaction of SO3 with H2SO4 and Its Implication for Aerosol Particle Formation in the Gas Phase and at the Air-Water Interface.
- Source :
- EGUsphere; 10/13/2023, p1-31, 31p
- Publication Year :
- 2023
-
Abstract
- The reactions between SO<subscript>3</subscript> and atmospheric acids are indispensable in improving the formation of aerosol particle. However, relative to those of SO<subscript>3</subscript> with organic acids, the reaction of SO<subscript>3</subscript> with inorganic acids has not received much attention. Here, we explore the atmospheric reaction between SO<subscript>3</subscript> and H<subscript>2</subscript>SO<subscript>4</subscript>, a typical inorganic acid, in the gas phase and at the air-water interface by using quantum chemical (QC) calculations and Born-Oppenheimer molecular dynamics simulations. We also report the effect of H<subscript>2</subscript>S<subscript>2</subscript>O<subscript>7</subscript>, the product of the reaction between SO<subscript>3</subscript> and H<subscript>2</subscript>SO<subscript>4</subscript>, on new particle formation (NPF) in various environments by using the Atmospheric Cluster Dynamics Code kinetic model and the QC calculation. The present findings show that the gas phase reactions of SO<subscript>3</subscript> + H<subscript>2</subscript>SO<subscript>4</subscript> without and with water molecule are both low energy barrier processes. With the involvement of interfacial water molecules, H<subscript>2</subscript>O-induced the formation of S<subscript>2</subscript>O<subscript>7</subscript><superscript>2-</superscript>⋅⋅⋅H<subscript>3</subscript>O<superscript>+</superscript> ion pair, HSO<subscript>4</subscript><superscript>-</superscript> mediated the formation of HSO<subscript>4</subscript><superscript>-</superscript>⋅⋅⋅H<subscript>3</subscript>O<superscript>+</superscript> ion pair and the deprotonation of H<subscript>2</subscript>S<subscript>2</subscript>O<subscript>7</subscript> were observed and proceeded on the picosecond time-scale. The present findings suggest the potential contribution of SO<subscript>3</subscript>-H<subscript>2</subscript>SO<subscript>4</subscript> reaction to NPF and aerosol particle growth as the facts that i) H<subscript>2</subscript>S<subscript>2</subscript>O<subscript>7</subscript> can directly participate in H<subscript>2</subscript>SO<subscript>4</subscript>-NH<subscript>3</subscript>-based cluster formation and can facilitate the fastest possible rate of NPF from H<subscript>2</subscript>SO<subscript>4</subscript>-NH<subscript>3</subscript>-based clusters by about a factor of 6.92 orders of magnitude at 278.15 K; and ii) the formed interfacial S<subscript>2</subscript>O<subscript>7</subscript><superscript>2-</superscript> can attract candidate species from the gas phase to the water surface, and thus, accelerate particle growth. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- Database :
- Complementary Index
- Journal :
- EGUsphere
- Publication Type :
- Academic Journal
- Accession number :
- 172989814
- Full Text :
- https://doi.org/10.5194/egusphere-2023-2009