Exploring the chemical fate of the sulfate radical anion by reaction with sulfur dioxide in the gas phase
Item
Title (Dublin Core)
Exploring the chemical fate of the sulfate radical anion by reaction with sulfur dioxide in the gas phase
Description (Dublin Core)
The gas phase reaction between SO<sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> and SO<sub>2</sub>, <i>n</i> = 0–2, is investigated using ab initio calculations and kinetic modelling. Structures of reactants, transition states and products are reported. Our calculations predict that the SO<sub>2</sub>SO</sub><sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> cluster ion, which is formed upon SO<sub>2</sub> and SO<sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> collision, can isomerize to SO<sub>3</sub>SO<sub>3</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub>. The overall reaction is SO<sub>2</sub> oxidation by the SO<sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> anionic cluster. The results show that SO<sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> is a good SO<sub>2</sub> oxidant, especially at low relative humidity, with a reaction rate constant up to 1.5 × 10<sup>−10</sup> cm<sup>3</sup> molecule<sup>−1</sup>s<sup>−1</sup>. At high relative humidity, instead, the re-evaporation of SO<sub>2</sub> from the SO<sub>2</sub>SO</sub<sub>4</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> cluster ion is favoured.
Creator (Dublin Core)
Tsona, N. T.
Bork, N.
Vehkamäki, H.
Date (Dublin Core)
2018-09-08
Type (Dublin Core)
Text
Format (Dublin Core)
application/pdf
Identifier (Dublin Core)
10.5194/acp-15-495-2015
https://acp.copernicus.org/articles/15/495/2015/
Source (Dublin Core)
eISSN: 1680-7324
Language (Dublin Core)
eng
