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Direct observation of the complex S(IV) equilibria at the liquid-vapor interface
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Journal Article
Direct observation of the complex S(IV) equilibria at the liquid-vapor interface
2024
Overview
The multi-phase oxidation of S(IV) plays a crucial role in the atmosphere, leading to the formation of haze and severe pollution episodes. We here contribute to its understanding on a molecular level by reporting experimentally determined p
K
a
values of the various S(IV) tautomers and reaction barriers for SO
2
formation pathways. Complementary state-of-the-art molecular-dynamics simulations reveal a depletion of bisulfite at low pH at the liquid-vapor interface, resulting in a different tautomer ratio at the interface compared to the bulk. On a molecular-scale level, we explain this with the formation of a stable contact ion pair between sulfonate and hydronium ions, and with the higher energetic barrier for the dehydration of sulfonic acid at the liquid-vapor interface. Our findings highlight the contrasting physicochemical behavior of interfacial versus bulk environments, where the pH dependence of the tautomer ratio reported here has a significant impact on both SO
2
uptake kinetics and reactions involving NO
x
and H
2
O
2
at aqueous aerosol interfaces.
The complex equilibria of sulfur compounds at the liquid-vapor interface play key roles in atmospheric processes. Here, using X-ray photoelectron spectroscopy, Raman spectroscopy, and molecular dynamics simulations the authors determining pKa values and tautomer ratios at the air-vapor interface in a liquid microjet.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
