SO2 has been proposed in solar geoengineering as a precursor of H2SO4 aerosol, a cooling agent active in the stratosphere to contrast climate change. Atmospheric ionization sources can ionize SO2 into excited states of SO2 center dot+ , which quickly reacts with trace gases in the stratosphere. In this work we explore the reaction of H2mml:mfenced close=")" open="(" separators=""D2 with SO2 center dot+ excited by tunable synchrotron radiation, leading to HSO2++H (DSO2++D ), where H contributes to O-3 depletion and OH formation. Density Functional Theory and Variational Transition State Theory have been used to investigate the dynamics of the title barrierless and exothermic reaction. The present results suggest that solar geoengineering models should test the reactivity of SO2 center dot+ with major trace gases in the stratosphere, such as H-2 since this is a relevant channel for the OH formation during the nighttime when there is not OH production by sunlight. OH oxides SO2, triggering the chemical reactions leading to H2SO4 aerosol.

The Reaction of Sulfur Dioxide Radical Cation with Hydrogen and its Relevance in Solar Geoengineering Models

Satta Mauro;Catone Daniele;Castrovilli Mattea Carmen;Bolognesi Paola;Zema Nicola;Avaldi Lorenzo
2020

Abstract

SO2 has been proposed in solar geoengineering as a precursor of H2SO4 aerosol, a cooling agent active in the stratosphere to contrast climate change. Atmospheric ionization sources can ionize SO2 into excited states of SO2 center dot+ , which quickly reacts with trace gases in the stratosphere. In this work we explore the reaction of H2mml:mfenced close=")" open="(" separators=""D2 with SO2 center dot+ excited by tunable synchrotron radiation, leading to HSO2++H (DSO2++D ), where H contributes to O-3 depletion and OH formation. Density Functional Theory and Variational Transition State Theory have been used to investigate the dynamics of the title barrierless and exothermic reaction. The present results suggest that solar geoengineering models should test the reactivity of SO2 center dot+ with major trace gases in the stratosphere, such as H-2 since this is a relevant channel for the OH formation during the nighttime when there is not OH production by sunlight. OH oxides SO2, triggering the chemical reactions leading to H2SO4 aerosol.
2020
Istituto di Struttura della Materia - ISM - Sede Roma Tor Vergata
ion-molecule reactions
rate coefficient
reaction mechanisms
synchrotron radiation
VTST
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14243/380328
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