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The Reaction of Sulfur Dioxide Radical Cation with Hydrogen and its Relevance in Solar Geoengineering Models
Authors:Dr. Mauro Satta  Dr. Antonella Cartoni  Dr. Daniele Catone  Dr. Mattea Carmen Castrovilli  Dr. Paola Bolognesi  Dr. Nicola Zema  Dr. Lorenzo Avaldi
Affiliation:1. ISMN (CNR) c/o Dipartimento di Chimica Sapienza Universita' di Roma, Pl.e Aldo Moro 5, Roma, Italy;2. Dipartimento di Chimica, Sapienza Universitá di Roma, Pl.e Aldo Moro 5, Roma, Italy;3. CNR-ISM, Area della Ricerca di Tor Vergata, Via del Fosso del Cavaliere, Roma, Italy;4. CNR-ISM, Area della Ricerca di Roma 1, Via Salaria Km 29,300, Monterotondo Scalo (RM), Italy
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 urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0001 , which quickly reacts with trace gases in the stratosphere. In this work we explore the reaction of urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0002 with urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0003 excited by tunable synchrotron radiation, leading to urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0004 (urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0005 ), where H contributes to O3 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 urn:x-wiley:14394235:media:cphc202000194:cphc202000194-math-0006 with major trace gases in the stratosphere, such as H2 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.
Keywords:ion-molecule reactions  rate coefficient  reaction mechanisms  synchrotron radiation  VTST
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