Title :

ONIOM QM/MM investigation of the iodide oxidation by ozone on particle

Author(s) :

Roose, Antoine [Auteur]
Laboratory of Environmental Chemistry [Villigen] [LUC]
Physico-Chimie Moléculaire Théorique [PCMT]
Finkenzeller, Henning [Auteur]
Department of Chemistry and Biochemistry [Boulder]
Réal, Florent [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Vallet, Valérie [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Toubin, Céline [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Gyrin, Severin [Auteur]
Laboratory of Environmental Chemistry [Villigen] [LUC]
Institute for Atmospheric and Climate Science [Zürich] [IAC]
Lezzi, Lucia [Auteur]
Laboratory of Environmental Chemistry [Villigen] [LUC]
Institute for Atmospheric and Climate Science [Zürich] [IAC]
Volkamer, Rainer [Auteur]
Department of Chemistry and Biochemistry [Boulder]
Institute for Atmospheric and Climate Science [Zürich] [IAC]
Ammann, Markus [Auteur]
Laboratory of Environmental Chemistry [Villigen] [LUC]

Conference title :

A Molecular Level Understanding of Atmospheric Aerosols (MUOAA 2022)

City :

Los Angeles

Country :

Etats-Unis d'Amérique

Start date of the conference :

2022-05-15

Publication date :

2022-05-15

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

Recently, Koenig et al. [1] measured both gas phase iodine species and particulate iodine (iodate and iodide) in the lower stratosphere indicating that tropospheric multiphase redox reactions prevent poorly soluble gaseous ...
Show more >Recently, Koenig et al. [1] measured both gas phase iodine species and particulate iodine (iodate and iodide) in the lower stratosphere indicating that tropospheric multiphase redox reactions prevent poorly soluble gaseous iodine species from removal by wet deposition leading to injections of inorganic iodine into the lower stratosphere. This may influence stratospheric ozone depletion both indirectly through activation of iodide to molecular halogens and directly through the aqueous phase reaction of ozone (O₃) with iodide [2]. The product of this reaction, IO^-, is reacting with I^- to I₂(g) under most circumstances. Sakamoto et al. [3] have suggested that in addition IO(g), may be formed. The primary reaction of iodide with O₃ depends on pH. Solute strength effects and the extent of a surface reaction have not been sufficiently established [3,4]. <br><br>An hybrid ONIOM QM/MM method [5] has been used to investigate the reactivity of ozone on a iodide-containing slab of water. The reaction pathway has been determined both at interface and in bulk phase. Both singlet and triplet state surface are investigated as the triplet state can be reached through photoexcitation of ozone or by spin state change along the reaction coordinate. These theoretical calculations provide insight into the uptake process at the molecular scale. Comparisons with experimental measurements performed using a trough reactor [6] coupled to Cavity Enhanced – Differential Optical Absorption Spectroscopy (CE-DOAS) [7,8] are also discussed.<br><br><b>References</b><br>[1] T. K. Koenig et al., PNAS, <b>117</b>, 4 (2020). <br>[2] L. J. Carpenter et al., Nat. Geosci., <b>6</b>, 108-111 (2013).<br>[3] Y. Sakamoto et al., J. Phys. Chem. A, <b>113</b>, 27 (2009).<br>[4] C. Moreno et al., Phys. Chem. Chem. Phys. <b>22</b>, 5625-5637 (2020). <br>[5] L. W. Chung et al., Chem. Rev., <b>115</b>, 12 (2015). <br>[6] L. Artiglia et al., Nat. Commun., <b>8</b>, 700 (2017).<br>[7] M. Wang et al., Atmos. Meas. Tech., <b>14</b>, 4187-4202 (2021).<br>[8] R. Thalman and R. Volkamer, Atmos. Meas. Tech., <b>3</b>, 2681-2721 (2010).<br>Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

ULNE
Physiques et Chimie de l'Environnement Atmosphérique

Collections :

• Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL