Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol

Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol

Effect of H<sub>2</sub>O and NH<sub>3</sub> on the synergistic oxidation reaction of SO<sub>2</sub> and NO<sub>2</sub> is investigated by theoretical calculation using the molecule system SO<sub>2</sub>-2NO<sub>2</sub>-nH<sub...

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Main Authors: Zehua Wang, Chenxi Zhang, Guochun Lv, Xiaomin Sun, Ning Wang, Zhiqiang Li
Format: Article
Language:English
Published: MDPI AG 2019-07-01
Series:International Journal of Molecular Sciences
Subjects:
sulfuric acid
sulfur dioxide
nitrogen dioxide
synergistic oxidation
hydrolysis reaction
Online Access:https://www.mdpi.com/1422-0067/20/15/3746
id doaj-3ffd95a82ea8487bb7df999d9a13c670
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spelling doaj-3ffd95a82ea8487bb7df999d9a13c6702020-11-24T21:21:02ZengMDPI AGInternational Journal of Molecular Sciences1422-00672019-07-012015374610.3390/ijms20153746ijms20153746Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate AerosolZehua Wang0Chenxi Zhang1Guochun Lv2Xiaomin Sun3Ning Wang4Zhiqiang Li5Environment Research Institute, Shandong University, Jinan 250100, ChinaCollege of Biological and Environmental Engineering, Binzhou University, Binzhou 256600, ChinaEnvironment Research Institute, Shandong University, Jinan 250100, ChinaEnvironment Research Institute, Shandong University, Jinan 250100, ChinaEnvironment Research Institute, Shandong University, Jinan 250100, ChinaCenter for Optics Research and Engineering (CORE), Shandong University, Qingdao 266237, ChinaEffect of H<sub>2</sub>O and NH<sub>3</sub> on the synergistic oxidation reaction of SO<sub>2</sub> and NO<sub>2</sub> is investigated by theoretical calculation using the molecule system SO<sub>2</sub>-2NO<sub>2</sub>-nH<sub>2</sub>O (<i>n</i> = 0, 1, 2, 3) and SO<sub>2</sub>-2NO<sub>2</sub>-nH<sub>2</sub>O-mNH<sub>3</sub> (<i>n</i> = 0, 1, 2; <i>m</i> = 1, 2). Calculated results show that SO<sub>2</sub> is oxidized to SO<sub>3</sub> by N<sub>2</sub>O<sub>4</sub> intermediate. The additional H<sub>2</sub>O in the systems can reduce the energy barrier of oxidation step. The increasing number of H<sub>2</sub>O molecules in the systems enhances the effect and promotes the production of HONO. When the proportion of H<sub>2</sub>O to NH<sub>3</sub> is 1:1, with NH<sub>3</sub> included in the system, the energy barrier is lower than two pure H<sub>2</sub>O molecules in the oxidation step. The present study indicates that the H<sub>2</sub>O and NH<sub>3</sub> have thermodynamic effects on promoting the oxidation reaction of SO<sub>2</sub> and NO<sub>2</sub>, and NH<sub>3</sub> has a more significant role in stabilizing product complexes. In these hydrolysis reactions, nethermost barrier energy (0.29 kcal/mol) can be found in the system SO<sub>2</sub>-2NO<sub>2</sub>-H<sub>2</sub>O. It is obvious that the production of HONO is energetically favorable. A new reaction mechanism about SO<sub>2</sub> oxidation in the atmosphere is proposed, which can provide guidance for the further study of aerosol surface reactions.https://www.mdpi.com/1422-0067/20/15/3746sulfuric acidsulfur dioxidenitrogen dioxidesynergistic oxidationhydrolysis reaction
collection DOAJ
language English
format Article
sources DOAJ
author Zehua Wang
Chenxi Zhang
Guochun Lv
Xiaomin Sun
Ning Wang
Zhiqiang Li
spellingShingle Zehua Wang
Chenxi Zhang
Guochun Lv
Xiaomin Sun
Ning Wang
Zhiqiang Li
Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
International Journal of Molecular Sciences
sulfuric acid
sulfur dioxide
nitrogen dioxide
synergistic oxidation
hydrolysis reaction
author_facet Zehua Wang
Chenxi Zhang
Guochun Lv
Xiaomin Sun
Ning Wang
Zhiqiang Li
author_sort Zehua Wang
title Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
title_short Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
title_full Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
title_fullStr Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
title_full_unstemmed Synergistic Reaction of SO<sub>2</sub> with NO<sub>2</sub> in Presence of H<sub>2</sub>O and NH<sub>3</sub>: A Potential Source of Sulfate Aerosol
title_sort synergistic reaction of so<sub>2</sub> with no<sub>2</sub> in presence of h<sub>2</sub>o and nh<sub>3</sub>: a potential source of sulfate aerosol
publisher MDPI AG
series International Journal of Molecular Sciences
issn 1422-0067
publishDate 2019-07-01
description Effect of H<sub>2</sub>O and NH<sub>3</sub> on the synergistic oxidation reaction of SO<sub>2</sub> and NO<sub>2</sub> is investigated by theoretical calculation using the molecule system SO<sub>2</sub>-2NO<sub>2</sub>-nH<sub>2</sub>O (<i>n</i> = 0, 1, 2, 3) and SO<sub>2</sub>-2NO<sub>2</sub>-nH<sub>2</sub>O-mNH<sub>3</sub> (<i>n</i> = 0, 1, 2; <i>m</i> = 1, 2). Calculated results show that SO<sub>2</sub> is oxidized to SO<sub>3</sub> by N<sub>2</sub>O<sub>4</sub> intermediate. The additional H<sub>2</sub>O in the systems can reduce the energy barrier of oxidation step. The increasing number of H<sub>2</sub>O molecules in the systems enhances the effect and promotes the production of HONO. When the proportion of H<sub>2</sub>O to NH<sub>3</sub> is 1:1, with NH<sub>3</sub> included in the system, the energy barrier is lower than two pure H<sub>2</sub>O molecules in the oxidation step. The present study indicates that the H<sub>2</sub>O and NH<sub>3</sub> have thermodynamic effects on promoting the oxidation reaction of SO<sub>2</sub> and NO<sub>2</sub>, and NH<sub>3</sub> has a more significant role in stabilizing product complexes. In these hydrolysis reactions, nethermost barrier energy (0.29 kcal/mol) can be found in the system SO<sub>2</sub>-2NO<sub>2</sub>-H<sub>2</sub>O. It is obvious that the production of HONO is energetically favorable. A new reaction mechanism about SO<sub>2</sub> oxidation in the atmosphere is proposed, which can provide guidance for the further study of aerosol surface reactions.
topic sulfuric acid
sulfur dioxide
nitrogen dioxide
synergistic oxidation
hydrolysis reaction
url https://www.mdpi.com/1422-0067/20/15/3746
work_keys_str_mv AT zehuawang synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
AT chenxizhang synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
AT guochunlv synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
AT xiaominsun synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
AT ningwang synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
AT zhiqiangli synergisticreactionofsosub2subwithnosub2subinpresenceofhsub2suboandnhsub3subapotentialsourceofsulfateaerosol
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