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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2018, 140, 35, 11020-11028
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Self-Catalytic Reaction of SO3 and NH3 To Produce Sulfamic Acid and Its Implication to Atmospheric Particle Formation

  • Hao Li
    Hao Li
    Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China
    Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588, United States
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    • , 
  • Jie Zhong
    Jie Zhong
    Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588, United States
    More by Jie Zhong
    • , 
  • Hanna Vehkamäki
    Hanna Vehkamäki
    Institute for Atmospheric and Earth System Research/Physics, University of Helsinki, PO Box 64 (Gustaf Hällströmin katu 2a), FI-00014 Helsinki, Finland
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    • , 
  • Theo Kurtén
    Theo Kurtén
    Institute for Atmospheric and Earth System Research/Chemistry, University of Helsinki, PO Box 64 (Gustaf Hällströmin katu 2a), FI-00014 Helsinki, Finland
    More by Theo Kurtén
    Orcidhttp://orcid.org/0000-0002-6416-4931
    • , 
  • Weigang Wang
    Weigang Wang
    Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, 100190 Beijing, China
    More by Weigang Wang
    • , 
  • Maofa Ge
    Maofa Ge
    Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, 100190 Beijing, China
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    Orcidhttp://orcid.org/0000-0002-1771-9359
    • , 
  • Shaowen Zhang
    Shaowen Zhang
    Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China
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    • , 
  • Zesheng Li
    Zesheng Li
    Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China
    More by Zesheng Li
    Orcidhttp://orcid.org/0000-0002-6993-8414
    • , 
  • Xiuhui Zhang*
    Xiuhui Zhang
    Key Laboratory of Cluster Science, Ministry of Education of China, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, P. R. China
    *E-mail: [email protected]
    More by Xiuhui Zhang
    Orcidhttp://orcid.org/0000-0001-9570-7882
    • , 
  • Joseph S. Francisco*
    Joseph S. Francisco
    Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588, United States
    *E-mail: [email protected]
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    Orcidhttp://orcid.org/0000-0002-5461-1486
    • , and 
  • Xiao Cheng Zeng*
    Xiao Cheng Zeng
    Department of Chemistry, University of Nebraska-Lincoln, Lincoln, Nebraska 68588, United States
    Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing 100029, China
    *E-mail: [email protected]
    More by Xiao Cheng Zeng
    Orcidhttp://orcid.org/0000-0003-4672-8585
Cite this: J. Am. Chem. Soc. 2018, 140, 35, 11020–11028
Publication Date (Web):August 8, 2018
https://doi.org/10.1021/jacs.8b04928
Copyright © 2018 American Chemical Society
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Abstract

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Sulfur trioxide (SO3) is one of the most active chemical species in the atmosphere, and its atmospheric fate has profound implications to air quality and human health. The dominant gas-phase loss pathway for SO3 is generally believed to be the reaction with water molecules, resulting in sulfuric acid. The latter is viewed as a critical component in the new particle formation (NPF). Herein, a new and competitive loss pathway for SO3 in the presence of abundant gas-phase ammonia (NH3) species is identified. Specifically, the reaction between SO3 and NH3, which produces sulfamic acid, can be self-catalyzed by the reactant (NH3). In dry and heavily polluted areas with relatively high concentrations of NH3, the effective rate constant for the bimolecular SO3–NH3 reaction can be sufficiently fast through this new loss pathway for SO3 to become competitive with the conventional loss pathway for SO3 with water. Furthermore, this study shows that the final product of the reaction, namely, sulfamic acid, can enhance the fastest possible rate of NPF from sulfuric acid and dimethylamine (DMA) by about a factor of 2. An alternative source of stabilizer for acid–base clustering in the atmosphere is suggested, and this new mechanism for NPF has potential to improve atmospheric modeling in highly polluted regions.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b04928.

  • Formation Gibbs free energies and the sum of evaporation rates of the clusters; imaginary frequencies of the transition states and the Wigner tunneling correction factor of the reactions; possible concentration of SFA in the experiment and in the real atmosphere; ratio of reaction rate for SO3 + NH3 reaction and SO3 + H2O reaction under different [NH3] and [H2O]; formation Gibbs free energies and a sum of evaporation rates of the clusters containing SFA, SA DMA, and NH3; enhancement strength of SFA; ratio of cluster formation rates as a function of the logarithm of [SA] and [DMA]; optimized geometries of key species involved in particle formation in gas-phase; ratio of cluster formation rates versus the logarithm of [DMA] (PDF)

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This article is cited by 35 publications.

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