High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures

Jiali Shen, Wiebke Scholz, Xu Cheng He, Putian Zhou, Guillaume Marie, Mingyi Wang, Ruby Marten, Mihnea Surdu, Birte Rörup, Rima Baalbaki, Antonio Amorim, Farnoush Ataei, David M. Bell, Barbara Bertozzi, Zoé Brasseur, Lucía Caudillo, Dexian Chen, Biwu Chu, Lubna Dada, Jonathan DuplissyHenning Finkenzeller, Manuel Granzin, Roberto Guida, Martin Heinritzi, Victoria Hofbauer, Siddharth Iyer, Deniz Kemppainen, Weimeng Kong, Jordan E. Krechmer, Andreas Kürten, Houssni Lamkaddam, Chuan Ping Lee, Brandon Lopez, Naser G.A. Mahfouz, Hanna E. Manninen, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Tatjana Müller, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Pontus Roldin, Siegfried Schobesberger, Mario Simon, Dominik Stolzenburg, Yee Jun Tham, António Tomé, Nsikanabasi Silas Umo, Dongyu Wang, Yonghong Wang, Stefan K. Weber, André Welti, Robin Wollesen De Jonge, Yusheng Wu, Marcel Zauner-Wieczorek, Felix Zust, Urs Baltensperger, Joachim Curtius, Richard C. Flagan, Armin Hansel, Ottmar Möhler, Tuukka Petäjä, Rainer Volkamer, Markku Kulmala, Katrianne Lehtipalo, Matti Rissanen, Jasper Kirkby, Imad El-Haddad, Federico Bianchi, Mikko Sipilä, Neil M. Donahue, Douglas R. Worsnop

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Abstract

Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly methanesulfonic acid, MSA, and sulfuric acid, H2SO4). Despite their importance, accurate prediction of MSA and H2SO4from DMS oxidation remains challenging. With comprehensive experiments carried out in the Cosmics Leaving Outdoor Droplets (CLOUD) chamber at CERN, we show that decreasing the temperature from +25 to -10 °C enhances the gas-phase MSA production by an order of magnitude from OH-initiated DMS oxidation, while H2SO4production is modestly affected. This leads to a gas-phase H2SO4-to-MSA ratio (H2SO4/MSA) smaller than one at low temperatures, consistent with field observations in polar regions. With an updated DMS oxidation mechanism, we find that methanesulfinic acid, CH3S(O)OH, MSIA, forms large amounts of MSA. Overall, our results reveal that MSA yields are a factor of 2-10 higher than those predicted by the widely used Master Chemical Mechanism (MCMv3.3.1), and the NOxeffect is less significant than that of temperature. Our updated mechanism explains the high MSA production rates observed in field observations, especially at low temperatures, thus, substantiating the greater importance of MSA in the natural sulfur cycle and natural CCN formation. Our mechanism will improve the interpretation of present-day and historical gas-phase H2SO4/MSA measurements.

Original languageEnglish
Pages (from-to)13931-13944
Number of pages14
JournalEnvironmental Science and Technology
Volume56
Issue number19
DOIs
Publication statusPublished - 2022
Publication typeA1 Journal article-refereed

Keywords

  • dimethyl sulfide (DMS)
  • low temperatures
  • methanesulfinic acid (CHS(O)OH, MSIA)
  • methanesulfonic acid (MSA)
  • OH-initiated oxidation

Publication forum classification

  • Publication forum level 2

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry

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