Shen, Jiali and Scholz, Wiebke and He, Xu-Cheng and Zhou, Putian and Marie, Guillaume and Wang, Mingyi and Marten, Ruby and Surdu, Mihnea and Rörup, Birte and Baalbaki, Rima and Amorim, Antonio and Ataei, Farnoush and Bell, David M. and Bertozzi, Barbara and Brasseur, Zoé and Caudillo, Lucía and Chen, Dexian and Chu, Biwu and Dada, Lubna and Duplissy, Jonathan and Finkenzeller, Henning and Granzin, Manuel and Guida, Roberto and Heinritzi, Martin and Hofbauer, Victoria and Iyer, Siddharth and Kemppainen, Deniz and Kong, Weimeng and Krechmer, Jordan E. and Kürten, Andreas and Lamkaddam, Houssni and Lee, Chuan Ping and Lopez, Brandon and Mahfouz, Naser G. A. and Manninen, Hanna E. and Massabò, Dario and Mauldin, Roy L. and Mentler, Bernhard and Müller, Tatjana and Pfeifer, Joschka and Philippov, Maxim and Piedehierro, Ana A. and Roldin, Pontus and Schobesberger, Siegfried and Simon, Mario and Stolzenburg, Dominik and Tham, Yee Jun and Tomé, António and Umo, Nsikanabasi Silas and Wang, Dongyu and Wang, Yonghong and Weber, Stefan K. and Welti, André and Wollesen de Jonge, Robin and Wu, Yusheng and Zauner-Wieczorek, Marcel and Zust, Felix and Baltensperger, Urs and Curtius, Joachim and Flagan, Richard C. and Hansel, Armin and Möhler, Ottmar and Petäjä, Tuukka and Volkamer, Rainer and Kulmala, Markku and Lehtipalo, Katrianne and Rissanen, Matti and Kirkby, Jasper and El-Haddad, Imad and Bianchi, Federico and Sipilä, Mikko and Donahue, Neil M. and Worsnop, Douglas R. (2022) High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures. Environmental Science and Technology, 56 (19). pp. 13931-13944. ISSN 0013-936X. PMCID PMC9535848. doi:10.1021/acs.est.2c05154. https://resolver.caltech.edu/CaltechAUTHORS:20221013-48885100.19
Full text is not posted in this repository. Consult Related URLs below.
Use this Persistent URL to link to this item: https://resolver.caltech.edu/CaltechAUTHORS:20221013-48885100.19
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 H2SO4 from 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 H₂SO₄ production 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 NOₓ effect 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.
| Item Type: | Article | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|---|
| Related URLs: |
| ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| ORCID: | |||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Additional Information: | This research has received funding from the Academy of Finland ACCC Flagship (no. 337549), the Academy of Finland Academy professorship (no. 302958), the Academy of Finland (nos. 307331, 337550, 296628, 328290), the European Research Council (ERC) (Projects 742206, 714621, 101002728, and 850614); the EU H2020 programme Marie Skłodowska Curie ITN “CLOUD-TRAIN” (764991), the Swiss National Science Foundation (no. 200021_169090, 200020_172602, 20FI20_172622), the US National Science Foundation (no. AGS1531284, AGS1801574, AGS1801897, AGS1801280, AGS2215522); the European Union’s Horizon 2020 Research and Innovation Programme (Marie Skłodowska Curie no. 895875 “NPF-PANDA”), the Portuguese Foundation for Science and Technology (no. CERN/FIS-COM/0028/2019), the Swedish Research Council Formas Project (no. 2018-01745-COBACCA), the Swedish Research Council VR Project (no. 2019-05006), the Crafoord Foundation Project (no. 20210969), EU H2020 project FORCeS (no. 821205), German Federal Ministry of Education and Research, CLOUD-16 (01LK1601A), and the doctoral scholarship (2021/1) of the University of Innsbruck. The authors thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Funders: |
| ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Issue or Number: | 19 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| PubMed Central ID: | PMC9535848 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| DOI: | 10.1021/acs.est.2c05154 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Record Number: | CaltechAUTHORS:20221013-48885100.19 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20221013-48885100.19 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| ID Code: | 117407 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Collection: | CaltechAUTHORS | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Deposited By: | Research Services Depository | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Deposited On: | 18 Oct 2022 22:26 | ||||||||||||||||||||||||||||||||||||||||||||||||||||||||
| Last Modified: | 18 Oct 2022 22:26 |
Repository Staff Only: item control page
