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

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.

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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:
URLURL TypeDescription CentralArticle
Shen, Jiali0000-0001-8701-7929
Scholz, Wiebke0000-0003-2617-620X
He, Xu-Cheng0000-0002-7416-306X
Zhou, Putian0000-0003-0803-7337
Marie, Guillaume0000-0003-1454-0908
Wang, Mingyi0000-0001-5782-2513
Marten, Ruby0000-0003-0417-4350
Surdu, Mihnea0000-0003-1815-2750
Rörup, Birte0000-0001-8755-9453
Baalbaki, Rima0000-0002-4480-2107
Amorim, Antonio0000-0003-0638-2321
Ataei, Farnoush0000-0001-8038-649X
Bell, David M.0000-0002-3958-2138
Bertozzi, Barbara0000-0003-2571-6585
Brasseur, Zoé0000-0001-5387-018X
Chen, Dexian0000-0001-6963-5205
Chu, Biwu0000-0002-7548-5669
Dada, Lubna0000-0003-1105-9043
Duplissy, Jonathan0000-0001-8819-0264
Finkenzeller, Henning0000-0002-8349-3714
Guida, Roberto0000-0001-8413-9672
Heinritzi, Martin0000-0002-9171-8127
Hofbauer, Victoria0000-0001-9036-4446
Iyer, Siddharth0000-0001-5989-609X
Kemppainen, Deniz0000-0001-8282-0501
Kong, Weimeng0000-0002-9432-2857
Krechmer, Jordan E.0000-0003-3642-0659
Kürten, Andreas0000-0002-8955-4450
Lamkaddam, Houssni0000-0001-5166-6353
Lee, Chuan Ping0000-0003-0051-8179
Mahfouz, Naser G. A.0000-0002-7097-1430
Manninen, Hanna E.0000-0002-0419-4020
Massabò, Dario0000-0001-7445-0328
Mauldin, Roy L.0000-0002-8569-8561
Mentler, Bernhard0000-0003-3852-0397
Müller, Tatjana0000-0001-6453-9134
Pfeifer, Joschka0000-0002-9172-4447
Philippov, Maxim0000-0003-4302-0020
Piedehierro, Ana A.0000-0002-1900-8139
Schobesberger, Siegfried0000-0002-5777-4897
Simon, Mario0000-0002-4900-7460
Stolzenburg, Dominik0000-0003-1014-1360
Tham, Yee Jun0000-0001-7924-5841
Tomé, António0000-0001-9144-7120
Wang, Dongyu0000-0001-7549-1578
Wang, Yonghong0000-0003-2498-9143
Weber, Stefan K.0000-0001-7408-9069
Welti, André0000-0002-3549-1212
Zauner-Wieczorek, Marcel0000-0002-0867-665X
Baltensperger, Urs0000-0003-0079-8713
Curtius, Joachim0000-0003-3153-4630
Flagan, Richard C.0000-0001-5690-770X
Hansel, Armin0000-0002-1062-2394
Möhler, Ottmar0000-0002-7551-9814
Petäjä, Tuukka0000-0002-1881-9044
Volkamer, Rainer0000-0002-0899-1369
Kulmala, Markku0000-0003-3464-7825
Lehtipalo, Katrianne0000-0002-1660-2706
Rissanen, Matti0000-0003-0463-8098
Kirkby, Jasper0000-0003-2341-9069
El-Haddad, Imad0000-0002-2461-7238
Bianchi, Federico0000-0003-2996-3604
Sipilä, Mikko0000-0002-8594-7003
Donahue, Neil M.0000-0003-3054-2364
Worsnop, Douglas R.0000-0002-8928-8017
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.
Funding AgencyGrant Number
Academy of Finland337549
Academy of Finland302958
Academy of Finland307331
Academy of Finland337550
Academy of Finland296628
Academy of Finland328290
European Research Council (ERC)742206
European Research Council (ERC)714621
European Research Council (ERC)101002728
European Research Council (ERC)850614
Marie Curie Fellowship764991
Swiss National Science Foundation (SNSF)200021_169090
Swiss National Science Foundation (SNSF)200020_172602
Swiss National Science Foundation (SNSF)20FI20_172622
Marie Curie Fellowship895875
Fundação para a Ciência e a Tecnologia (FCT)CERN/FIS-COM/0028/2019
Swedish Research Council2018-01745-COBACCA
Swedish Research Council2019-05006
Crafoord Foundation20210969
European Research Council (ERC)821205
Bundesministerium für Bildung und Forschung (BMBF)01LK1601A
University of Innsbruck2021/1
Issue or Number:19
PubMed Central ID:PMC9535848
Record Number:CaltechAUTHORS:20221013-48885100.19
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117407
Deposited By: Research Services Depository
Deposited On:18 Oct 2022 22:26
Last Modified:18 Oct 2022 22:26

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