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High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures
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 comp...
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| Lenguaje: | eng |
| Publicado: |
2022
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| Materias: | |
| Acceso en línea: | https://dx.doi.org/10.1021/acs.est.2c05154 http://cds.cern.ch/record/2852836 |
| _version_ | 1780977171856097280 |
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| author | Shen, Jiali Scholz, Wiebke He, Xu-Cheng Zhou, Putian Marie, Guillaume Wang, Mingyi Marten, Ruby Surdu, Mihnea Rörup, Birte Baalbaki, Rima Amorim, Antonio Ataei, Farnoush Bell, David M Bertozzi, Barbara Brasseur, Zoé Caudillo, Lucía Chen, Dexian Chu, Biwu Dada, Lubna Duplissy, Jonathan Finkenzeller, Henning Granzin, Manuel Guida, Roberto Heinritzi, Martin Hofbauer, Victoria Iyer, Siddharth Kemppainen, Deniz Kong, Weimeng Krechmer, Jordan E Kürten, Andreas Lamkaddam, Houssni Lee, Chuan Ping Lopez, Brandon Mahfouz, Naser G A Manninen, Hanna E Massabò, Dario Mauldin, Roy L Mentler, Bernhard Müller, Tatjana Pfeifer, Joschka Philippov, Maxim Piedehierro, Ana A Roldin, Pontus Schobesberger, Siegfried Simon, Mario Stolzenburg, Dominik Tham, Yee Jun Tomé, António Umo, Nsikanabasi Silas Wang, Dongyu Wang, Yonghong Weber, Stefan K Welti, André Wollesen de Jonge, Robin Wu, Yusheng Zauner-Wieczorek, Marcel Zust, Felix Baltensperger, Urs Curtius, Joachim Flagan, Richard C Hansel, Armin Möhler, Ottmar Petäjä, Tuukka Volkamer, Rainer Kulmala, Markku Lehtipalo, Katrianne Rissanen, Matti Kirkby, Jasper El-Haddad, Imad Bianchi, Federico Sipilä, Mikko Donahue, Neil M Worsnop, Douglas R |
| author_facet | Shen, Jiali Scholz, Wiebke He, Xu-Cheng Zhou, Putian Marie, Guillaume Wang, Mingyi Marten, Ruby Surdu, Mihnea Rörup, Birte Baalbaki, Rima Amorim, Antonio Ataei, Farnoush Bell, David M Bertozzi, Barbara Brasseur, Zoé Caudillo, Lucía Chen, Dexian Chu, Biwu Dada, Lubna Duplissy, Jonathan Finkenzeller, Henning Granzin, Manuel Guida, Roberto Heinritzi, Martin Hofbauer, Victoria Iyer, Siddharth Kemppainen, Deniz Kong, Weimeng Krechmer, Jordan E Kürten, Andreas Lamkaddam, Houssni Lee, Chuan Ping Lopez, Brandon Mahfouz, Naser G A Manninen, Hanna E Massabò, Dario Mauldin, Roy L Mentler, Bernhard Müller, Tatjana Pfeifer, Joschka Philippov, Maxim Piedehierro, Ana A Roldin, Pontus Schobesberger, Siegfried Simon, Mario Stolzenburg, Dominik Tham, Yee Jun Tomé, António Umo, Nsikanabasi Silas Wang, Dongyu Wang, Yonghong Weber, Stefan K Welti, André Wollesen de Jonge, Robin Wu, Yusheng Zauner-Wieczorek, Marcel Zust, Felix Baltensperger, Urs Curtius, Joachim Flagan, Richard C Hansel, Armin Möhler, Ottmar Petäjä, Tuukka Volkamer, Rainer Kulmala, Markku Lehtipalo, Katrianne Rissanen, Matti Kirkby, Jasper El-Haddad, Imad Bianchi, Federico Sipilä, Mikko Donahue, Neil M Worsnop, Douglas R |
| author_sort | Shen, Jiali |
| collection | CERN |
| description | 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. |
| id | cern-2852836 |
| institution | Organización Europea para la Investigación Nuclear |
| language | eng |
| publishDate | 2022 |
| record_format | invenio |
| spelling | cern-28528362023-03-18T19:34:46Zdoi:10.1021/acs.est.2c05154http://cds.cern.ch/record/2852836engShen, JialiScholz, WiebkeHe, Xu-ChengZhou, PutianMarie, GuillaumeWang, MingyiMarten, RubySurdu, MihneaRörup, BirteBaalbaki, RimaAmorim, AntonioAtaei, FarnoushBell, David MBertozzi, BarbaraBrasseur, ZoéCaudillo, LucíaChen, DexianChu, BiwuDada, LubnaDuplissy, JonathanFinkenzeller, HenningGranzin, ManuelGuida, RobertoHeinritzi, MartinHofbauer, VictoriaIyer, SiddharthKemppainen, DenizKong, WeimengKrechmer, Jordan EKürten, AndreasLamkaddam, HoussniLee, Chuan PingLopez, BrandonMahfouz, Naser G AManninen, Hanna EMassabò, DarioMauldin, Roy LMentler, BernhardMüller, TatjanaPfeifer, JoschkaPhilippov, MaximPiedehierro, Ana ARoldin, PontusSchobesberger, SiegfriedSimon, MarioStolzenburg, DominikTham, Yee JunTomé, AntónioUmo, Nsikanabasi SilasWang, DongyuWang, YonghongWeber, Stefan KWelti, AndréWollesen de Jonge, RobinWu, YushengZauner-Wieczorek, MarcelZust, FelixBaltensperger, UrsCurtius, JoachimFlagan, Richard CHansel, ArminMöhler, OttmarPetäjä, TuukkaVolkamer, RainerKulmala, MarkkuLehtipalo, KatrianneRissanen, MattiKirkby, JasperEl-Haddad, ImadBianchi, FedericoSipilä, MikkoDonahue, Neil MWorsnop, Douglas RHigh Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low TemperaturesAstrophysics and AstronomyDimethyl 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.oai:cds.cern.ch:28528362022 |
| spellingShingle | Astrophysics and Astronomy Shen, Jiali Scholz, Wiebke He, Xu-Cheng Zhou, Putian Marie, Guillaume Wang, Mingyi Marten, Ruby Surdu, Mihnea Rörup, Birte Baalbaki, Rima Amorim, Antonio Ataei, Farnoush Bell, David M Bertozzi, Barbara Brasseur, Zoé Caudillo, Lucía Chen, Dexian Chu, Biwu Dada, Lubna Duplissy, Jonathan Finkenzeller, Henning Granzin, Manuel Guida, Roberto Heinritzi, Martin Hofbauer, Victoria Iyer, Siddharth Kemppainen, Deniz Kong, Weimeng Krechmer, Jordan E Kürten, Andreas Lamkaddam, Houssni Lee, Chuan Ping Lopez, Brandon Mahfouz, Naser G A Manninen, Hanna E Massabò, Dario Mauldin, Roy L Mentler, Bernhard Müller, Tatjana Pfeifer, Joschka Philippov, Maxim Piedehierro, Ana A Roldin, Pontus Schobesberger, Siegfried Simon, Mario Stolzenburg, Dominik Tham, Yee Jun Tomé, António Umo, Nsikanabasi Silas Wang, Dongyu Wang, Yonghong Weber, Stefan K Welti, André Wollesen de Jonge, Robin Wu, Yusheng Zauner-Wieczorek, Marcel Zust, Felix Baltensperger, Urs Curtius, Joachim Flagan, Richard C Hansel, Armin Möhler, Ottmar Petäjä, Tuukka Volkamer, Rainer Kulmala, Markku Lehtipalo, Katrianne Rissanen, Matti Kirkby, Jasper El-Haddad, Imad Bianchi, Federico Sipilä, Mikko Donahue, Neil M Worsnop, Douglas R High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title | High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title_full | High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title_fullStr | High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title_full_unstemmed | High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title_short | High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
| title_sort | high gas-phase methanesulfonic acid production in the oh-initiated oxidation of dimethyl sulfide at low temperatures |
| topic | Astrophysics and Astronomy |
| url | https://dx.doi.org/10.1021/acs.est.2c05154 http://cds.cern.ch/record/2852836 |
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