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High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures - CERN Document Server
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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. 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" /> <meta name="keywords" content="CERN Document Server, WebSearch, CERN Document Server" /> <script type="text/javascript" src="https://cds.cern.ch/js/jquery.min.js"></script> <!-- WebNews CSS library --> <link rel="stylesheet" href="https://cds.cern.ch/img/webnews.css" type="text/css" /> <!-- WebNews JS library --> <script type="text/javascript" src="https://cds.cern.ch/js/webnews.js?v=20131009"></script> <meta property="fb:app_id" content="137353533001720"/> <script type="text/x-mathjax-config"> MathJax.Hub.Config({ tex2jax: {inlineMath: [['$','$']], processEscapes: true}, showProcessingMessages: false, messageStyle: "none" }); </script> <script src="/MathJax/MathJax.js?config=TeX-AMS_CHTML" type="text/javascript"> </script> <!-- GoogleScholar --> <meta content="submitter : High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures" name="citation_title" /> <meta content="Shen, Jiali" name="citation_author" /> <meta content="Weber, Stefan K" name="citation_author" /> <meta content="Lee, Chuan Ping" name="citation_author" /> <meta content="Scholz, Wiebke" name="citation_author" /> <meta content="Bianchi, Federico" name="citation_author" /> <meta content="Petäjä, Tuukka" name="citation_author" /> <meta content="Chen, Dexian" name="citation_author" /> <meta content="Caudillo, Lucía" name="citation_author" /> <meta content="Kemppainen, Deniz" name="citation_author" /> <meta content="Hofbauer, Victoria" name="citation_author" /> <meta content="Wang, Dongyu" name="citation_author" /> <meta content="Guida, Roberto" name="citation_author" /> <meta content="Philippov, Maxim" name="citation_author" /> <meta content="Wollesen de Jonge, Robin" 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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." property="og:description" /> <!-- Twitter Card --> <meta content="summary" name="twitter:card" /> <style></style> </head> <body class="CERN32Document32Server search" lang="no"> <!-- toolbar starts --> <div id="cern-toolbar"> <h1><a href="http://cern.ch" title="CERN">CERN <span>Accelerating science</span></a></h1> <ul> <li class="cern-accountlinks"><a class="cern-account" href="https://cds.cern.ch/youraccount/login?ln=no&referer=https%3A//cds.cern.ch/record/2852836%3Fln%3Dno" title="Sign in to your CERN account">Sign in</a></li> <li><a class="cern-directory" href="http://cern.ch/directory" title="Search CERN resources and browse the directory">Directory</a></li> </ul> </div> <!-- toolbar ends --> <!-- Nav header starts--> <div role="banner" class="clearfix" id="header"> <div class="header-inner inner"> <hgroup class="clearfix"> <h2 id="site-name"> <a rel="home" title="Home" href="/"><span>CERN Document Server</span></a> </h2> <h3 id="site-slogan">Access articles, reports and multimedia content in HEP</h3> </hgroup><!-- /#name-and-slogan --> <div role="navigation" id="main-navigation" class="cdsmenu"> <h2 class="element-invisible">Main menu</h2><ul class="links inline clearfix"> <li class="menu-386 first active-trail"><a class="active-trail" href="https://cds.cern.ch/?ln=no">Søk</a></li> <li class="menu-444 "><a class="" title="" href="https://cds.cern.ch/submit?ln=no">Send inn</a></li> <li class="menu-426 "><a class="" href="https://cds.cern.ch/help/?ln=no">Hjelp</a></li> <li class="leaf hassubcdsmenu"> <a hreflang="en" class="header" href="https://cds.cern.ch/youraccount/display?ln=no">Brukerinnstillinger</a> <ul class="subsubcdsmenu"><li><a href="https://cds.cern.ch/youralerts/list?ln=no">Your alerts</a></li><li><a href="https://cds.cern.ch/yourbaskets/display?ln=no">Your baskets</a></li><li><a href="https://cds.cern.ch/yourcomments?ln=no">Your comments</a></li><li><a href="https://cds.cern.ch/youralerts/display?ln=no">Your searches</a></li></ul></li> </ul> </div> </div> </div> <!-- Nav header ends--> <table class="navtrailbox"> <tr> <td class="navtrailboxbody"> <a href="/?ln=no" class="navtrail">Hovedsiden</a> > High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures </td> </tr> </table> </div> <div class="pagebody"><div class="pagebodystripemiddle"> <div class="detailedrecordbox"> <div class="detailedrecordtabs"> <div> <ul class="detailedrecordtabs"><li class="on first"><a href="/record/2852836/?ln=no">Informasjon </a></li><li class=""><a href="/record/2852836/files?ln=no">Files </a></li></ul> <div id="tabsSpacer" style="clear:both;height:0px"> </div></div> </div> <div class="detailedrecordboxcontent"> <div class="top-left-folded"></div> <div class="top-right-folded"></div> <div class="inside"> <!--<div style="height:0.1em;"> </div> <p class="notopgap"> </p>--> <abbr class="unapi-id" title="2852836"></abbr> <style type="text/css"> <!-- ul.detailedrecordtabs li.on a{background-color:#4D94CC;color:#fff !important;border-bottom:1px solid #4D94CC!important;} div.detailedrecordboxcontent {padding-top:0px !important;} --> </style> <table class="formatRecordTableFullWidth" > <tr> <td class="formatRecordHeader" style="background-image: url('https://cds.cern.ch/img/journals.jpg');" colspan="2"> <!--YTD: record may have more than one 690C.a tag--> Article </td> </tr> <script type="text/javascript"> $( document ).ready(function() { $('.showAuthor').on('click', function() { var author = '<p>' + $(this).data('name') + '</p>'; var affiliation = $(this).data('affiliation') + '</br>'; var contribution = $(this).data('contribution') + '</br>'; $.magnificPopup.open({ items: { src: '<div id="ovelary-mathjax" class="overlay-white oc-content overlay-white-500">' + author + affiliation + contribution + '</div>', type: 'inline' }, callbacks: { open: function() { var div = document.getElementById("overlay-mathjax") MathJax.Hub.Queue(["Typeset", MathJax.Hub, div]); }, } }) }) }); </script> <tr><td class="formatRecordLabel"> Title </td><td style="padding-left:5px;"><b>High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures</b></td></tr> <tr><td class="formatRecordLabel"><span style="white-space:nowrap;"> Author(s) </span> </td><td style="padding-left:5px;"> <script type="text/javascript"> function toggle_authors_visibility(){ var more = document.getElementById('more'); var link = document.getElementById('link'); var extension = document.getElementById('extension'); if (more.style.display=='none'){ more.style.display = ''; extension.style.display = 'none'; link.innerHTML = "Skjul" } else { more.style.display = 'none'; extension.style.display = ''; link.innerHTML = "Vis alle 73 forfattere" } link.style.color = "rgb(204,0,0);" } function set_up(){ var extension = document.getElementById('extension'); extension.innerHTML = ""; toggle_authors_visibility(); } </script> <a name="show_hide" /><a href="https://cds.cern.ch/search?f=author&p=Shen%2C%20Jiali&ln=no">Shen, Jiali</a> ; <a href="https://cds.cern.ch/search?f=author&p=Scholz%2C%20Wiebke&ln=no">Scholz, Wiebke</a> ; <a href="https://cds.cern.ch/search?f=author&p=He%2C%20Xu-Cheng&ln=no">He, Xu-Cheng</a> ; <a href="https://cds.cern.ch/search?f=author&p=Zhou%2C%20Putian&ln=no">Zhou, Putian</a> ; <a href="https://cds.cern.ch/search?f=author&p=Marie%2C%20Guillaume&ln=no">Marie, Guillaume</a> ; <a href="https://cds.cern.ch/search?f=author&p=Wang%2C%20Mingyi&ln=no">Wang, Mingyi</a> ; <a href="https://cds.cern.ch/search?f=author&p=Marten%2C%20Ruby&ln=no">Marten, Ruby</a> ; 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<a href="https://cds.cern.ch/search?f=author&p=Donahue%2C%20Neil%20M&ln=no">Donahue, Neil M</a> ; <a href="https://cds.cern.ch/search?f=author&p=Worsnop%2C%20Douglas%20R&ln=no">Worsnop, Douglas R</a></span> <span id="extension"></span> <small><i><a id="link" href="#" onclick="toggle_authors_visibility()" style="color:rgb(204,0,0);"></a></i></small><script type="text/javascript">set_up()</script></td></tr> <tr><td class="formatRecordLabel"> Publication </td><td style="padding-left:5px;">2022</td></tr> <tr><td class="formatRecordLabel"> Number of pages </td><td style="padding-left:5px;">14</td></tr> <tr><td class="formatRecordLabel"> In: </td><td style="padding-left:5px;"><a href="http://dx.doi.org/10.1021/acs.est.2c05154"><i>Environ. Sci. Technol.</i> 56 (2022) 13931-13944</a> </a></td></tr> <tr><td class="formatRecordLabel"> DOI </td><td style="padding-left:5px;"><a href="http://dx.doi.org/10.1021/acs.est.2c05154" title="DOI" target="_blank">10.1021/acs.est.2c05154</a> <tr><td class="formatRecordLabel"> Subject category </td><td style="padding-left:5px;">Astrophysics and Astronomy</td></tr> <tr><td class="formatRecordLabel"> Accelerator/Facility, Experiment </td><td style="padding-left:5px;"><a href="https://cds.cern.ch/search?p=CLOUD&f=693__a">CLOUD</a></td></tr> <tr><td class="formatRecordLabel"> Abstract </td><td style="padding-left:5px;">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.</td></tr> <tr><td class="formatRecordLabel"> Copyright/License </td><td style="padding-left:5px;">© 2022-2024 The Authors (License: <a href="https://creativecommons.org/licenses/by/4.0/">CC-BY-4.0</a>)</td></tr> </table> <br/>Corresponding record in: <a href="http://inspirehep.net/record/2639824">Inspire</a> <small> </small> <br/> <br/><br/><div align="right"><div style="padding-bottom:2px;padding-top:30px;"><span class="moreinfo" style="margin-right:10px;"> <a href="" class="moreinfo">Back to search</a> </span></div></div> <div class="bottom-left-folded"><div class="recordlastmodifiedbox" style="position:relative;margin-left:1px"> Element opprettet 2023-03-18, sist endret 2023-03-18</div></div> <div class="bottom-right-folded" style="text-align:right;padding-bottom:2px;"> <span class="moreinfo" style="margin-right:10px;"><a href="/search?ln=no&p=recid%3A2852836&rm=wrd" class="moreinfo">Lignende elementer</a></span></div> </div> </div> </div> <br/> <br /> <div class="detailedrecordminipanel"> <div class="top-left"></div><div class="top-right"></div> <div class="inside"> <div id="detailedrecordminipanelfile" style="width:33%;float:left;text-align:center;margin-top:0"> <div><small class="detailedRecordActions">Fulltekst:</small> <br /><a href="/record/2852836/files/acs.est.2c05154.pdf"><img style="border:none" src="/img/file-icon-text-34x48.gif" alt="Last ned fulltekst" /><br />PDF</a><br /></div> </div> <div id="detailedrecordminipanelreview" style="width:30%;float:left;text-align:center"> </div> <div id="detailedrecordminipanelactions" style="width:36%;float:right;text-align:right;"> <ul class="detailedrecordactions"> <li><a href="/yourbaskets/add?ln=no&recid=2852836">Legg i egen kurv</a></li> <li>Eksporter som <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/hx?ln=no">BibTeX</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/hm?ln=no">MARC</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xm?ln=no">MARCXML</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xd?ln=no">DC</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xe?ln=no">EndNote</a>, <!-- <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xe8x?ln=no">EndNote (8-X)</a>,--> <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xn?ln=no">NLM</a>, <a style="text-decoration:underline;font-weight:normal" href="/record/2852836/export/xw?ln=no">RefWorks</a> </li> </ul> <div style='padding-left: 13px;'> <!-- JQuery Bookmark Button BEGIN --> <div id="bookmark"></div> <div id="bookmark_sciencewise"></div> <style type="text/css"> #bookmark_sciencewise, #bookmark {float: left;} #bookmark_sciencewise li {padding: 2px; width: 25px;} #bookmark_sciencewise ul, #bookmark ul {list-style-image: none;} </style> <script type="text/javascript" src="/js/jquery.bookmark.min.js"></script> <style type="text/css">@import "/css/jquery.bookmark.css";</style> <script type="text/javascript">// <![CDATA[ $.bookmark.addSite('sciencewise', 'ScienceWise.info', 'https://cds.cern.ch/img/sciencewise.png', 'en', 'bookmark', 'http://sciencewise.info/bookmarks/cds:2852836/add'); $('#bookmark_sciencewise').bookmark({sites: ['sciencewise']}); $('#bookmark').bookmark({ sites: ['facebook', 'twitter', 'linkedin', 'google_plusone'], icons: '/img/bookmarks.png', url: 'https://cds.cern.ch/record/2852836', addEmail: true, title: "High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures", description: "Dimethyl sulfide (DMS) influences climate via cloud condensation nuclei (CCN) formation resulting from its oxidation products (mainly\nmethanesulfonic acid, MSA, and sulfuric acid, H2SO4). Despite their importance,\naccurate prediction of MSA and H2SO4 from DMS oxidation remains\nchallenging. With comprehensive experiments carried out in the Cosmics\nLeaving Outdoor Droplets (CLOUD) chamber at CERN, we show that\ndecreasing the temperature from +25 to \u221210 \u00b0C enhances the gas-phase MSA\nproduction by an order of magnitude from OH-initiated DMS oxidation, while\nH2SO4 production is modestly affected. This leads to a gas-phase H2SO4-to-MSA\nratio (H2SO4/MSA) smaller than one at low temperatures, consistent with field\nobservations in polar regions. With an updated DMS oxidation mechanism, we\nfind that methanesulfinic acid, CH3S(O)OH, MSIA, forms large amounts of\nMSA. Overall, our results reveal that MSA yields are a factor of 2\u221210 higher than\nthose predicted by the widely used Master Chemical Mechanism (MCMv3.3.1), and the NOx effect is less significant than that of\ntemperature. Our updated mechanism explains the high MSA production rates observed in field observations, especially at low\ntemperatures, thus, substantiating the greater importance of MSA in the natural sulfur cycle and natural CCN formation. 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