التفاصيل البيبلوغرافية
العنوان: |
High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures |
المؤلفون: |
Shen, J., Roldin, P., Wollesen De Jonge, R., Bianchi, Federico, Worsnop, D.R. |
المصدر: |
Environmental Science and Technology MERGE: ModElling the Regional and Global Earth system. 56(19):13931-13944 |
مصطلحات موضوعية: |
dimethyl sulfide (DMS), low temperatures, methanesulfinic acid (CH3S(O)OH, MSIA), methanesulfonic acid (MSA), OH-initiated oxidation, Gases, Organic acids, Oxidation, Acid production, Dimethyl sulphide, Dimethylsulphide, Gas-phases, Lows-temperatures, Methanesulphinic acid (CH3S(O)OH, Methanesulphonic acid, OH, Sulfur compounds, Naturvetenskap, Geovetenskap och miljövetenskap, Meteorologi och atmosfärforskning, Natural Sciences, Earth and Related Environmental Sciences, Meteorology and Atmospheric Sciences, Kemi, Annan kemi, Chemical Sciences, Other Chemistry Topics |
الوصف: |
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. © 2022 The Authors. Published by American Chemical Society. |
URL الوصول: |
https://lup.lub.lu.se/record/f1e4662f-d171-42ec-a7f5-95a4c12e1113 http://dx.doi.org/10.1021/acs.est.2c05154 |
قاعدة البيانات: |
SwePub |