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High Gas-Phase Meth...
High Gas-Phase Methanesulfonic Acid Production in the OH-Initiated Oxidation of Dimethyl Sulfide at Low Temperatures
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- Shen, J. (author)
- University of Helsinki
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- Roldin, P. (author)
- Lund University,Lunds universitet,MERGE: ModElling the Regional and Global Earth system,Centrum för miljö- och klimatvetenskap (CEC),Naturvetenskapliga fakulteten,Kärnfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,LTH profilområde: Aerosoler,LTH profilområden,Centre for Environmental and Climate Science (CEC),Faculty of Science,Nuclear physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Aerosols,LTH Profile areas,Faculty of Engineering, LTH
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- Wollesen De Jonge, R. (author)
- Lund University,Lunds universitet,MERGE: ModElling the Regional and Global Earth system,Centrum för miljö- och klimatvetenskap (CEC),Naturvetenskapliga fakulteten,Kärnfysik,Fysiska institutionen,Institutioner vid LTH,Lunds Tekniska Högskola,LTH profilområde: Aerosoler,LTH profilområden,Centre for Environmental and Climate Science (CEC),Faculty of Science,Nuclear physics,Department of Physics,Departments at LTH,Faculty of Engineering, LTH,LTH Profile Area: Aerosols,LTH Profile areas,Faculty of Engineering, LTH
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- Bianchi, Federico (author)
- University of Helsinki
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- Worsnop, D.R. (author)
- University of Helsinki
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(creator_code:org_t)
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et al
- 2022-09-22
- 2022
- English 14 s.
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In: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:19, s. 13931-13944
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Abstract
Subject headings
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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. © 2022 The Authors. Published by American Chemical Society.
Subject headings
- NATURVETENSKAP -- Geovetenskap och miljövetenskap -- Meteorologi och atmosfärforskning (hsv//swe)
- NATURAL SCIENCES -- Earth and Related Environmental Sciences -- Meteorology and Atmospheric Sciences (hsv//eng)
- NATURVETENSKAP -- Kemi -- Annan kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Other Chemistry Topics (hsv//eng)
Keyword
- 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, MSIA)
- Methanesulphonic acid
- OH -
- Sulfur compounds
Publication and Content Type
- art (subject category)
- ref (subject category)
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