Atmospheric Gas-Phase Formation of Methanesulfonic Acid

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Standard

Atmospheric Gas-Phase Formation of Methanesulfonic Acid. / Chen, Jing; Lane, Joseph R.; Bates, Kelvin H.; Kjaergaard, Henrik G.

I: Environmental Science and Technology, Bind 57, Nr. 50, 2023, s. 21168−21177.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt

Harvard

Chen, J, Lane, JR, Bates, KH & Kjaergaard, HG 2023, 'Atmospheric Gas-Phase Formation of Methanesulfonic Acid', Environmental Science and Technology, bind 57, nr. 50, s. 21168−21177. https://doi.org/10.1021/acs.est.3c07120

APA

Chen, J., Lane, J. R., Bates, K. H., & Kjaergaard, H. G. (2023). Atmospheric Gas-Phase Formation of Methanesulfonic Acid. Environmental Science and Technology, 57(50), 21168−21177. https://doi.org/10.1021/acs.est.3c07120

Vancouver

Chen J, Lane JR, Bates KH, Kjaergaard HG. Atmospheric Gas-Phase Formation of Methanesulfonic Acid. Environmental Science and Technology. 2023;57(50):21168−21177. https://doi.org/10.1021/acs.est.3c07120

Author

Chen, Jing ; Lane, Joseph R. ; Bates, Kelvin H. ; Kjaergaard, Henrik G. / Atmospheric Gas-Phase Formation of Methanesulfonic Acid. I: Environmental Science and Technology. 2023 ; Bind 57, Nr. 50. s. 21168−21177.

Bibtex

@article{7c872680ae0344eeb8dfacd2b2c8ab9b,
title = "Atmospheric Gas-Phase Formation of Methanesulfonic Acid",
abstract = "Despite its impact on the climate, the mechanism of methanesulfonic acid (MSA) formation in the oxidation of dimethyl sulfide (DMS) remains unclear. The DMS + OH reaction is known to form methanesulfinic acid (MSIA), methane sulfenic acid (MSEA), the methylthio radical (CH3S), and hydroperoxymethyl thioformate (HPMTF). Among them, HPMTF reacts further to form SO2 and OCS, while the other three form the CH3SO2 radical. Based on theoretical calculations, we find that the CH3SO2 radical can add O2 to form CH3S(O)2OO, which can react further to form MSA. The branching ratio is highly temperature sensitive, and the MSA yield increases with decreasing temperature. In warmer regions, SO2 is the dominant product of DMS oxidation, while in colder regions, large amounts of MSA can form. Global modeling indicates that the proposed temperature-sensitive MSA formation mechanism leads to a substantial increase in the simulated global atmospheric MSA formation and burden.",
keywords = "dimethyl sulfide oxidation, global modeling, mechanism, quantum chemical computation, sulfuric acid",
author = "Jing Chen and Lane, {Joseph R.} and Bates, {Kelvin H.} and Kjaergaard, {Henrik G.}",
note = "Funding Information: This research was supported by research grants from VILLUM FONDEN (VIL50443) and the Alfred P. Sloan Foundation (G-2019-12281). Funding Information: We thank Torsten Berndt and Jonas Elm for the helpful discussions. We thank Jiali Shen and Federico Bianchi for sharing their experimental data. This project was supported by the High-Performance Computing Center at the University of Copenhagen (HPC-UCPH), and the New Zealand eScience Infrastructure (NeSI). Publisher Copyright: {\textcopyright} 2023 American Chemical Society",
year = "2023",
doi = "10.1021/acs.est.3c07120",
language = "English",
volume = "57",
pages = "21168−21177",
journal = "Environmental Science & Technology",
issn = "0013-936X",
publisher = "American Chemical Society",
number = "50",

}

RIS

TY - JOUR

T1 - Atmospheric Gas-Phase Formation of Methanesulfonic Acid

AU - Chen, Jing

AU - Lane, Joseph R.

AU - Bates, Kelvin H.

AU - Kjaergaard, Henrik G.

N1 - Funding Information: This research was supported by research grants from VILLUM FONDEN (VIL50443) and the Alfred P. Sloan Foundation (G-2019-12281). Funding Information: We thank Torsten Berndt and Jonas Elm for the helpful discussions. We thank Jiali Shen and Federico Bianchi for sharing their experimental data. This project was supported by the High-Performance Computing Center at the University of Copenhagen (HPC-UCPH), and the New Zealand eScience Infrastructure (NeSI). Publisher Copyright: © 2023 American Chemical Society

PY - 2023

Y1 - 2023

N2 - Despite its impact on the climate, the mechanism of methanesulfonic acid (MSA) formation in the oxidation of dimethyl sulfide (DMS) remains unclear. The DMS + OH reaction is known to form methanesulfinic acid (MSIA), methane sulfenic acid (MSEA), the methylthio radical (CH3S), and hydroperoxymethyl thioformate (HPMTF). Among them, HPMTF reacts further to form SO2 and OCS, while the other three form the CH3SO2 radical. Based on theoretical calculations, we find that the CH3SO2 radical can add O2 to form CH3S(O)2OO, which can react further to form MSA. The branching ratio is highly temperature sensitive, and the MSA yield increases with decreasing temperature. In warmer regions, SO2 is the dominant product of DMS oxidation, while in colder regions, large amounts of MSA can form. Global modeling indicates that the proposed temperature-sensitive MSA formation mechanism leads to a substantial increase in the simulated global atmospheric MSA formation and burden.

AB - Despite its impact on the climate, the mechanism of methanesulfonic acid (MSA) formation in the oxidation of dimethyl sulfide (DMS) remains unclear. The DMS + OH reaction is known to form methanesulfinic acid (MSIA), methane sulfenic acid (MSEA), the methylthio radical (CH3S), and hydroperoxymethyl thioformate (HPMTF). Among them, HPMTF reacts further to form SO2 and OCS, while the other three form the CH3SO2 radical. Based on theoretical calculations, we find that the CH3SO2 radical can add O2 to form CH3S(O)2OO, which can react further to form MSA. The branching ratio is highly temperature sensitive, and the MSA yield increases with decreasing temperature. In warmer regions, SO2 is the dominant product of DMS oxidation, while in colder regions, large amounts of MSA can form. Global modeling indicates that the proposed temperature-sensitive MSA formation mechanism leads to a substantial increase in the simulated global atmospheric MSA formation and burden.

KW - dimethyl sulfide oxidation

KW - global modeling

KW - mechanism

KW - quantum chemical computation

KW - sulfuric acid

U2 - 10.1021/acs.est.3c07120

DO - 10.1021/acs.est.3c07120

M3 - Journal article

C2 - 38051922

AN - SCOPUS:85180102630

VL - 57

SP - 21168−21177

JO - Environmental Science & Technology

JF - Environmental Science & Technology

SN - 0013-936X

IS - 50

ER -

ID: 377818613