New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals.

Autor:	Rosati B; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark.; Faculty of Physics, University of Vienna, Boltzmanngasse 5, Vienna AT-1090, Austria., Christiansen S; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Wollesen de Jonge R; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Roldin P; Division of Nuclear Physics, Lund University, P.O. Box 118, Lund SE-221 00, Sweden., Jensen MM; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Wang K; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Moosakutty SP; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark.; Clean Combustion Research Center, King Abdullah University of Science and Technology, Thuwal KSA-23955, Saudi Arabia., Thomsen D; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Salomonsen C; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Hyttinen N; Nano and Molecular Systems Research Unit, University of Oulu, P.O. Box 3000, Oulu FI-90014, Finland.; Department of Applied Physics, University of Eastern Finland, P.O. Box 1627, Kuopio FI-70211, Finland., Elm J; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Feilberg A; Department of Biological and Chemical Engineering, Aarhus University, Finlandsgade 12, Aarhus N DK-8200, Denmark., Glasius M; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark., Bilde M; Department of Chemistry, Aarhus University, Langelandsgade 140, Aarhus C DK-8000, Denmark.
Jazyk:	angličtina
Zdroj:	ACS earth & space chemistry [ACS Earth Space Chem] 2021 Apr 15; Vol. 5 (4), pp. 801-811. Date of Electronic Publication: 2021 Mar 25.
DOI:	10.1021/acsearthspacechem.0c00333
Abstrakt:	Dimethyl sulfide (DMS) is produced by plankton in oceans and constitutes the largest natural emission of sulfur to the atmosphere. In this work, we examine new particle formation from the primary pathway of oxidation of gas-phase DMS by OH radicals. We particularly focus on particle growth and mass yield as studied experimentally under dry conditions using the atmospheric simulation chamber AURA. Experimentally, we show that aerosol mass yields from oxidation of 50-200 ppb of DMS are low (2-7%) and that particle growth rates (8.2-24.4 nm/h) are comparable with ambient observations. An HR-ToF-AMS was calibrated using methanesulfonic acid (MSA) to account for fragments distributed across both the organic and sulfate fragmentation table. AMS-derived chemical compositions revealed that MSA was always more dominant than sulfate in the secondary aerosols formed. Modeling using the Aerosol Dynamics, gas- and particle-phase chemistry kinetic multilayer model for laboratory CHAMber studies (ADCHAM) indicates that the Master Chemical Mechanism gas-phase chemistry alone underestimates experimentally observed particle formation and that DMS multiphase and autoxidation chemistry is needed to explain observations. Based on quantum chemical calculations, we conclude that particle formation from DMS oxidation in the ambient atmosphere will most likely be driven by mixed sulfuric acid/MSA clusters clustering with both amines and ammonia. Competing Interests: The authors declare no competing financial interest. (© 2021 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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