Universität zu Köln

Shen, Hongru ORCID: 0000-0002-5689-1549, Vereecken, Luc ORCID: 0000-0001-7845-684X, Kang, Sungah, Pullinen, Iida ORCID: 0000-0003-1558-2720, Fuchs, Hendrik ORCID: 0000-0003-1263-0061, Zhao, Defeng ORCID: 0000-0002-8790-7283 and Mentel, Thomas F. (2022). Unexpected significance of a minor reaction pathway in daytime formation of biogenic highly oxygenated organic compounds. Sci. Adv., 8 (42). WASHINGTON: AMER ASSOC ADVANCEMENT SCIENCE. ISSN 2375-2548

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Abstract

Secondary organic aerosol (SOA), formed by oxidation of volatile organic compounds, substantially influence air quality and climate. Highly oxygenated organic molecules (HOMs), particularly those formed from biogenic monoterpenes, contribute a large fraction of SOA. During daytime, hydroxyl radicals initiate monoterpene oxidation, mainly by hydroxyl addition to monoterpene double bonds. Naturally, related HOM formation mechanisms should be induced by that reaction route, too. However, for a-pinene, the most abundant atmospheric monoterpene, we find a previously unidentified competitive pathway under atmospherically relevant conditions: HOM formation is predominately induced via hydrogen abstraction by hydroxyl radicals, a generally minor reaction pathway. We show by observations and theoretical calculations that hydrogen abstraction followed by formation and rearrangement of alkoxy radicals is a prerequisite for fast daytime HOM formation. Our analysis provides an accurate mechanism and yield, demonstrating that minor reaction pathways can become major, here for SOA formation and growth and related impacts on air quality and climate.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Shen, Hongru UNSPECIFIED orcid.org/0000-0002-5689-1549 UNSPECIFIED Vereecken, Luc UNSPECIFIED orcid.org/0000-0001-7845-684X UNSPECIFIED Kang, Sungah UNSPECIFIED UNSPECIFIED UNSPECIFIED Pullinen, Iida UNSPECIFIED orcid.org/0000-0003-1558-2720 UNSPECIFIED Fuchs, Hendrik UNSPECIFIED orcid.org/0000-0003-1263-0061 UNSPECIFIED Zhao, Defeng UNSPECIFIED orcid.org/0000-0002-8790-7283 UNSPECIFIED Mentel, Thomas F. UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-681642
DOI:	10.1126/sciadv.abp8702
Journal or Publication Title:	Sci. Adv.
Volume:	8
Number:	42
Date:	2022
Publisher:	AMER ASSOC ADVANCEMENT SCIENCE
Place of Publication:	WASHINGTON
ISSN:	2375-2548
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language INITIATED ATMOSPHERIC OXIDATION; H-ATOM ABSTRACTION; OXIDIZED MULTIFUNCTIONAL COMPOUNDS; CORRELATED MOLECULAR CALCULATIONS; ALPHA-PINENE PHOTOOXIDATION; MAIN-GROUP THERMOCHEMISTRY; GAUSSIAN-BASIS SETS; GAS-PHASE REACTIONS; PEROXY-RADICALS; TROPOSPHERIC DEGRADATION Multiple languages Multidisciplinary Sciences Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/68164