Evaluation of OH and HO2 concentrations and their budgets during photooxidation of 2-methyl-3-butene-2-ol (MBO) in the atmospheric simulation chamber SAPHIR

  • Several previous field studies have reported unexpectedly large concentrations of hydroxyl and hydroperoxyl radicals (OH and HO2, respectively) in forested environments that could not be explained by the traditional oxidation mechanisms that largely underestimated the observations. These environments were characterized by large concentrations of biogenic volatile organic compounds (BVOC) and low nitrogen oxide concentration. In isoprene-dominated environments, models developed to simulate atmospheric photochemistry generally underestimated the observed OH radical concentrations. In contrast, HO2 radical concentration showed large discrepancies with model simulations mainly in non-isoprene-dominated forested environments. An abundant BVOC emitted by lodgepole and ponderosa pines is 2-methyl-3-butene-2-ol (MBO), observed in large concentrations for studies where the HO2 concentration was poorly described by model simulations. In this work, the photooxidation of MBO by OH wasSeveral previous field studies have reported unexpectedly large concentrations of hydroxyl and hydroperoxyl radicals (OH and HO2, respectively) in forested environments that could not be explained by the traditional oxidation mechanisms that largely underestimated the observations. These environments were characterized by large concentrations of biogenic volatile organic compounds (BVOC) and low nitrogen oxide concentration. In isoprene-dominated environments, models developed to simulate atmospheric photochemistry generally underestimated the observed OH radical concentrations. In contrast, HO2 radical concentration showed large discrepancies with model simulations mainly in non-isoprene-dominated forested environments. An abundant BVOC emitted by lodgepole and ponderosa pines is 2-methyl-3-butene-2-ol (MBO), observed in large concentrations for studies where the HO2 concentration was poorly described by model simulations. In this work, the photooxidation of MBO by OH was investigated for NO concentrations lower than 200 pptv in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich. Measurements of OH and HO2 radicals, OH reactivity (kOH), MBO, OH precursors, and organic products (acetone and formaldehyde) were used to test our current understanding of the OH-oxidation mechanisms for MBO by comparing measurements with model calculations. All the measured trace gases agreed well with the model results (within 15 %) indicating a well understood mechanism for the MBO oxidation by OH. Therefore, the oxidation of MBO cannot contribute to reconciling the unexplained high OH and HO2 radical concentrations found in previous field studies.show moreshow less

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Author:Anna NovelliORCiD, Martin Kaminski, Michael RolletterORCiD, Ismail-Hakki Acir, Birger BohnORCiD, Hans-Peter DornORCiD, Xin Li, Anna Lutz, Sascha NehrORCiDGND, Franz Rohrer, Ralf Tillmann, Robert WegenerORCiD, Frank Holland, Andreas HofzumahausORCiD, Astrid Kiendler-ScharrORCiD, Andreas WahnerORCiD, Hendrik FuchsORCiD
Qualitätssicherung:peer reviewed
open access:Gold - Erstveröffentlichung mit Lizenzhinweis
Fachbereich/Einrichtung:Hochschule Düsseldorf / Fachbereich - Maschinenbau und Verfahrenstechnik
Document Type:Article
Year of Completion:2018
Language of Publication:English
Publisher:Copernicus
Parent Title (English):Atmospheric Chemistry and Physics
Volume:18
Issue:15
Page Number:14
First Page:11409
Last Page:11422
DOI:https://doi.org/10.5194/acp-18-11409-2018
ISSN:1680-7324
Tag:Luftreinhaltung
Dewey Decimal Classification:6 Technik, Medizin, angewandte Wissenschaften / 62 Ingenieurwissenschaften / 620 Ingenieurwissenschaften und zugeordnete Tätigkeiten
Licence (German):Creative Commons - CC BY - Namensnennung 4.0 International
Release Date:2024/11/20
Note:
Code and data availability
The data from the experiments in the SAPHIR chamber used in this work are available on the EUROCHAMP data home page (https://data.eurochamp.org/, last access: 1 October 2019, EUROCHAMP, 2019).

Supplement
The supplement related to this article is available online at: https://doi.org/10.5194/acp-20-3333-2020-supplement.
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