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Published September 6, 2016 | Published
Journal Article Open

Atmospheric mixing ratios of methyl ethyl ketone (2-butanone) in tropical, boreal, temperate and marine environments

Abstract

Methyl ethyl ketone (MEK) enters the atmosphere following direct emission from vegetation and anthropogenic activities, as well as being produced by the gas-phase oxidation of volatile organic compounds (VOCs) such as n-butane. This study presents the first overview of ambient MEK measurements at six different locations, characteristic of forested, urban and marine environments. In order to understand better the occurrence and behaviour of MEK in the atmosphere, we analyse diel cycles of MEK mixing ratios, vertical profiles, ecosystem flux data, and HYSPLIT back trajectories, and compare with co-measured VOCs. MEK measurements were primarily conducted with proton-transfer-reaction mass spectrometer (PTR-MS) instruments. Results from the sites under biogenic influence demonstrate that vegetation is an important source of MEK. The diel cycle of MEK follows that of ambient temperature and the forest structure plays an important role in air mixing. At such sites, a high correlation of MEK with acetone was observed (e.g. r^2 = 0.96 for the SMEAR Estonia site in a remote hemiboreal forest in Tartumaa, Estonia, and r^2 = 0.89 at the ATTO pristine tropical rainforest site in central Amazonia). Under polluted conditions, we observed strongly enhanced MEK mixing ratios. Overall, the MEK mixing ratios and flux data presented here indicate that both biogenic and anthropogenic sources contribute to its occurrence in the global atmosphere.

Additional Information

© Author(s) 2016. This work is distributed under the Creative Commons Attribution 3.0 License. Received: 12 Apr 2016 – Published in Atmos. Chem. Phys. Discuss.: 25 Apr 2016. Revised: 10 Aug 2016 – Accepted: 17 Aug 2016 – Published: 06 Sep 2016. For ATTO, we thank the Max Planck Society and the Instituto Nacional de Pesquisas da Amazonia for continuous support. Furthermore, we acknowledge the support by the ATTO project (German Federal Ministry of Education and Research, BMBF funds 01LB1001A; Brazilian Ministério da Ciência, Tecnologia e Inovação FINEP/MCTI contract 01.11.01248.00), UEA and FAPEAM, LBA/INPA, and SDS/CEUC/RDS-Uatumã. We would especially like to thank all the people involved in the logistical support of the ATTO project, in particular Reiner Ditz and Hermes Braga Xavier. We acknowledge the micrometeorological group of INPA/LBA for their collaboration concerning the meteorological parameters, with special thanks to Marta Sá, Antonio Huxley and Leonardo Oliveira. We would like to acknowledge Stefan Wolff for the construction, support and maintenance of the inlet system. We are grateful to Nina Knothe for logistical help. We would also like to thank Thomas Klüpfel for all the great support provided with the PTR-MS operation in the laboratory as well as in the field. This paper contains results of research conducted under the Technical/Scientific Cooperation Agreement between the National Institute for Amazonian Research, the State University of Amazonas, and the Max-Planck-Gesellschaft e.V.; the opinions expressed are the entire responsibility of the authors and not of the participating institutions. For TT34, we thank the Natural Environment Research Council for funding the CLAIRE-UK project (reference NE/I012567/1), A. Valach, B. Davison and M. Shaw for assistance and A. R. MacKenzie for valuable discussions. For SMEAR, we would like to acknowledge the EU Regional Development Foundation: "Environmental Conservation and Environmental Technology R&D Programme" project BioAtmos (3.2.0802.11-0043), "Internationalization of Science Programme" project INSMEARIN (10.1-6/13/1028), and the "Estonian Research Infrastructures Roadmap" project Estonian Environmental Observatory (3.2.0304.11-0395). We express our gratitude to the Archimedes Foundation (international programme DoRa) and the "Freunde und Förderer der Goethe Universität" that provided funding to E. Bourtsoukidis for conducting research in Estonia. We would like to additionally thank Dominika Radacki, Javier Roales, Beate Noe, Eero Talts, Ahto Kangur and Miguel P. Estrada for providing valuable help with the setup and transportation. Special thanks to Boris Bonn for the insightful discussions and comments during the production of this article. For O_3HP, the measurements presented in this study were supported by the European Commission's 7th Framework Programme under grant agreement number 287382 "PIMMS", as well as by ANR-CANOPEE and ChArMEx, CEA and CNRS. We acknowledge B. Bonsang and C. Kalogridis for the GC-FID measurements, J. P. Orts and I. Reiter for logistical support, and J. Lathière for managing the CANOPÉE project. For T2, we thank Bruno Takeshi for all the logistical support. Furthermore, we acknowledge the support by FAPESP grant 2013/25058-1 and 2013/05014-0. For CYPHEX, the authors gratefully acknowledge the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model and READY website (http://www.ready.noaa.gov) used in this publication. The article processing charges for this open-access publication were covered by the Max Planck Society. Edited by: E. Harris. Reviewed by: two anonymous referees.

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