This title appears in the Scientific Report :
2017
Please use the identifier:
http://dx.doi.org/10.1002/kin.21130 in citations.
Highly Oxygenated Molecules from Atmospheric Autoxidation of Hydrocarbons: A Prominent Challenge for Chemical Kinetic Studies
Highly Oxygenated Molecules from Atmospheric Autoxidation of Hydrocarbons: A Prominent Challenge for Chemical Kinetic Studies
Recent advances in chemical ionization mass spectrometry have allowed the detection of a new group of compounds termed highly oxygenated molecules (HOM). These are atmospheric oxidation products of volatile organic compounds (VOC) retaining most of their carbon backbone, and with O/C ratios around u...
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Personal Name(s): | Ehn, Mikael (Corresponding author) |
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Berndt, Torsten / Wildt, Jürgen / Mentel, Thomas F. | |
Contributing Institute: |
Troposphäre; IEK-8 |
Published in: | International journal of chemical kinetics, 49 (2017) 11, S. 821 - 831 |
Imprint: |
New York, NY
Wiley
2017
|
DOI: |
10.1002/kin.21130 |
Document Type: |
Journal Article |
Research Program: |
Tropospheric trace substances and their transformation processes |
Publikationsportal JuSER |
Recent advances in chemical ionization mass spectrometry have allowed the detection of a new group of compounds termed highly oxygenated molecules (HOM). These are atmospheric oxidation products of volatile organic compounds (VOC) retaining most of their carbon backbone, and with O/C ratios around unity. Owing to their surprisingly high yields and low vapor pressures, the importance of HOM for aerosol formation has been easy to verify. However, the opposite can be said concerning the exact formation pathways of HOM from major aerosol precursor VOC. While the role of peroxy radical autoxidation, i.e., consecutive intramolecular H-shifts followed by O2 addition, has been recognized, the detailed formation mechanisms remain highly uncertain. A primary reason is that the autoxidation process occurs on sub-second timescales and is extremely sensitive to environmental conditions like gas composition, temperature, and pressure. This, in turn, poses a great challenge for chemical kinetics studies to be able to mimic the relevant atmospheric reaction pathways, while simultaneously using conditions suitable for studying the short-lived radical intermediates. In this perspective, we define six specific challenges for this community to directly observe the initial steps of atmospherically relevant autoxidation reactions and thereby facilitate vital improvements in the understanding of VOC degradation and organic aerosol formation. |