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@ARTICLE{Mentel:202148,
author = {Mentel, T. F. and Springer, M. and Ehn, M. and Kleist, E.
and Pullinen, I. and Kurtén, T. and Rissanen, M. and
Wahner, A. and Wildt, J.},
title = {{F}ormation of highly oxidized multifunctional compounds:
autoxidation of peroxy radicals formed in the ozonolysis of
alkenes – deduced from structure–product relationships},
journal = {Atmospheric chemistry and physics},
volume = {15},
number = {12},
issn = {1680-7324},
address = {Katlenburg-Lindau},
publisher = {EGU},
reportid = {FZJ-2015-04437},
pages = {6745 - 6765},
year = {2015},
abstract = {It has been postulated that secondary organic particulate
matter plays a pivotal role in the early growth of newly
formed particles in forest areas. The recently detected
class of extremely low volatile organic compounds (ELVOC)
provides the missing organic vapors and possibly contributes
a significant fraction to atmospheric SOA (secondary organic
aerosol). The sequential rearrangement of peroxy radicals
and subsequent O2 addition results in ELVOC which are highly
oxidized multifunctional molecules (HOM). Key for efficiency
of such HOM in early particle growth is that their formation
is induced by one attack of the oxidant (here O3), followed
by an autoxidation process involving molecular oxygen.
Similar mechanisms were recently observed and predicted by
quantum mechanical calculations e.g., for isoprene. To
assess the atmospheric importance and therewith the
potential generality, it is crucial to understand the
formation pathway of HOM.To elucidate the formation path of
HOM as well as necessary and sufficient structural
prerequisites of their formation we studied homologous
series of cycloalkenes in comparison to two monoterpenes. We
were able to directly observe highly oxidized
multifunctional peroxy radicals with 8 or 10 O atoms by an
Atmospheric Pressure interface High Resolution Time of
Flight Mass Spectrometer (APi-TOF-MS) equipped with a
NO3−-chemical ionization (CI) source. In the case of O3
acting as an oxidant, the starting peroxy radical is formed
on the so-called vinylhydroperoxide path. HOM peroxy
radicals and their termination reactions with other peroxy
radicals, including dimerization, allowed for analyzing the
observed mass spectra and narrowing down the likely
formation path. As consequence, we propose that HOM are
multifunctional percarboxylic acids, with carbonyl,
hydroperoxy, or hydroxy groups arising from the termination
steps. We figured that aldehyde groups facilitate the
initial rearrangement steps. In simple molecules like
cycloalkenes, autoxidation was limited to both terminal C
atoms and two further C atoms in the respective α
positions. In more complex molecules containing tertiary H
atoms or small, constrained rings, even higher oxidation
degrees were possible, either by simple H shift of the
tertiary H atom or by initialization of complex ring-opening
reactions.},
cin = {IEK-8 / IBG-2},
ddc = {550},
cid = {I:(DE-Juel1)IEK-8-20101013 / I:(DE-Juel1)IBG-2-20101118},
pnm = {243 - Tropospheric trace substances and their
transformation processes (POF3-243) / HITEC - Helmholtz
Interdisciplinary Doctoral Training in Energy and Climate
Research (HITEC) (HITEC-20170406)},
pid = {G:(DE-HGF)POF3-243 / G:(DE-Juel1)HITEC-20170406},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000357117500012},
doi = {10.5194/acp-15-6745-2015},
url = {https://juser.fz-juelich.de/record/202148},
}