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@ARTICLE{Luo:1008188,
author = {Luo, Hao and Vereecken, Luc and Shen, Hongru and Kang,
Sungah and Pullinen, Iida and Hallquist, Mattias and Fuchs,
Hendrik and Wahner, Andreas and Kiendler-Scharr, Astrid and
Mentel, Thomas F. and Zhao, Defeng},
title = {{F}ormation of highly oxygenated organic molecules from the
oxidation of limonene by {OH} radical: significant
contribution of {H}-abstraction pathway},
reportid = {FZJ-2023-02234},
year = {2022},
abstract = {Highly oxygenated organic molecules (HOM) play a pivotal
role in the formation of secondary organic aerosol (SOA).
Therefore, the distribution and yields of HOM are
fundamental to understand their fate and chemical evolution
in the atmosphere, and it is conducive to ultimately assess
the impact of SOA on air quality and climate change. In this
study, gas-phase HOM formed from the reaction of limonene
with OH radical in photooxidation were investigated in the
SAPHIR chamber (Simulation of Atmospheric PHotochemistry In
a large Reaction chamber) using a time-of-flight chemical
ionization mass spectrometer with nitrate reagent ion
(NO3−-CIMS). A large number of HOM, including monomers
(C9–10) and dimers (C17–20), were detected and
classified into various families. Both closed-shell products
and open-shell peroxy radicals (RO2), were identified under
low NO (0.1 ppt–~0.2 ppb) and high NO conditions (17 ppb).
C10 monomers are the most abundant HOM products and account
for over 80 $\%$ total HOM. Closed-shell C10 monomers were
formed from two peroxy radical familie,
C10H15Ox•(x=7–12) and C10H17Ox•(x=8–13), and their
respective termination reactions with NO, RO2, and HO2.
While C10H17Ox• is likely formed by OH addition to C10H16,
the dominant initial step of limonene+OH, C10H15Ox•, is
likely formed via H-abstraction by OH. C10H15Ox• and
related products contributed 43 $\%$ and 46 $\%$ of C10-HOM
at low and high NO, demonstrating that H-abstraction
pathways play a significant role in HOM formation in the
reaction of limonene+OH. Combining theoretical kinetic
calculations, structure activity relationships (SARs),
literature data, and the observed RO2 intensities, we
proposed tentative mechanisms of HOM formation from both
pathways. We further estimated the molar yields of HOM to be
3.04−1.64+3.89 $\%$ and 0.82−0.44+1.05 $\%$ at low and
high NO, respectively. Our study highlights the importance
of H-abstraction by OH and provides yield and tentative
pathways in the OH oxidation of limonene to simulate the HOM
formation and assess their role in SOA formation.},
cin = {IEK-8},
cid = {I:(DE-Juel1)IEK-8-20101013},
pnm = {2111 - Air Quality (POF4-211)},
pid = {G:(DE-HGF)POF4-2111},
typ = {PUB:(DE-HGF)25},
doi = {10.5194/acp-2022-803},
url = {https://juser.fz-juelich.de/record/1008188},
}