Chlorine-initiated oxidation of <i>n</i>-alkanes under high-NO<sub><i>x</i></sub> conditions: insights into secondary organic aerosol composition and volatility using a FIGAERO–CIMS
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Published:2018-10-30
Issue:21
Volume:18
Page:15535-15553
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ISSN:1680-7324
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Container-title:Atmospheric Chemistry and Physics
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language:en
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Short-container-title:Atmos. Chem. Phys.
Author:
Wang Dongyu S.ORCID, Hildebrandt Ruiz LeaORCID
Abstract
Abstract. Chlorine-initiated oxidation of n-alkanes (C8−12) under high-nitrogen oxide conditions was investigated. Observed secondary organic
aerosol yields (0.16 to 1.65) are higher than those for OH-initiated
oxidation of C8−12 alkanes (0.04 to 0.35). A high-resolution
time-of-flight chemical ionization mass spectrometer coupled to a Filter
Inlet for Gases and AEROsols (FIGAERO–CIMS) was used to characterize the gas-
and particle-phase molecular composition. Chlorinated organics were observed,
which likely originated from chlorine addition to the double bond present on
the heterogeneously produced dihydrofurans. A two-dimensional thermogram
representation was developed to visualize the composition and relative volatility
of organic aerosol components using unit-mass resolution data. Evidence of
oligomer formation and thermal decomposition was observed. Aerosol yield and
oligomer formation were suppressed under humid conditions (35 % to
67 % RH) relative to dry conditions (under 5 % RH). The temperature
at peak desorption signal, Tmax, a proxy for aerosol volatility,
was shown to change with aerosol filter loading, which should be constrained
when evaluating aerosol volatilities using the FIGAERO–CIMS. Results suggest
that long-chain anthropogenic alkanes could contribute significantly to
ambient aerosol loading over their atmospheric lifetime.
Funder
Welch Foundation National Science Foundation
Publisher
Copernicus GmbH
Subject
Atmospheric Science
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