online molecular characterisation of organic aerosols in an atmospheric chamber using extractive electrospray ionisation mass spectrometry
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ID: 219471
2017
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Abstract
The oxidation of biogenic volatile organic compounds
(VOCs) represents a substantial source of secondary organic aerosol (SOA) in
the atmosphere. In this study, we present online measurements of the
molecular constituents formed in the gas and aerosol phases during α-pinene oxidation in the Cambridge Atmospheric Simulation Chamber (CASC). We
focus on characterising the performance of extractive electrospray ionisation
(EESI) mass spectrometry (MS) for particle analysis. A number of new aspects
of EESI-MS performance are considered here. We show that relative
quantification of organic analytes can be achieved in mixed organic–inorganic
particles. A comprehensive assignment of mass spectra for α-pinene
derived SOA in both positive and negative ion modes is obtained using an
ultra-high-resolution mass spectrometer. We compare these online spectra to
conventional offline ESI-MS spectra and find good agreement in terms of the compounds
identified, without the need for complex sample work-up procedures. Under our
experimental conditions, EESI-MS signals arise only from particle-phase
analytes. High-time-resolution (7 min) EESI-MS spectra are compared with
simulations from the near-explicit Master Chemical Mechanism (MCM) for a
range of reaction conditions. We show that MS peak abundances scale with
modelled concentrations for condensable products (pinonic acid, pinic acid,
OH-pinonic acid). Relative quantification is achieved throughout SOA
formation as the composition, size and mass (5–2400 µg m−3)
of particles is evolving. This work provides a robust demonstration of the
advantages of EESI-MS for chamber studies over offline ESI-MS (time
resolution, relative quantification) and over
hardonline techniques (molecular information).
| Reference Key |
gallimore2017atmosphericonline
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|---|---|
| Authors | ;P. J. Gallimore;C. Giorio;C. Giorio;B. M. Mahon;M. Kalberer |
| Journal | Journal of agricultural and food chemistry |
| Year | 2017 |
| DOI |
10.5194/acp-17-14485-2017
|
| URL | |
| Keywords |
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