Issue 6, 2021

Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry

Abstract

Aerosol particles negatively affect human health while also having climatic relevance due to, for example, their ability to act as cloud condensation nuclei. Ultrafine particles (diameter Dp < 100 nm) typically comprise the largest fraction of the total number concentration, however, their chemical characterization is difficult because of their low mass. Using an extractive electrospray time-of-flight mass spectrometer (EESI-TOF), we characterize the molecular composition of freshly nucleated particles from naphthalene and β-caryophyllene oxidation products at the CLOUD chamber at CERN. We perform a detailed intercomparison of the organic aerosol chemical composition measured by the EESI-TOF and an iodide adduct chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols (FIGAERO-I-CIMS). We also use an aerosol growth model based on the condensation of organic vapors to show that the chemical composition measured by the EESI-TOF is consistent with the expected condensed oxidation products. This agreement could be further improved by constraining the EESI-TOF compound-specific sensitivity or considering condensed-phase processes. Our results show that the EESI-TOF can obtain the chemical composition of particles as small as 20 nm in diameter with mass loadings as low as hundreds of ng m−3 in real time. This was until now difficult to achieve, as other online instruments are often limited by size cutoffs, ionization/thermal fragmentation and/or semi-continuous sampling. Using real-time simultaneous gas- and particle-phase data, we discuss the condensation of naphthalene oxidation products on a molecular level.

Graphical abstract: Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry

Supplementary files

Article information

Article type
Paper
Submitted
26 Jun 2021
Accepted
10 Aug 2021
First published
23 Aug 2021
This article is Open Access
Creative Commons BY-NC license

Environ. Sci.: Atmos., 2021,1, 434-448

Molecular characterization of ultrafine particles using extractive electrospray time-of-flight mass spectrometry

M. Surdu, V. Pospisilova, M. Xiao, M. Wang, B. Mentler, M. Simon, D. Stolzenburg, C. R. Hoyle, D. M. Bell, C. P. Lee, H. Lamkaddam, F. Lopez-Hilfiker, L. R. Ahonen, A. Amorim, A. Baccarini, D. Chen, L. Dada, J. Duplissy, H. Finkenzeller, X. He, V. Hofbauer, C. Kim, A. Kürten, A. Kvashnin, K. Lehtipalo, V. Makhmutov, U. Molteni, W. Nie, A. Onnela, T. Petäjä, L. L. J. Quéléver, C. Tauber, A. Tomé, R. Wagner, C. Yan, A. S. H. Prevot, J. Dommen, N. M. Donahue, A. Hansel, J. Curtius, P. M. Winkler, M. Kulmala, R. Volkamer, R. C. Flagan, J. Kirkby, D. R. Worsnop, J. G. Slowik, D. S. Wang, U. Baltensperger and I. E. Haddad, Environ. Sci.: Atmos., 2021, 1, 434 DOI: 10.1039/D1EA00050K

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