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Analytical and Bioanalytical Chemistry

, Volume 407, Issue 20, pp 5911–5922 | Cite as

Online determination of polycyclic aromatic hydrocarbon formation from a flame soot generator

  • Laarnie Mueller
  • Gert Jakobi
  • Juergen Orasche
  • Erwin Karg
  • Martin Sklorz
  • Gülcin Abbaszade
  • Benedict Weggler
  • Lianpeng Jing
  • Juergen Schnelle-KreisEmail author
  • Ralf Zimmermann
Research Paper
Part of the following topical collections:
  1. Aerosols and Health

Abstract

In this study, we produced a class of diffusion flame soot particles with varying chemical and physical properties by using the mini-Combustion Aerosol STandard (CAST) and applying varying oxidant gas flow rates under constant propane, quenching, and dilution gas supply. We varied the soot properties by using the following fuel-to-air equivalence ratios (Φ): 1.13, 1.09, 1.04, 1.00, 0.96, and 0.89. Within this Φ range, we observed drastic changes in the physical and chemical properties of the soot. Oxidant-rich flames (Φ < 1) were characterized by larger particle size, lower particle number concentration, higher black carbon (BC) concentration, lower brown carbon BrC.[BC]−1 than fuel-rich flames (Φ > 1). To investigate the polycyclic aromatic hydrocarbons (PAH) formation online, we developed a new method for quantification by using the one 13C-containing doubly charged PAH ion in a high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS). The time-resolved concentration showed that the larger PAHs prevailed in the fuel-rich flames and diminished in the oxidant-rich flames. By comparison with the offline in situ derivatization-thermal-desorption gas-chromatography time-of-flight mass spectrometry (IDTD-GC-ToF-MS), we found that the concentration by using the HR-ToF-AMS was underestimated, especially for lower mass PAHs (C14–C18) in the fuel-rich flames possibly due to size limitation and degradation of semi-volatile species under high vacuum and desorption temperature in the latter. For oxidant-rich flames, the large PAHs (C20 and C22) were detected in the HR-ToF-AMS while it was not possible in IDTD-GC-ToF-MS due to matrix effect. The PAH formation was discussed based on the combination of our results and with respect to Φ settings.

Keywords

Aerosols/particulates Online analytical method Doubly charge isotope ion PAH formation Soot 

Notes

Acknowledgments

This work was supported by the Initiative and Networking Fund of the Helmholtz Association. We also acknowledge Ms. Kerstin Koch for the technical assistance.

Supplementary material

216_2015_8549_MOESM1_ESM.pdf (865 kb)
ESM 1 (PDF 865 kb)

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Copyright information

© Springer-Verlag Berlin Heidelberg 2015

Authors and Affiliations

  • Laarnie Mueller
    • 1
    • 2
    • 3
  • Gert Jakobi
    • 1
    • 3
  • Juergen Orasche
    • 1
    • 2
    • 3
  • Erwin Karg
    • 1
    • 3
  • Martin Sklorz
    • 2
  • Gülcin Abbaszade
    • 1
  • Benedict Weggler
    • 1
    • 2
    • 3
  • Lianpeng Jing
    • 4
  • Juergen Schnelle-Kreis
    • 1
    Email author
  • Ralf Zimmermann
    • 1
    • 2
    • 3
  1. 1.Joint Mass Spectrometry Center, Cooperation Group Comprehensive Molecular AnalyticsHelmholtz Zentrum MuenchenNeuherbergGermany
  2. 2.Joint Mass Spectrometry Centre, Chair of Analytical ChemistryInstitute of Chemistry, University of RostockRostockGermany
  3. 3.Helmholtz Virtual Institute of Complex Molecular Systems in Environmental Health (HICE)
  4. 4.Jing-Cast LtdZollikofenSwitzerland

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