CaltechAUTHORS
Published July 7, 2020 | Version Supplemental Material
Journal Article Open

Photo-oxidation of aromatic hydrocarbons produces low-volatility organic compounds

Creators

  • 1. ROR icon Carnegie Mellon University
  • 2. ROR icon Paul Scherrer Institute
  • 3. ROR icon University of Vienna
  • 4. ROR icon Aerodyne Research
  • 5. ROR icon Goethe University Frankfurt
  • 6. ROR icon University of Colorado Boulder
  • 7. ROR icon University of Lisbon
  • 8. ROR icon University of Helsinki
  • 9. ROR icon Helsinki Institute of Physics
  • 10. ROR icon ETH Zurich
  • 11. ROR icon California Institute of Technology
  • 12. ROR icon Pusan National University
  • 13. ROR icon P.N. Lebedev Physical Institute of the Russian Academy of Sciences
  • 14. ROR icon Finnish Meteorological Institute
  • 15. ROR icon Universität Innsbruck
  • 16. ROR icon Tampere University
  • 17. ROR icon University of Beira Interior
  • 18. ROR icon European Organization for Nuclear Research
  • 19. ROR icon Nanjing University
  • 20. ROR icon Beijing University of Chemical Technology

Abstract

To better understand the role of aromatic hydrocarbons in new-particle formation, we measured the particle-phase abundance and volatility of oxidation products following the reaction of aromatic hydrocarbons with OH radicals. For this we used thermal desorption in an iodide-adduct Time-of-Flight Chemical-Ionization Mass Spectrometer equipped with a Filter Inlet for Gases and AEROsols (FIGAERO-ToF-CIMS). The particle-phase volatility measurements confirm that oxidation products of toluene and naphthalene can contribute to the initial growth of newly formed particles. Toluene-derived (C₇) oxidation products have a similar volatility distribution to that of α-pinene-derived (C₁₀) oxidation products, while naphthalene-derived (C₁₀) oxidation products are much less volatile than those from toluene or α-pinene; they are thus stronger contributors to growth. Rapid progression through multiple generations of oxidation is more pronounced in toluene and naphthalene than in α-pinene, resulting in more oxidation but also favoring functional groups with much lower volatility per added oxygen atom, such as hydroxyl and carboxylic groups instead of hydroperoxide groups. Under conditions typical of polluted urban settings, naphthalene may well contribute to nucleation and the growth of the smallest particles, whereas the more abundant alkyl benzenes may overtake naphthalene once the particles have grown beyond the point where the Kelvin effect strongly influences the condensation driving force.

Additional Information

© 2020 American Chemical Society. Received: April 4, 2020; Revised: June 2, 2020; Accepted: June 9, 2020; Published: June 9, 2020. We thank the European Organization for Nuclear Research (CERN) for supporting CLOUD with important technical and financial resources and for providing a particle beam from the CERN Proton Synchrotron. This research has received funding from the U.S. National Science Foundation under grants AGS-1447056, AGS-1439551, AGS-1649147, AGS-1602086, and AGS-1801897; the German Federal Ministry of Education and Research (No. 01LK1601A); ERC-Consolidator Grant NANODYNAMITE 616075; Horizon 2020 Marie Skłodowska-Curie Grant 656994 ("Nano-CAVa"); ERC Advanced "ATM-GP" grant No. 227463; the Presidium of the Russian Academy of Sciences, the Program "High energy physics and neutrino astrophysics" 2015; the Swiss National Science Foundation Projects 200020_152907, 20FI20_159851, 200021_169090, 200020_172602, and 20FI20_172622. The FIGAERO–CIMS was supported by an MRI grant for the U.S. NSF AGS-1531284 as well as the Wallace Research Foundation. O.G. thanks the Doctoral Programme in Atmospheric Sciences at the University of Helsinki for financial support. Author Contributions: M.W., D.C., M.X., J.K., D.R.W., U.B., J.Do., I.E.-H., and N.M.D. designed the research; M.W., D.C., M.X., Q.Y., D.S., V.H., P.Y., A.L.V., R.L.M., A.A., A.B., B.B., S.B., L.D., A.D., J.Du., H.F., O.G., X.H., C.R.H., C.K., A.K., K.L., F.L., U.M., T.P., V.P., L.L. J.Q., M.R., M.S., C.T., A.T., A.C.W., L.W., J.K., J.Do., and I.E.-H. performed the research; M.W., M.X., D.S., and N.M.D. contributed new reagents/analytic tools; M.W., M.X., D.S., P.Y., and M.S. analyzed the data; and M.W., D.C., M.X., A.L.V., U.M., J.K., U.B., J.Do., I.E.-H., and N.M.D. wrote the paper. The authors declare no competing financial interest.

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Additional details

Identifiers

Eprint ID
103803
Resolver ID
CaltechAUTHORS:20200609-144136778

Funding

CERN
NSF
AGS-1447056
NSF
AGS-1439551
NSF
AGS-1649147
NSF
AGS-1602086
NSF
AGS-1801897
Bundesministerium für Bildung und Forschung (BMBF)
01LK1601A
European Research Council (ERC)
616075
Marie Curie Fellowship
656994
European Research Council (ERC)
227463
Presidium of the Russian Academy of Sciences
Swiss National Science Foundation (SNSF)
200020_152907
Swiss National Science Foundation (SNSF)
20FI20_159851
Swiss National Science Foundation (SNSF)
200021_169090
Swiss National Science Foundation (SNSF)
200020_172602
Swiss National Science Foundation (SNSF)
20FI20_172622
NSF
AGS-1531284
Wallace Research Foundation
University of Helsinki

Dates

Created
2020-06-09
Created from EPrint's datestamp field
Updated
2021-11-16
Created from EPrint's last_modified field