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Photoenhanced ozone loss on solid pyrene films.

Sarah A Styler1, Marcello Brigante, Barbara D'Anna

  • 1Department of Chemistry, University of Toronto, Toronto, Ontario, Canada M5S 3H6.

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This study reveals that UV light significantly enhances ozone reactions with pyrene films, affecting both ozone uptake and pyrene degradation through distinct surface mechanisms. Understanding these heterogeneous reactions is crucial for atmospheric chemistry.

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Area of Science:

  • Atmospheric Chemistry
  • Heterogeneous Reactions
  • Photochemistry

Background:

  • Ozone is a key atmospheric oxidant involved in numerous gas-phase and heterogeneous reactions.
  • Polycyclic aromatic hydrocarbons like pyrene are present in the atmosphere and can react with ozone.
  • Understanding the kinetics and mechanisms of these reactions is vital for air quality modeling.

Purpose of the Study:

  • To investigate the heterogeneous reaction kinetics of gas-phase ozone with solid pyrene films.
  • To determine the influence of near-UV radiation on ozone uptake and pyrene degradation.
  • To elucidate the underlying surface reaction mechanisms, including light-enhanced pathways.

Main Methods:

  • Utilized a coated-wall flow tube system to measure ozone uptake by pyrene films.
  • Employed laser-induced fluorescence to monitor pyrene loss within the film upon ozone exposure.
  • Investigated the effects of ozone concentration, UV-A radiation, and relative humidity.

Main Results:

  • Both ozone uptake and pyrene loss followed a Langmuir-Hinshelwood-type surface mechanism.
  • Near-UV radiation significantly increased the reactive uptake coefficient of ozone by pyrene films.
  • Light enhanced pyrene loss, but less so than ozone uptake, with humidity decreasing the uptake coefficient.

Conclusions:

  • A proposed mechanism involves light-enhanced ozone uptake via excited pyrene reactions with O2(1Σg+).
  • Enhanced pyrene loss is attributed to a charge-transfer complex between excited pyrene and ozone.
  • Disparities in gas-phase versus surface results highlight the importance of multifaceted experimental approaches.