Kinetics of NO3 Uptake on Pyrene as a Representative Organic Aerosols

Kinetics of NO3 Uptake on Pyrene as a Representative Organic Aerosols The uptake of NO3 on a pyrene coating at [NO3] = 2.5 × 1012–1.2 × 1013 cm−3 is studied using a coated-insert flow tube reactor coupled to a mass spectrometer. It is established that, in this concentration range, the uptake occurs by the impact recombination mechanism, whereas the consumption of surface sites involves the unimolecular decomposition of stabilized surface complexes. Several hundreds of NO3 radicals are consumed per surface site destroyed. The uptake coefficient depends on the exposure time, being described by the expression γ(t) = γ0exp(−t/τ), where γ0 and τ are parameters dependent on the NO3 concentration. Based on the Langmuir adsorption concept, the following elementary parameters determining the uptake process are estimated: the Langmuir coefficient, K L = 7.1 × 10−13 cm3; the desorption rate constant, k d = 44 s−1; and the rate constant for the unimolecular heterogeneous conversion of surface complexes, k r = 6.6 × 10−2 s−1. Gas chromatography–mass spectrometry measurements showed that the main products of the reaction are phthalates. The nitropyrene yield is found to be ~0.6%. http://www.deepdyve.com/assets/images/DeepDyve-Logo-lg.png Russian Journal of Physical Chemistry B Springer Journals

Kinetics of NO3 Uptake on Pyrene as a Representative Organic Aerosols

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Publisher
Pleiades Publishing
Copyright
Copyright © 2018 by Pleiades Publishing, Ltd.
Subject
Chemistry; Physical Chemistry
ISSN
1990-7931
eISSN
1990-7923
D.O.I.
10.1134/S1990793118020136
Publisher site
See Article on Publisher Site

Abstract

The uptake of NO3 on a pyrene coating at [NO3] = 2.5 × 1012–1.2 × 1013 cm−3 is studied using a coated-insert flow tube reactor coupled to a mass spectrometer. It is established that, in this concentration range, the uptake occurs by the impact recombination mechanism, whereas the consumption of surface sites involves the unimolecular decomposition of stabilized surface complexes. Several hundreds of NO3 radicals are consumed per surface site destroyed. The uptake coefficient depends on the exposure time, being described by the expression γ(t) = γ0exp(−t/τ), where γ0 and τ are parameters dependent on the NO3 concentration. Based on the Langmuir adsorption concept, the following elementary parameters determining the uptake process are estimated: the Langmuir coefficient, K L = 7.1 × 10−13 cm3; the desorption rate constant, k d = 44 s−1; and the rate constant for the unimolecular heterogeneous conversion of surface complexes, k r = 6.6 × 10−2 s−1. Gas chromatography–mass spectrometry measurements showed that the main products of the reaction are phthalates. The nitropyrene yield is found to be ~0.6%.

Journal

Russian Journal of Physical Chemistry BSpringer Journals

Published: May 29, 2018

References

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