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Issue 37, 2014
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Direct observation of OH formation from stabilised Criegee intermediates

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Abstract

The syn-CH3CHOO Criegee intermediate formed from the ozonolysis of propene and (E)-2-butene was detected via unimolecular decomposition and subsequent detection of OH radicals by a LIF-FAGE instrument. An observed time dependent OH concentration profile was analysed using a detailed model focusing on the speciated chemistry of Criegee intermediates based on the recent literature. The absolute OH concentration was found to depend on the steady state concentration of syn-CH3CHOO at the injection point while the time dependence of the OH concentration profile was influenced by the sum of the rates of unimolecular decomposition of syn-CH3CHOO and wall loss. By varying the most relevant parameters influencing the SCI chemistry in the model and based on the temporal OH concentration profile, the unimolecular decomposition rate k (293 K) of syn-CH3CHOO was shown to lie within the range 3–30 s−1, where a value of 20 ± 10 s−1 yields the best agreement with the CI chemistry literature.

Graphical abstract: Direct observation of OH formation from stabilised Criegee intermediates

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Publication details

The article was received on 20 Jun 2014, accepted on 04 Aug 2014 and first published on 07 Aug 2014


Article type: Paper
DOI: 10.1039/C4CP02719A
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Citation: Phys. Chem. Chem. Phys., 2014,16, 19941-19951
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    Direct observation of OH formation from stabilised Criegee intermediates

    A. Novelli, L. Vereecken, J. Lelieveld and H. Harder, Phys. Chem. Chem. Phys., 2014, 16, 19941
    DOI: 10.1039/C4CP02719A

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