Direct observation of OH formation from stabilised Criegee intermediates

Novelli, A.; Vereecken, L.; Lelieveld, J.; Harder, H.

doi:10.1039/c4cp02719a

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Direct observation of OH formation from stabilised Criegee intermediates

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Novelli, A.
Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Vereecken, L.
Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Lelieveld, J.
Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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Harder, H.
Atmospheric Chemistry, Max Planck Institute for Chemistry, Max Planck Society;

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引用

Novelli, A., Vereecken, L., Lelieveld, J., & Harder, H. (2014). Direct observation of OH formation from stabilised Criegee intermediates. Physical Chemistry Chemical Physics, 16(37), 19941-19951. doi:10.1039/c4cp02719a.

引用: https://hdl.handle.net/11858/00-001M-0000-0024-B286-E

要旨

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.