Unimolecular Reaction Rate Measurement of syn -CH3 CHOO

The Journal of Physical Chemistry Letters
Xiaohu ZhouXueming Yang

Abstract

The unimolecular reactions of Criegee intermediates (CIs) are thought to be one of the significant sources of atmospheric OH radicals. However, stark discrepancies exist in the unimolecular reaction rate of the methyl-substituted CI CH3CHOO, typically from ozonolysis of alkenes such as trans-2-butene, between the results of ozonolysis of alkene experiments and the up-to-date theoretical calculations. That no further progress has been made since the method that directly produces CIs in the laboratory was developed is mostly attributed to the existence of two conformers, syn- and anti-CH3CHOO, and the methodological limitations of sensitive conformer-specific detection. We report a conformer-specific measurement of the unimolecular reaction rate of syn-CH3CHOO by using a high-repetition-rate laser-induced fluorescence method. At 298 K, the observed value of 182 ± 66 s-1 is in good agreement with recent theoretical calculations.

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Citations

Jun 8, 2021·Physical Chemistry Chemical Physics : PCCP·Xiaohu ZhouXueming Yang
Jun 3, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Michael F VanscoRebecca L Caravan
Jul 28, 2021·The Journal of Physical Chemistry. a·Mei-Tsan KuoKaito Takahashi
Jul 3, 2020·The Journal of Physical Chemistry. a·Xiaohu ZhouXueming Yang
Sep 25, 2021·The Journal of Physical Chemistry. a·Siyue LiuWenrui Dong

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