Chemical Kinetic Study of the Reaction of CH2OO with CH3O2
JOURNAL OF PHYSICAL CHEMISTRY LETTERS(2024)
摘要
Criegee intermediates play an important role in the oxidizing capacity of the Earth's troposphere. Although extensive studies have been conducted on Criegee intermediates in the past decade, their kinetics with radical species remain underexplored. We investigated the kinetics of the simplest Criegee intermediate, CH2 OO, with the methyl peroxy radical, CH3 O2 , as a model system to explore the reactivities of Criegee intermediates with peroxy radicals. Using a multipass UV-Vis spectrometer coupled to a pulsed-laser photolysis flow reactor, CH2 OO and CH3 O2 were generated simultaneously from the photolysis of CH2 I2 /CH3 I/O2 /N2 mixtures with CH2 OO measured directly near 340 nm. We determined a reaction rate coefficient kCH2 OO+CH3 O2 = (1.7 +/- 0.5) x 10-11 cm3 s-1 at 294 K and 10 Torr, where the influence of iodine adducts is reduced. This rate coefficient is faster than previous theoretical predictions, highlighting the challenges in accurately describing the interaction between zwitterionic and biradical characteristics of Criegee intermediates.
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