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Observation of the simplest Criegee intermediate CH[subscript 2]OO in the gas-phase ozonolysis of ethylene

Author(s)
Womack, Caroline C.; Martin-Drumel, Marie-Aline; Brown, Gordon G.; Field, Robert W.; McCarthy, Michael C.
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Abstract
Ozonolysis is one of the dominant oxidation pathways for tropospheric alkenes. Although numerous studies have confirmed a 1,3-cycloaddition mechanism that generates a Criegee intermediate (CI) with form R[subscript 1]R[subscript 2]COO, no small CIs have ever been directly observed in the ozonolysis of alkenes because of their high reactivity. We present the first experimental detection of CH[subscript 2]OO in the gas-phase ozonolysis of ethylene, using Fourier transform microwave spectroscopy and a modified pulsed nozzle, which combines high reactant concentrations with rapid sampling and sensitive detection. Nine other product species of the O[subscript 3] + C[subscript 2]H[subscript 4] reaction were also detected, including formaldehyde, formic acid, dioxirane, and ethylene ozonide. The presence of all these species can be attributed to the unimolecular and bimolecular reactions of CH[subscript 2]OO, and their abundances are in qualitative agreement with published mechanisms and rate constants.
Date issued
2015-03
URI
http://hdl.handle.net/1721.1/96419
Department
Massachusetts Institute of Technology. Department of Chemistry
Journal
Science Advances
Publisher
American Association for the Advancement of Science (AAAS)
Citation
Womack, C. C., M.-A. Martin-Drumel, G. G. Brown, R. W. Field, and M. C. McCarthy. “Observation of the Simplest Criegee Intermediate CH[subscript 2]OO in the Gas-Phase Ozonolysis of Ethylene.” Science Advances 1, no. 2 (March 1, 2015): e1400105–e1400105.
Version: Final published version
ISSN
2375-2548

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