Journal
SCIENCE
Volume 335, Issue 6065, Pages 204-207Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1213229
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Funding
- Division of Chemical Sciences, Geosciences, and Biosciences, the Office of Basic Energy Sciences, the U.S. Department of Energy
- Natural Environment Research Council
- Office of Science, Office of Basic Energy Sciences, Materials Sciences Division, of the U. S. Department of Energy at Lawrence Berkeley National Laboratory [DE-AC02-05CH11231]
- National Nuclear Security Administration [DE-AC04-94-AL85000]
- NERC [NE/G01972X/1, NE/I014381/1, NE/J009008/1, NE/I010505/1] Funding Source: UKRI
- Natural Environment Research Council [NE/I014381/1, NE/J009008/1, NE/I010505/1, NE/G01972X/1] Funding Source: researchfish
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Ozonolysis is a major tropospheric removal mechanism for unsaturated hydrocarbons and proceeds via Criegee intermediates-carbonyl oxides-that play a key role in tropospheric oxidation models. However, until recently no gas-phase Criegee intermediate had been observed, and indirect determinations of their reaction kinetics gave derived rate coefficients spanning orders of magnitude. Here, we report direct photoionization mass spectrometric detection of formaldehyde oxide (CH2OO) as a product of the reaction of CH2I with O-2. This reaction enabled direct laboratory determinations of CH2OO kinetics. Upper limits were extracted for reaction rate coefficients with NO and H2O. The CH2OO reactions with SO2 and NO2 proved unexpectedly rapid and imply a substantially greater role of carbonyl oxides in models of tropospheric sulfate and nitrate chemistry than previously assumed.
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