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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 (CH(2)OO) as a product of the reaction of CH(2)I with O(2). This reaction enabled direct laboratory determinations of CH(2)OO kinetics. Upper limits were extracted for reaction rate coefficients with NO and H(2)O. The CH(2)OO reactions with SO(2) and NO(2) proved unexpectedly rapid and imply a substantially greater role of carbonyl oxides in models of tropospheric sulfate and nitrate chemistry than previously assumed.
|Translated title of the contribution||Direct Kinetic Measurements of Criegee Intermediate (CH(2)OO) Formed by Reaction of CH(2)I with O(2)|
|Pages (from-to)||204 - 207|
|Number of pages||4|
|Publication status||Published - Jan 2012|
Bibliographical noteAuthor of Publication Reviewed: Welz, O ; Savee, JD ; Osborn, DL ; Vasu, SS; Percival, CJ ; Shallcross, DE ; Taatjes, CA
Publisher: AMER ASSOC ADVANCEMENT SCIENCE
The gas phase atmospheric photolysis and reactions of key alkyl nitrates and their role in NOy partitioning.
1/10/09 → 1/04/13