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Direct measurements of conformer-dependent reactivity of the criegee intermediate CH3CHOO

Direct measurements of conformer-dependent reactivity of the criegee intermediate CH3CHOO
Direct measurements of conformer-dependent reactivity of the criegee intermediate CH3CHOO
Although carbonyl oxides, "Criegee intermediates," have long been implicated in tropospheric oxidation, there have been few direct measurements of their kinetics, and only for the simplest compound in the class, CH2OO. Here, we report production and reaction kinetics of the next larger Criegee intermediate, CH3CHOO. Moreover, we independently probed the two distinct CH3CHOO conformers, syn- and anti-, both of which react readily with SO2 and with NO2. We demonstrate that anti-CH3CHOO is substantially more reactive toward water and SO2 than is syn-CH3CHOO. Reaction with water may dominate tropospheric removal of Criegee intermediates and determine their atmospheric concentration. An upper limit is obtained for the reaction of syn-CH3CHOO with water, and the rate constant for reaction of anti-CH3CHOO with water is measured as 1.0 × 10(-14) ± 0.4 × 10(-14) centimeter(3) second(-1).
0036-8075
177-180
Taatjes, C.A.
c8715b77-7051-4e8e-a4f4-73f28223a29d
Wetz, O.
e882d93f-0aa0-4a72-b349-2f78baa7b8ef
Eskola, A.J.
313baf1e-6d2d-4243-9649-d64e7e776e98
Savee, J.D.
08f5f12b-60c5-468a-bc05-490be367cf35
Scheer, A.M.
39383d59-0448-4577-8aad-8825fc257fba
Shallcross, D.E.
9b36ee5a-feb1-4fea-a34c-f56e64dfae28
Rotavera, B.
f21c59d0-db74-4e5e-af91-27f25d9ce51a
Lee, E.P.F.
f47c6d5d-2d1f-4f03-a3ff-03658812d80b
Dyke, John M.
46393b45-6694-46f3-af20-d7369d26199f
Mok, Daniel K.W.
49a4e516-0e71-4f59-a3ec-bd607b47ef33
Osborn, D.
0f42fc79-3c65-4e97-864f-fa161f3dbdda
Percival, C.J.
30c8a344-01f8-4917-a8d2-9d161ddd111d
Taatjes, C.A.
c8715b77-7051-4e8e-a4f4-73f28223a29d
Wetz, O.
e882d93f-0aa0-4a72-b349-2f78baa7b8ef
Eskola, A.J.
313baf1e-6d2d-4243-9649-d64e7e776e98
Savee, J.D.
08f5f12b-60c5-468a-bc05-490be367cf35
Scheer, A.M.
39383d59-0448-4577-8aad-8825fc257fba
Shallcross, D.E.
9b36ee5a-feb1-4fea-a34c-f56e64dfae28
Rotavera, B.
f21c59d0-db74-4e5e-af91-27f25d9ce51a
Lee, E.P.F.
f47c6d5d-2d1f-4f03-a3ff-03658812d80b
Dyke, John M.
46393b45-6694-46f3-af20-d7369d26199f
Mok, Daniel K.W.
49a4e516-0e71-4f59-a3ec-bd607b47ef33
Osborn, D.
0f42fc79-3c65-4e97-864f-fa161f3dbdda
Percival, C.J.
30c8a344-01f8-4917-a8d2-9d161ddd111d

Taatjes, C.A., Wetz, O., Eskola, A.J., Savee, J.D., Scheer, A.M., Shallcross, D.E., Rotavera, B., Lee, E.P.F., Dyke, John M., Mok, Daniel K.W., Osborn, D. and Percival, C.J. (2013) Direct measurements of conformer-dependent reactivity of the criegee intermediate CH3CHOO. Science, 340 (6129), 177-180. (doi:10.1126/science.1234689). (PMID:23580524)

Record type: Article

Abstract

Although carbonyl oxides, "Criegee intermediates," have long been implicated in tropospheric oxidation, there have been few direct measurements of their kinetics, and only for the simplest compound in the class, CH2OO. Here, we report production and reaction kinetics of the next larger Criegee intermediate, CH3CHOO. Moreover, we independently probed the two distinct CH3CHOO conformers, syn- and anti-, both of which react readily with SO2 and with NO2. We demonstrate that anti-CH3CHOO is substantially more reactive toward water and SO2 than is syn-CH3CHOO. Reaction with water may dominate tropospheric removal of Criegee intermediates and determine their atmospheric concentration. An upper limit is obtained for the reaction of syn-CH3CHOO with water, and the rate constant for reaction of anti-CH3CHOO with water is measured as 1.0 × 10(-14) ± 0.4 × 10(-14) centimeter(3) second(-1).

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Published date: 12 April 2013
Organisations: Chemistry

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Local EPrints ID: 351486
URI: http://eprints.soton.ac.uk/id/eprint/351486
ISSN: 0036-8075
PURE UUID: 18663d90-fffe-4a20-a9da-c9114cf94fa6
ORCID for John M. Dyke: ORCID iD orcid.org/0000-0002-9808-303X

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Date deposited: 22 Apr 2013 14:31
Last modified: 17 Dec 2019 02:04

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Contributors

Author: C.A. Taatjes
Author: O. Wetz
Author: A.J. Eskola
Author: J.D. Savee
Author: A.M. Scheer
Author: D.E. Shallcross
Author: B. Rotavera
Author: E.P.F. Lee
Author: John M. Dyke ORCID iD
Author: Daniel K.W. Mok
Author: D. Osborn
Author: C.J. Percival

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