Criegee intermediates and their impacts on the troposphere
Abstract
We report Criegee intermediates (CIs), carbonyl oxides formed in ozonolysis of alkenes, play key roles in the troposphere. The decomposition of CIs can be a significant source of OH to the tropospheric oxidation cycle especially during nighttime and winter months. A variety of model-measurement studies have estimated surface-level stabilized Criegee intermediate (sCI) concentrations on the order of 1 × 104 cm-3 to 1 × 105 cm-3, which makes a non-negligible contribution to the oxidising capacity in the terrestrial boundary layer. The reactions of sCI with the water monomer and the water dimer have been found to be the most important bimolecular reactions to the tropospheric sCI loss rate, at least for the smallest carbonyl oxides; the products from these reactions (e.g. hydroxymethyl hydroperoxide, HMHP) are also of importance to the atmospheric oxidation cycle. The sCI can oxidise SO2 to form SO3, which can go on to form a significant amount of H2SO4 which is a key atmospheric nucleation species and therefore vital to the formation of clouds. Lastly, the sCI can also react with carboxylic acids, carbonyl compounds, alcohols, peroxy radicals and hydroperoxides, and the products of these reactions are likely to be highly oxygenated species, with low vapour pressures,more »
- Authors:
-
[1];
[2];
[3];
[3];
[1]
- University of Bristol (United Kingdom). School of Chemistry
- California Inst. of Technology (CalTech), Pasadena, CA (United States). Jet Propulsion Laboratory
- Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1426808
- Report Number(s):
- SAND-2018-1551J
Journal ID: ISSN 2050-7887; ESPICZ; 660688
- Grant/Contract Number:
- AC04-94AL85000; NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science: Processes & Impacts
- Additional Journal Information:
- Journal Volume: 20; Journal Issue: 3; Journal ID: ISSN 2050-7887
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES
Citation Formats
Khan, M. A. H., Percival, C. J., Caravan, R. L., Taatjes, C. A., and Shallcross, D. E.. Criegee intermediates and their impacts on the troposphere. United States: N. p., 2018.
Web. doi:10.1039/C7EM00585G.
Khan, M. A. H., Percival, C. J., Caravan, R. L., Taatjes, C. A., & Shallcross, D. E.. Criegee intermediates and their impacts on the troposphere. United States. https://doi.org/10.1039/C7EM00585G
Khan, M. A. H., Percival, C. J., Caravan, R. L., Taatjes, C. A., and Shallcross, D. E.. Thu .
"Criegee intermediates and their impacts on the troposphere". United States. https://doi.org/10.1039/C7EM00585G. https://www.osti.gov/servlets/purl/1426808.
@article{osti_1426808,
title = {Criegee intermediates and their impacts on the troposphere},
author = {Khan, M. A. H. and Percival, C. J. and Caravan, R. L. and Taatjes, C. A. and Shallcross, D. E.},
abstractNote = {We report Criegee intermediates (CIs), carbonyl oxides formed in ozonolysis of alkenes, play key roles in the troposphere. The decomposition of CIs can be a significant source of OH to the tropospheric oxidation cycle especially during nighttime and winter months. A variety of model-measurement studies have estimated surface-level stabilized Criegee intermediate (sCI) concentrations on the order of 1 × 104 cm-3 to 1 × 105 cm-3, which makes a non-negligible contribution to the oxidising capacity in the terrestrial boundary layer. The reactions of sCI with the water monomer and the water dimer have been found to be the most important bimolecular reactions to the tropospheric sCI loss rate, at least for the smallest carbonyl oxides; the products from these reactions (e.g. hydroxymethyl hydroperoxide, HMHP) are also of importance to the atmospheric oxidation cycle. The sCI can oxidise SO2 to form SO3, which can go on to form a significant amount of H2SO4 which is a key atmospheric nucleation species and therefore vital to the formation of clouds. Lastly, the sCI can also react with carboxylic acids, carbonyl compounds, alcohols, peroxy radicals and hydroperoxides, and the products of these reactions are likely to be highly oxygenated species, with low vapour pressures, that can lead to nucleation and SOA formation over terrestrial regions.},
doi = {10.1039/C7EM00585G},
journal = {Environmental Science: Processes & Impacts},
number = 3,
volume = 20,
place = {United States},
year = {2018},
month = {2}
}
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Figure 1: Formation of a primary ozonide followed by decomposition to a carbonyl and Criegee intermediate
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Works referencing / citing this record:
Investigating the Tropospheric Chemistry of Acetic Acid Using the Global 3‐D Chemistry Transport Model, STOCHEM‐CRI
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Rapid unimolecular reaction of stabilized Criegee intermediates and implications for atmospheric chemistry
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Calculation of the absolute photoionization cross-sections for C1–C4 Criegee intermediates and vinyl hydroperoxides
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Fourier-transform microwave spectroscopy on weakly bound complexes of CH 2 OO with Ar, CO, and N 2
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Unimolecular decay dynamics of Criegee intermediates: Energy-resolved rates, thermal rates, and their atmospheric impact
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