Atmospheric Chemistry of Perfluorinated Aldehyde Hydrates (n-CxF2x+1CH(OH)2,x= 1, 3, 4): Hydration, Dehydration, and Kinetics and Mechanism of Cl Atom and OH Radical Initiated Oxidation

Sulbaek Andersen, M. P.; Toft, A.; Nielsen, O. J.; Hurley, M. D.; Wallington, T. J.; Chishima, H.; Tonokura, K.; Mabury, S. A.; Martin, J. W.; Ellis, D. A.

doi:10.1021/jp060404z

Cited by 30Atmospheric chemistry and aerosolsAtmospheric Ozone and ClimatePer- and polyfluoroalkyl substances research

Atmospheric Chemistry of Perfluorinated Aldehyde Hydrates (n-CxF2x+1CH(OH)2,x= 1, 3, 4): Hydration, Dehydration, and Kinetics and Mechanism of Cl Atom and OH Radical Initiated Oxidation

Sulbaek Andersen, M. P., Toft, A., Nielsen, O. J., Hurley, M. D., Wallington, T. J., Chishima, H., Tonokura, K., Mabury, S. A. +2 more·2006·The Journal of Physical Chemistry A

DOI 10.1021/jp060404z

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Abstract

Smog chamber/Fourier transform infrared (FTIR) techniques were used to measure k(Cl+C(x)F(2x+1)CH(OH)(2)) (x = 1, 3, 4) = (5.84 +/- 0.92) x 10(-13) and k(OH+C(x)F(2x+1)CH(OH)(2)) = (1.22 +/- 0.26) x 10(-13) cm(3) molecule(-1) s(-1) in 700 Torr of N(2) or air at 296 +/- 2 K. The Cl initiated oxidation of CF(3)CH(OH)(2) in 700 Torr of air gave CF(3)COOH in a molar yield of 101 +/- 6%. IR spectra of C(x)F(2x+1)CH(OH)(2) (x = 1, 3, 4) were recorded and are presented. An upper limit of k(CF(3)CHO+H(2)O) < 2 x 10(-23) cm(3) molecule(-1) s(-1) was established for the gas-phase hydration of CF(3)CHO. Bubbling CF(3)CHO/air mixtures through liquid water led to >80% conversion of CF(3)CHO into the hydrate within the approximately 2 s taken for passage through the bubbler. These results suggest that OH radical initiated oxidation of C(x)F(2x+1)CH(OH)(2) hydrates could be a significant source of perfluorinated carboxylic acids in the environment.

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The reaction of OH radicals with the hydrated form of CF3CHO in the gas phase is known to be an effective route for formation of TFA (100%).
“The reaction of OH radicals with the hydrated form of CF3CHO in the gas phase is known to be an effective route for formation of TFA (100%) [211]”
From Changes in tropospheric air quality related to the protection of stratospheric ozone in a changing climate (2023) · cites this paper as [211]

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Authors: Sulbaek Andersen, M. P., Toft, A., Nielsen, O. J., Hurley, M. D., Wallington, T. J., Chishima, H., Tonokura, K., Mabury, S. A., Martin, J. W., & Ellis, D. A.
Affiliations: Department of Chemistry, University of Copenhagen, Universitet sparken 5, DK-2100 Copenhagen, Denmark, Department of Chemistry, University of Southern Denmark, Campusvej 55, DK-5230 Odense M, Denmark, Ford Motor Company, P. O. Box 2053, Dearborn, Michigan 48121-2053, Environmental Science Center, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan, and Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, Ontario, Canada M5S 3H6
University of Copenhagen (DK)
ORCID: Nielsen, O. J.
Hurley, M. D.
Wallington, T. J.
Tonokura, K.
Mabury, S. A.
Martin, J. W.
Venue: The Journal of Physical Chemistry A
Publisher: American Chemical Society (ACS)
Published: 2006-07-20
Volume: 110
Issue: 32
Pages: 9854-9860
ISSN: 1089-5639 (ISSN-L)
1520-5215
DOI: 10.1021/jp060404z
OpenAlex: W1979336000
Cited by: 30
References: 22
Citations by year: 2026: 1 · 2025: 3 · 2023: 2 · 2017: 1 · 2016: 1 · 2015: 4 · 2014: 2 · 2013: 2
FWCI: 1.74
Type: journal article
Language: en
Open access: closed
Locations: The Journal of Physical Chemistry A (publishedVersion)
PubMed (publishedVersion)
Research at the University of Copenhagen (University of Copenhagen) (submittedVersion)
Topics: Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric chemistry and aerosols
Physical Sciences › Earth and Planetary Sciences › Atmospheric Science › Atmospheric Ozone and Climate
Physical Sciences › Environmental Science › Environmental Chemistry › Per- and polyfluoroalkyl substances research
Keywords: chlorine atom oxidation, hydroxyl radical oxidation, gas-phase hydration, dehydration, reaction kinetics, reaction mechanism, perfluorinated carboxylic acids, atmospheric chemistry, smog chamber experiments

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Atmospheric Chemistry of Perfluorinated Aldehyde Hydrates (n-CxF2x+1CH(OH)2,x= 1, 3, 4): Hydration, Dehydration, and Kinetics and Mechanism of Cl Atom and OH Radical Initiated Oxidation

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