D/H kinetic isotope effect in the reaction CH sub(4)+Cl

The D/H kinetic isotope effect (KIE sub(Cl) super(D)) in the reaction of CH sub(4) with Cl has been investigated using a tunable diode laser absorption spectrometer (TDLAS) to measure super(12)CH sub(3)D/ super(12)CH sub(4) ratios. A KIE sub(Cl) super(D) of 1.508 plus or minus 0.041 was obtained at...

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Published inGeophysical research letters Vol. 23; no. 24; pp. 3619 - 3622
Main Authors Saueressig, G, Bergamaschi, P, Crowley, J N, Fischer, H, Harris, G W
Format Journal Article
LanguageEnglish
Published 01.12.1996
Subjects
Absorption spectroscopy
Fourier transforms
Fractionation
Geophysics
Infrared
Isotope effect
Reaction kinetics
Temperature dependence
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Summary:The D/H kinetic isotope effect (KIE sub(Cl) super(D)) in the reaction of CH sub(4) with Cl has been investigated using a tunable diode laser absorption spectrometer (TDLAS) to measure super(12)CH sub(3)D/ super(12)CH sub(4) ratios. A KIE sub(Cl) super(D) of 1.508 plus or minus 0.041 was obtained at room temperature (296 K). Experiments employing Fourier transform infrared measurements of super(12)CH sub(3)D/ super(12)CH sub(4) ratios confirmed this result. An investigation of the temperature dependence showed an increase of KIE sub(Cl) super(D) (1.592 plus or minus 0.057 at 223 K) with decreasing temperature. This very large D/H fractionation effect affects the overall isotope fractionation in the middle and upper stratosphere, where Cl contributes substantially to the total removal of CH sub(4).
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ISSN:0094-8276
1944-8007
DOI:10.1029/96GL03292