Atmospheric chemistry of CH3CHF2 (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NOx

Fumikazu Taketani; Tomoki Nakayama; Kenshi Takahashi; Yutaka Matsumi; Michael D. Hurley; Timothy J. Wallington; Anne Toft; Mads Peter Sulbæk Andersen

doi:10.1021/jp052270f

Atmospheric chemistry of CH₃CHF₂ (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x

Fumikazu Taketani, Tomoki Nakayama, Kenshi Takahashi, Yutaka Matsumi, Michael D. Hurley, Timothy J. Wallington, Anne Toft, Mads Peter Sulbæk Andersen

Kemisk Institut

13 Citationer (Scopus)

Abstract

Smog chamber/Fourier transform infrared (FTIR) and laser-induced fluorescence (LIF) spectroscopic techniques were used to study the atmospheric degradation of CH3CHF2. The kinetics and products of the Cl(2P(3/2)) (denoted Cl) atom- and the OH radical-initiated oxidation of CH3CHF2 in 700 Torr of air or N2; diluents at 295 +/- 2 K were studied using smog chamber/FTIR techniques. Relative rate methods were used to measure k(Cl + CH3CHF2) = (2.37 +/- 0.31) x 10(-13) and k(OH + CH3CHF2) = (3.08 +/- 0.62) x 10(-14) cm3 molecule(-1) s(-1). Reaction with Cl atoms gives CH3CF2 radicals in a yield of 99.2 +/- 0.1% and CH2CHF2 radicals in a yield of 0.8 +/- 0.1%. Reaction with OH radicals gives CH3CF2 radicals in a yield >75% and CH2CHF2 radicals in a yield 10(10) s(-1)) decomposition to give CH3 radicals and COF2. The remaining approximately 70% become thermalized, CH3CF2O, and undergo decomposition more slowly at a rate of approximately 2 x 10(3) s(-1). At high concentrations (>50 mTorr), NO(x) is an efficient scavenger for CH3CF2O radicals leading to the formation of CH3COF and FNO.

Originalsprog	Engelsk
Tidsskrift	Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory
Vol/bind	109
Udgave nummer	40
Sider (fra-til)	9061-9069
Antal sider	9
ISSN	1089-5639
DOI	https://doi.org/10.1021/jp052270f
Status	Udgivet - 2005

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10.1021/jp052270f

Citationsformater

Taketani, F., Nakayama, T., Takahashi, K., Matsumi, Y., Hurley, M. D., Wallington, T. J., Toft, A., & Andersen, M. P. S. (2005). Atmospheric chemistry of CH₃CHF₂ (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x. Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, 109(40), 9061-9069. https://doi.org/10.1021/jp052270f

Atmospheric chemistry of CH₃CHF₂ (HFC-152a) : kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x. / Taketani, Fumikazu; Nakayama, Tomoki; Takahashi, Kenshi et al.

I: Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, Bind 109, Nr. 40, 2005, s. 9061-9069.

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

Taketani, F, Nakayama, T, Takahashi, K, Matsumi, Y, Hurley, MD, Wallington, TJ, Toft, A & Andersen, MPS 2005, 'Atmospheric chemistry of CH₃CHF₂ (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x', Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory, bind 109, nr. 40, s. 9061-9069. https://doi.org/10.1021/jp052270f

Taketani F, Nakayama T, Takahashi K, Matsumi Y, Hurley MD, Wallington TJ et al. Atmospheric chemistry of CH₃CHF₂ (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x. Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory. 2005;109(40):9061-9069. doi: 10.1021/jp052270f

Taketani, Fumikazu ; Nakayama, Tomoki ; Takahashi, Kenshi et al. / Atmospheric chemistry of CH₃CHF₂ (HFC-152a) : kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x. I: Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory. 2005 ; Bind 109, Nr. 40. s. 9061-9069.

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title = "Atmospheric chemistry of CH3CHF2 (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NOx",

abstract = "Smog chamber/Fourier transform infrared (FTIR) and laser-induced fluorescence (LIF) spectroscopic techniques were used to study the atmospheric degradation of CH3CHF2. The kinetics and products of the Cl(2P(3/2)) (denoted Cl) atom- and the OH radical-initiated oxidation of CH3CHF2 in 700 Torr of air or N2; diluents at 295 +/- 2 K were studied using smog chamber/FTIR techniques. Relative rate methods were used to measure k(Cl + CH3CHF2) = (2.37 +/- 0.31) x 10(-13) and k(OH + CH3CHF2) = (3.08 +/- 0.62) x 10(-14) cm3 molecule(-1) s(-1). Reaction with Cl atoms gives CH3CF2 radicals in a yield of 99.2 +/- 0.1% and CH2CHF2 radicals in a yield of 0.8 +/- 0.1%. Reaction with OH radicals gives CH3CF2 radicals in a yield >75% and CH2CHF2 radicals in a yield 10(10) s(-1)) decomposition to give CH3 radicals and COF2. The remaining approximately 70% become thermalized, CH3CF2O, and undergo decomposition more slowly at a rate of approximately 2 x 10(3) s(-1). At high concentrations (>50 mTorr), NO(x) is an efficient scavenger for CH3CF2O radicals leading to the formation of CH3COF and FNO.",

author = "Fumikazu Taketani and Tomoki Nakayama and Kenshi Takahashi and Yutaka Matsumi and Hurley, {Michael D.} and Wallington, {Timothy J.} and Anne Toft and Andersen, {Mads Peter Sulb{\ae}k}",

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doi = "10.1021/jp052270f",

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pages = "9061--9069",

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T1 - Atmospheric chemistry of CH3CHF2 (HFC-152a)

T2 - kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NOx

AU - Taketani, Fumikazu

AU - Nakayama, Tomoki

AU - Takahashi, Kenshi

AU - Matsumi, Yutaka

AU - Hurley, Michael D.

AU - Wallington, Timothy J.

AU - Toft, Anne

AU - Andersen, Mads Peter Sulbæk

PY - 2005

Y1 - 2005

N2 - Smog chamber/Fourier transform infrared (FTIR) and laser-induced fluorescence (LIF) spectroscopic techniques were used to study the atmospheric degradation of CH3CHF2. The kinetics and products of the Cl(2P(3/2)) (denoted Cl) atom- and the OH radical-initiated oxidation of CH3CHF2 in 700 Torr of air or N2; diluents at 295 +/- 2 K were studied using smog chamber/FTIR techniques. Relative rate methods were used to measure k(Cl + CH3CHF2) = (2.37 +/- 0.31) x 10(-13) and k(OH + CH3CHF2) = (3.08 +/- 0.62) x 10(-14) cm3 molecule(-1) s(-1). Reaction with Cl atoms gives CH3CF2 radicals in a yield of 99.2 +/- 0.1% and CH2CHF2 radicals in a yield of 0.8 +/- 0.1%. Reaction with OH radicals gives CH3CF2 radicals in a yield >75% and CH2CHF2 radicals in a yield 10(10) s(-1)) decomposition to give CH3 radicals and COF2. The remaining approximately 70% become thermalized, CH3CF2O, and undergo decomposition more slowly at a rate of approximately 2 x 10(3) s(-1). At high concentrations (>50 mTorr), NO(x) is an efficient scavenger for CH3CF2O radicals leading to the formation of CH3COF and FNO.

AB - Smog chamber/Fourier transform infrared (FTIR) and laser-induced fluorescence (LIF) spectroscopic techniques were used to study the atmospheric degradation of CH3CHF2. The kinetics and products of the Cl(2P(3/2)) (denoted Cl) atom- and the OH radical-initiated oxidation of CH3CHF2 in 700 Torr of air or N2; diluents at 295 +/- 2 K were studied using smog chamber/FTIR techniques. Relative rate methods were used to measure k(Cl + CH3CHF2) = (2.37 +/- 0.31) x 10(-13) and k(OH + CH3CHF2) = (3.08 +/- 0.62) x 10(-14) cm3 molecule(-1) s(-1). Reaction with Cl atoms gives CH3CF2 radicals in a yield of 99.2 +/- 0.1% and CH2CHF2 radicals in a yield of 0.8 +/- 0.1%. Reaction with OH radicals gives CH3CF2 radicals in a yield >75% and CH2CHF2 radicals in a yield 10(10) s(-1)) decomposition to give CH3 radicals and COF2. The remaining approximately 70% become thermalized, CH3CF2O, and undergo decomposition more slowly at a rate of approximately 2 x 10(3) s(-1). At high concentrations (>50 mTorr), NO(x) is an efficient scavenger for CH3CF2O radicals leading to the formation of CH3COF and FNO.

U2 - 10.1021/jp052270f

DO - 10.1021/jp052270f

M3 - Journal article

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SN - 1089-5639

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JO - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

JF - Journal of Physical Chemistry Part A: Molecules, Spectroscopy, Kinetics, Environment and General Theory

IS - 40

ER -

Atmospheric chemistry of CH3CHF2 (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NOx

Abstract

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Atmospheric chemistry of CH₃CHF₂ (HFC-152a): kinetics, mechanisms, and products of Cl atom- and OH radical-initiated oxidation in the presence and absence of NO_x