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Laser photolysis/laser-induced fluorescence studies of reaction rates of OH with CH3Cl, CH2Cl2, and CHCl3 over an extended temperature range

✍ Scribed by Philip H. Taylor; Joe A. D'angelo; Marc C. Martin; James H. Kasner; Barry Dellinger

Publisher: John Wiley and Sons
Year: 1989
Tongue: English
Weight: 929 KB
Volume: 21
Category: Article
ISSN: 0538-8066
DOI: 10.1002/kin.550210908

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✦ Synopsis

A modified laser photolysis/laser-induced fluorescence technique has been used to measure atmospheric pressure absolute rate coefficients for the reaction of hydroxyl (OH) radicals with the chlorinated methanes (CH,CI, CH2C12, and CHCI,). Data have been obtained for these compounds over the widest temperature range (292-800 K) that has been reported in the literature using a single experimental apparatus. The temperature dependence of the rate data is best represented by the following threeparameter expressions: CH,CI: 8.38 2 1.07 x T'3"='"'"1 exp [ -2387.4 i-142.8/RT] (cm"/molec-sl CH,Cl,: 1.52 2 0.16 x 10." T1"xf"45 exp[-1236.3 +-119.5/RT] (cm3/molec-s) CHCI.,: 1.92 _f 0.21 x 10-' O T2'X'03404' exp[ -188.3 _f 119.3/fZT] (cm"/molec-s)

Uncertainties in the pre-exponential and exponential term are expressed as 95% confidence intervals. For the temperature exponent, error limits represent a ?lo% change in the total error of best fit. The degree of curvature in the Arrhenius plots appeared to increase with increasing C1 substitution of the reactant, However, the uncertainty in the temperature exponent for the CH,Cl data was large in comparison with the other chlorinated methanes. Thus, data of greater precision a t elevated temperatures are necessary to further explore this relationship. The rate coefficients were compared with recent semiempirical and transition state theory models for haloalkane-OH hydrogen transfer reactions over a temperature range of 250-800 K. The transition state model of Cohen and Benson was in excellent agreement with the CH&1 and CH,CI, data. The semiempirical structure activity relationship developed by Atkinson represented the best fit of the

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