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Decomposition and vibrational relaxation in CH{sub 3}I and self-reaction of CH{sub 3} radicals.

Journal Article · · J. Phys. Chem. A
DOI:https://doi.org/10.1021/jp903336u· OSTI ID:1012802
; ;  [1]
  1. Chemical Sciences and Engineering Division

Vibrational relaxation and dissociation of CH{sub 3}I, 2-20% in krypton, have been investigated behind incident shock waves in a diaphragmless shock tube at 20, 66, 148, and 280 Torr and 630-2200 K by laser schlieren densitometry. The effective collision energy obtained from the vibrational relaxation experiments has a small, positive temperature dependence, {Delta}E{sub down} = 63 x (T/298){sup 0.56} cm{sup -1}. First-order rate coefficients for dissociation of CH{sub 3}I show a strong pressure dependence and are close to the low-pressure limit. Restricted-rotor Gorin model RRKM calculations fit the experimental results very well with {Delta}E{sub down} = 378 x (T/298){sup 0.457} cm{sup -1}. The secondary chemistry of this reaction system is dominated by reactions of methyl radicals and the reaction of the H atom with CH{sub 3}I. The results of the decomposition experiments are very well simulated with a model that incorporates methyl recombination and reactions of methylene. Second-order rate coefficients for ethane dissociation to two methyl radicals were derived from the experiments and yield k = (4.50 {+-} 0.50) x 10{sup 17} exp(-32709/T) cm{sup 3} mol{sup -1} s{sup -1}, in good agreement with previous measurements. Rate coefficients for H + CH{sub 3}I were also obtained and give k = (7.50 {+-} 1.0) x 10{sup 13} exp(-601/T) cm{sup 3} mol{sup -1} s{sup -1}, in reasonable agreement with a previous experimental value.

Research Organization:
Argonne National Laboratory (ANL)
Sponsoring Organization:
SC
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1012802
Report Number(s):
ANL/CSE/JA-64036
Journal Information:
J. Phys. Chem. A, Journal Name: J. Phys. Chem. A Journal Issue: 29 ; Jul. 1, 2009 Vol. 113; ISSN 1089-5639
Country of Publication:
United States
Language:
ENGLISH

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