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• W2011091003 startingPage "4062" @default.
• W2011091003 abstract "We have studied the two-channel thermal decomposition of methyl radicals in argon, involving the reactions CH3 + Ar → CH + H2 + Ar (1a) and CH3 + Ar → CH2 + H + Ar (1b), in shock tube experiments over the 2253−3527 K temperature range, at pressures between 0.7 and 4.2 atm. CH was monitored by continuous-wave, narrow-line-width laser absorption at 431.1311 nm. The collision-broadening coefficient for CH in argon, 2γCH-Ar, was measured via repeated single-frequency experiments in the ethane pyrolysis system behind reflected shock waves. The measured 2γCH-Ar value and updated spectroscopic and molecular parameters were used to calculate the CH absorption coefficient at 431.1311 nm (23194.80 cm-1), which was then used to convert raw traces of fractional transmission to quantitative CH concentration time histories in the methyl decomposition experiments. The rate coefficient of reaction 1a was measured by monitoring CH radicals generated upon shock-heating highly dilute mixtures of ethane, C2H6, or methyl iodide, CH3I, in an argon bath. A detailed chemical kinetic mechanism was used to model the measured CH time histories. Within experimental uncertainty and scatter, no pressure dependence could be discerned in the rate coefficient of reaction 1a in the 0.7−4.2 atm pressure range. A least-squares, two-parameter fit of the current measurements, applicable between 2706 and 3527 K, gives k1a (cm3 mol-1 s-1) = 3.09 × 1015 exp[−40700/T (K)]. The rate coefficient of reaction 1b was determined by shock-heating dilute mixtures of C2H6 or CH3I and excess O2 in argon. During the course of reaction, OH radicals were monitored using the well-characterized R1(5) line of the OH A−X (0,0) band at 306.6871 nm (32606.52 cm-1). H atoms generated via reaction 1b rapidly react with O2, which is present in excess, forming OH. The OH traces are primarily sensitive to reaction 1b, reaction 9 (H + O2 → OH + O) and reaction 10 (CH3 + O2 → products), where the rate coefficients of reactions 9 and 10 are relatively well-established. No pressure dependence could be discerned for reaction 1b between 1.1 and 3.9 atm. A two-parameter, least-squares fit of the current data, valid over the 2253−2975 K temperature range, yields the rate expression k1b (cm3 mol-1 s-1) = 2.24 × 1015 exp[−41600/T (K)]. Theoretical calculations carried out using a master equation/RRKM analysis fit the measurements reasonably well." @default.
• W2011091003 created "2016-06-24" @default.
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• W2011091003 date "2007-02-22" @default.
• W2011091003 modified "2023-10-11" @default.
• W2011091003 title "High-Temperature Shock Tube Measurements of Methyl Radical Decomposition" @default.
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• W2011091003 doi "https://doi.org/10.1021/jp0677187" @default.
• W2011091003 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/17388279" @default.
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