Journal of the Chemical Society - Faraday Transactions p. 2317 - 2324 (1991)
Update date:2022-08-16
Topics:
Davies, Joanne W.
Green, Nicholas J. B.
Pilling, Michael J.
The rate constant for the CH3 + NO reaction has been measured by laser flash photolysis/absorption spectroscopy over the temperature range 296-509 K and at pressures of 25-600 Torr.The data have been analysed using a global variant of the Troe factorisation technique which provides parameters for the representation of k1(P,T) over the experimental range.In addition, a further global technique for analysing the experimental data, based on inverse Laplace transformation of k1infinite(T), coupled with a master equation treatment, has been developed.The advantage of this approach is that it emphasises the relationship between the limiting high-pressure rate coefficient and the energy-dependent lifetime of the adduct.In the present reaction system, this approach enables the lowest triplet state to be implicated in the reaction; it is proposed that, following its formation, the triplet undergoes rapid intersystem crossing to the ground singlet state.The limiting rate parameters returned from the analysis are k1infinite = 1.5 x 10-11 exp(-60 K/T) cm3 mlecule-1 s-1, k10 = 6.9 x 10-32 exp(1430 K/T) cm6 molecule-2 s-1, <ΔE>down = 235 cm-1, for Ar as the diluent gas.
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