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Temperature and Pressure Dependences of the Reactions of Fe + with Methyl Halides CH 3 X (X = Cl, Br, I): Experiments and Kinetic Modeling Results.
Journal of Physical Chemistry. A 2017 June 2
The pressure and temperature dependences of the reactions of Fe+ with methyl halides CH3 X (X = Cl, Br, I) in He were measured in a selected ion flow tube over the ranges 0.4 to 1.2 Torr and 300-600 K. FeX+ was observed for all three halides and FeCH3 + was observed for the CH3 I reaction. FeCH3 X+ adducts (for all X) were detected in all reactions. The results were interpreted assuming two-state reactivity with spin-inversions between sextet and quartet potentials. Kinetic modeling allowed for a quantitative representation of the experiments and for extrapolation to conditions outside the experimentally accessible range. The modeling required quantum-chemical calculations of molecular parameters and detailed accounting of angular momentum effects. The results show that the FeX+ products come via an insertion mechanism, while the FeCH3 + can be produced from either insertion or SN 2 mechanisms, but the latter we conclude is unlikely at thermal energies. A statistical modeling cannot reproduce the competition between the bimolecular pathways in the CH3 I reaction, indicating that some more direct process must be important.
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