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An ab initio investigation of the reactions of 1,1 and 1,2-dichloroethane with hydroxyl radical

Journal Article · · Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory
DOI:https://doi.org/10.1021/jp991660x· OSTI ID:20013046

The hydrogen abstraction reactions by OH radical from 1,1-dichloroethane and 1,2-dichloroethane have been investigated by ab initio molecular orbital theory. Optimized geometries and harmonic vibrational frequencies have been calculated for all reactants, transition structures, and products at the (U)HF/6-311G(d,p) and (U)MP2 = full/6-311G(d,p) levels of theory. Single point QCISD(T)/6-311G(d,p)//(U)MP2 = full/6-311G(d,p) calculations have also been carried out for the inclusion of higher order electron correlation. Three distinct transition structures have been located for the H{sub 3}C-CHCl{sub 2} + OH reaction (one for {alpha}-abstraction and two for {beta}-abstraction). Four transition structures have been located for the reaction ClH{sub 2}C-CH{sub 2}Cl + OH. The calculated barrier heights, reaction enthalpies, and change in entropy are found to be in good agreement with available experimental values. In addition, the rate constants calculated by using the transition state theory are found to be in good agreement with the experimental results. Non-Arrhenius behavior of the rate constants arises from the tunneling effects and availability of multiple reaction channels.

Research Organization:
National Inst. of Materials and Chemical Research, Ibaraki (JP)
OSTI ID:
20013046
Journal Information:
Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory, Journal Name: Journal of Physical Chemistry A: Molecules, Spectroscopy, Kinetics, Environment, amp General Theory Journal Issue: 50 Vol. 103; ISSN 1089-5639; ISSN JPCAFH
Country of Publication:
United States
Language:
English

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