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Ab initio study of the reaction pathways for OH + C/sub 2/H/sub 4/. -->. HOCH/sub 2/CH/sub 2/. -->. products

Journal Article · · J. Am. Chem. Soc.; (United States)
DOI:https://doi.org/10.1021/ja00257a017· OSTI ID:7076524

The energetically favorable reaction paths for the unimolecular decomposition of the primary addition product of OH + C/sub 2/H/sub 4/ have been studied with ab initio techniques. Equilibrium geometries and transition structures were fully optimized with 3-21G and 6-31G* basis sets at the Hartree-Fock level. Heats of reaction and barrier heights have been computed with Moeller-Plesset perturbation theory up to fourth order, with and without annihilation of spin contamination. At the MP4 level barrier heights are lowered by 2-7 kcal/mol when the largest spin contaminant is removed. After the addition of OH + C/sub 2/H/sub 4/ to form the 2-hydroxyethyl radical, the most favorable reaction path (other than decomposition to reactants) is the (1,3)-hydrogen shift to form ethoxy radical followed by a dissociation into CH/sub 3/ + CH/sub 2/O. Other slightly higher energy paths include dissociation of ethoxy into H + CH/sub 3/CHO and decomposition of the 2-hydroxyethyl radical into H + HOCHCH/sub 2/.

Research Organization:
Wayne State Univ., Detroit, MI (USA)
OSTI ID:
7076524
Journal Information:
J. Am. Chem. Soc.; (United States), Journal Name: J. Am. Chem. Soc.; (United States) Vol. 109:23; ISSN JACSA
Country of Publication:
United States
Language:
English