Bypassing the Multi-reference Character of Singlet Molecular Oxygen.
Part 2: Ene-reaction
Abstract
Theoretical calculations involving singlet molecular oxygen (O2(1g)) are
challeng- ing due to their inherent multi-reference character. We have
tested the quality of re- stricted and unrestricted DFT geometries
obtained for the reaction between singlet oxy- gen and a series of
alkenes (propene, 2-methylpropene, trans-butene, 2-methylbutene and
2,3-dimethylbutene) which are able to follow the ene-reaction. The
electronic en- ergy of the obtained geometries are rened using 3 dierent
methods which account for the multi-reference character of singlet
oxygen. The results show that the mechanism for the ene-reaction is
qualitatively dierent when either one or two allylic-hydrogen groups are
available for the reaction. When one allylic-hydrogen group is available
the UDFT calculations predict a stepwise addition forming a biradical
intermediate, while, the RDFT calculations predict a concerted reaction
where both hydrogen abstrac- tion and oxygen addition occur
simultaneously. When two allylic-hydrogen groups are available for the
reaction then UDFT and RDFT predict the same reaction mechanism, namely
that the reaction occurs as a stepwise addition without a stable
intermediate between the two transition states. The calculated rate
constants are in reasonable agreement with experimental data, except for
trans-butene where the calculated rate constant is three orders of
magnitude lower than the experimental one. In conclusion we nd that the
simple bypassing scheme tested in this paper is a robust approach for
calculations of reaction involving singlet oxygen in the limit that the
transition state processes low multi-reference character. 2