posted on 2015-12-17, 06:31authored bySamantha
E. Shockley, Jeffrey C. Holder, Brian M. Stoltz
A catalytic, enantioselective
formal synthesis of (+)-dichroanone
and (+)-taiwaniaquinone H is reported. The all-carbon quaternary stereocenter
was constructed by asymmetric conjugate addition catalyzed by a palladium(II)
(S)-tert-butylpyridinooxazoline complex.
The unexpected formation of a [3.2.1] bicyclic intermediate required
the identification of a new route. Analysis of the Hammett constants
for para-substituted arenes enabled the rational
design of a highly enantioselective conjugate addition substrate that
led to the completion of the formal synthesis.