SHORT COMMUNICATION
DOI: 10.1002/ejoc.200900800
Vinylic Substitutions Promoted by PhSeZnCl: Synthetic and Theoretical
Investigations
Stefano Santoro,
[a]
Benedetta Battistelli,
[a]
Lorenzo Testaferri,
[a]
Marcello Tiecco,
[a]
and
Claudio Santi*
[a]
Keywords: Selenium / Zinc / Vinylic substitution / Nucleophilic substitution / DFT calculations
Vinyl selenides can be easily obtained through nucleophilic
substitution of the corresponding halides by using PhSeZnCl
in THF as well as “on water” conditions. The reaction is ste-
reospecific with retention of the alkene geometry. The only
exception has been observed in the reaction conducted on a
β-chloro-α,β-unsaturated ketone, which afforded the (Z)
Introduction
Phenyl selenolate is one of the most convenient organo-
selenium reagents, and its role in effecting many synthetic
transformation is known.
[1]
A number of procedures for the
“in situ” generation of selenolates have been reported,
[2]
but
most of them suffer from serious drawbacks such as bad
smelling, moisture sensitivity, strong basic reaction condi-
tions, use of hazardous organic solvents. Recently, the use
of zinc as reducing agent for the preparation of selenols was
reported,
[3]
and we demonstrated that treatment of com-
mercially available PhSeCl with a stoichiometric amount of
zinc powder in refluxing THF leads to the corresponding
solid and air-stable zinc selenolate 1 through an oxidative
insertion of zinc into the selenium–chlorine bond
[4]
(Fig-
ure 1).
Figure 1. Bench-stable selenolate PhSeZnCl (1).
This reagent has been efficiently employed in the ring
opening of epoxides, and we reported also an unexpected
rate acceleration when these reactions were effected by “on
water” conditions.
[5]
[a] Dipartimento di Chimica e Tecnologia del Farmaco, Università
di Perugia,
via Del Liceo 1, 06123 Perugia, Italy
Fax: +39-075-5855116
E-mail: santi@unipg.it
Supporting information for this article is available on the
WWW under http://dx.doi.org/10.1002/ejoc.200900800.
Eur. J. Org. Chem. 2009, 4921–4925 © 2009 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 4921
product starting from either the (E) or (Z) isomer. DFT calcu-
lations have been performed in order to investigate the reac-
tion mechanism, the stereochemistry of the process and the
role of the zinc atom.
(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim,
Germany, 2009)
Here we report that 1 can be used for the synthesis of
vinylic selenides starting from the corresponding halides.
Many vinylic sulfide, selenide and telluride preparations in-
volve the use of expensive catalysts or not readily available
starting materials.
[6]
Moreover, often the products are ob-
tained as mixtures of regio- or stereoisomers. Vinylic sele-
nides are intermediates of great synthetic interest, and their
versatility in organic synthesis is well documented through
the publication of a number of reviews and books.
[6b,7]
They
combine the functional transformations achieved by the
well-known reactions of organoselenium compounds (e.g.
selenoxides, syn elimination) with the ability of carbon–car-
bon bond-forming reactions involving the double bond, as-
sociated with the capacity of selenium to stabilize adjacent
positive and negative charges (Scheme 1).
Scheme 1. Vinylic selenides as useful synthetic intermediates.