Pergamon Tetrahedron Letters 41 (2000) 1227–1230
TETRAHEDRON
LETTERS
Coupling of chiral 1-bromo-1,2-dienes with zinc-based cuprates:
a new procedure for the regio and stereoselective synthesis of
functionalized acetylenic compounds
Anna Maria Caporusso,
*
Sara Filippi, Federica Barontini and Piero Salvadori
Centro di Studio del CNR per le Macromolecole Stereordinate ed Otticamente Attive, Dipartimento di Chimica e Chimica,
Industriale dell’Università di Pisa, Via Risorgimento 35, 56126 Pisa, Italy
Received 12 October 1999; accepted 3 December 1999
Abstract
Zinc alkylcyanocuprates (Knochel reagents) are found to be active in the cross-coupling reaction with allenic
bromides affording acetylenic products with a high regio and stereoselective 1,3-anti substitution. The coupling
process, which has been successfully extended to functionalized cuprates, can also be performed with alkylzinc
chlorides in the presence of catalytic amounts of cuprous salts. © 2000 Elsevier Science Ltd. All rights reserved.
Keywords: coupling reactions; copper; copper compounds; allenes; alkynes.
Few simple organic molecules are the object of more interest than acetylenes for molecular engineering
work in organic and organometallic chemistry.
1
In particular, optically active 1-alkynes are often essential
as versatile building blocks for the construction of more complex chiral molecules.
2
In previous papers
3–6
we discussed utilization of enantioenriched 3-substituted and 3,3-disubstituted
1-bromo-1,2-dienes 1 as precursors of chiral 1-alkynes 2, characterized by a tertiary or a quaternary
stereogenic center in the α-position to the triple bond, via a cross-coupling reaction with bromocuprates
(RCuBr)MgBr
.
LiBr, obtained in THF from equimolar amounts of Grignard reagents and LiCuBr
2
. The
reaction proceeds in a highly 1,3-anti stereoselective fashion, but the regioselectivity appears to be
sensitive to steric interactions at the reaction sites, the bulk of the R substituents in the copper species
being the dominant factor. The acetylenic compounds 2 can be obtained in good yields (70–98%)
independent of the structure of the allenic bromide only employing phenyl
3
or n-alkyl bromocuprates;
6
when tertiary, secondary or α-branched primary copper reagents are used, the competitive formation of
allenic derivatives 3 can be favoured (Table 1).
6
We report here new results that emphasize the dramatic improvement of our coupling methodology
when cuprates based on organozinc derivatives are used.
*
Corresponding author.
0040-4039/00/$ - see front matter © 2000 Elsevier Science Ltd. All rights reserved.
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