Pergamon
Tetrahedron 54 (1998) 13793-13804
TETRAHEDRON
Catalytic alternative of the Ulimann reaction
Jwanro Hassan, Vincent Penalva, Laurence Lavenot, Christel Gozzi and Marc Lemaire*
Institut de Recherches sur la Catalyse et Laboratoire de Catalyse et Synthrse Organique, CNRS, Universit6
C. Bernard. CPE, B~.t.308, 43 bd. du 11 nov., 69622 Villeurbanne, France
Received 8 June 1998; accepted 10 September 1998
Abstract: Symmetrical functionalized biaryls and biheterocyclescould be obtained in good yield via
homocouplingof aryl halides by using Pd(OAc)2 as catalyst with base and isopropanol.This alternative
of the UIImann reactionhas proved to be compatiblewith sensitivefunctional groups. © 1998Elsevier
Science Ltd. All rights reserved.
The preparation and utilization of biaryl system is a demanding goal, seeing that biaryls have a large
number of physical and chemical properties and can be used as monomers for the synthesis of conductive
polymers, l,2,3,4 important biaryl natural products such as steganone,5 supramolecular,6 as ligand catalysts and
receptrice macrocyclic moleculesT.There are many methods to prepare symmetrical biaryls, the main way being
the UIImann reaction which requires equimolar amounts of copper. 8 Among the other methods, the synthesis of
biaryls by arylboronic acid, 9 arylzinc 10 and arylstannanes 11 derivatives were carried out. These methods are
effective but need stoichiometric or over stoichiometric amounts of organometallic intermediate. Recently other
methods have been developed; the Ni(0)/Zn 12 coupling was used to synthesize bipyridines with good yields but
this method also needs an equivalent of nickel and zinc. The nickel-containingcomplex reducing agents NiCRA-
bpy was used to synthesize biaryls 13 but an excess of Nail and 2,2'-bipyridine (bpy) were required. Otherwise,
a variety of bipyridines and biaryls can be synthesized in moderate to good yields by using the nickel (II)
complex 14 furthermore this method is effective for the homocoupling of aryl chlorides. In most cases, an excess
of Zinc and Et4NI were required. In contrary, the Pd/formiate 15 coupling in phase transfer catalysis condition
requires a catalytic amount of metal but leads to moderate yields and is not compatible with functional g:oups
such as aldehyde or nitro which are reduced in similar condition.
This paper shows the effectiveness of Pd(OAc)2 as catalyst with base and isopropanol for the direct
synthesis of symmetrical biaryls via homocoupling of aryl halides. 16 This catalytic system has been already
proved to be efficient for the synthesis of acenaphthylene derivatives,17 as well as in our laboratory for the direct
arylation of activated thiophens by iodoaryls.18 In this work, the scope and limitations of the symmetrical
coupling reaction (scheme 1) are evaluated by testing a wide variety of aryl halides.
R R
~._X Pd(OAc)2 / nBu4NBr ~ ~
Scheme 1 : Homocoupling of aryl halides
Fax: 04-72-43-14-08 E-mail: Marc.Lemaire@univ-lyonl.fr
0040-4020/98/$ - see front matter © 1998 Elsevier Science Ltd. All rights reserved.
PII: S0040-4020(98)00849-7