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238 Current Organic Chemistry, 2013, 17, 238-256
Ionic Liquids and the Heck Coupling Reaction: An Update
Patrícia Prediger,
a,b
Yves Génisson
a*
and Carlos Roque Duarte Correia
b*
a
UMR5068, CNRS-Université Paul Sabatier, Toulouse, France
b
Instituto de Química, Universidade Estadual de Campinas, UNICAMP, C.P. 6154, CEP. 13084-971, Campinas, São Paulo, Brazil
Abstract: In this review update we provide a critical analysis of recent results concerning the use of ionic liquids (ILs) as viable, effec-
tive, and environmental friendly media for the Heck reactions (HR). The examples selected illustrate the multifaceted action of ILs as
nanoparticles stabilizers, promoters of ligand-assisted HR, promoters of phosphine-free HR, solvent for the Heck-Matsuda reactions em-
ploying arenediazonium salts, in the dehydrative Heck olefination, and as charged-tagged pre-catalysts. These selected reports aim at
demonstrating the scope and the impact of Ils on new discoveries, as well as to illustrate the new opportunities and challenges they offer
for those interested in catalysis and organic synthesis in general.
Keywords: Ionic liquids, Heck reaction, Palladium-nanoparticles , N-heterocyclic carbenes.
1. INTRODUCTION
After a decade of exponential development, the field of ionic
liquids (ILs) technology has reached a substantial degree of matur-
ity in several aspects, including preparation, purification and phys-
icochemical characterization [1]. Over the same period, other do-
mains of application of ILs have progressively grown such as ana-
lytical chemistry [2] or biomass valorization [3]. The area of cataly-
sis and organometallic chemistry, with the early identification of
ILs as unique media [4], has also strongly contributed to their cur-
rent wide recognition [5]. Yet, as demonstrated by the profusion of
recent works reported here, many opportunities and challenges are
still open in this domain.
ILs have been proposed as an eco-friendly alternative to com-
mon volatile molecular solvents. This arises from several key fea-
tures such as their thermal stability, negligible vapor pressure and
they are virtually non-inflammable [6]. The tunable physicochemi-
cal profile of ILs, such as water/solvent relative miscibility or liquid
state temperature range, has also called the attention of the chemical
community, offering prospects for innovative process developments
[7]. Their potential for recyclability in particular underlies all the
above-mentioned physicochemical characteristics of ILs.
Among the Pd(0)-catalyzed cross couplings, the reaction be-
tween an aryl halide and an olefin, known as the Heck-Mizoroki
arylation holds a prominent place [8]. It has become a versatile and
ubiquitous synthetic tool for the creation of strategic Csp
2
-Csp
2
bonds in complex molecules. A myriad of reaction cocktails have
been proposed for the Heck coupling, varying the source of Pd(0),
the metal ligand, the solvent and the base. However, such a sophis-
tication of the reaction systems normally goes along with more
constraining reaction conditions and costly reagents [9]. In this
context, ILs have offered unexpected opportunities for a striking
simplification of the Heck coupling procedure, potentially acting as
a recoverable reaction medium and reaction promoter [10]. This has
further led to specifically functionalized ionic structures, called
Task Specific ILs (TSILs), designed to accelerate a reaction step (as
*
Address correspondence to this author at the Instituto de Química, Universidade
Estadual de Campinas, UNICAMP, C.P. 6154, CEP. 13084-971, Campinas, São Paulo,
Brazil; Tel: +55 19 35213086; Fax: +55 19 3521 3023: E-mail: roque@iqm.unicamp.br
a base) or to complex the metallic species (as a ligand) [11]. Other
approaches, such as the catalyst’s immobilization, were also pur-
sued with the development of supported ILs [12].
A comprehensive overview of the Heck reaction in ILs has been
published by Bellina and Chiappe in March 2010 [13]. The present
review intends to give an update of the work published in this
highly active area from mid 2010.
2. THE DIFFERENT TYPES OF EFFECT OF ILS ON THE
HECK REACTION
One of the most important roles of the ionic medium on palla-
dium-catalyzed transformations may be the stabilization of the ac-
tive catalytic species. This has notably led to the development of
practical aerobic and ligand-free coupling procedures. The general
promoting effects of ILs on palladium-catalyzed cross couplings,
including the Heck reaction, are basically of two main types:
nanoparticles stabilization or diaminocarbene ligands generation.
2.1. ILs as Nanoparticles Stabilizer
The first effect of ILs on palladium catalysis deals with
nanoparticles stabilization [14]. Indeed, the efficiency of the Heck
coupling largely depends on the generation of stable Pd(0) colloidal
solutions from a precatalyst. In situ Pd nanoparticles generation in
standard ammonium or imidazolium ILs have been examined in
depth [15]. It may be easily accomplished, for example by reduc-
tion (either upon hydrogenation or strong heating) of a Pd(II) salt or
decomposition of an organometallic complex [16]. The formation
of a dispersed metallic suspension, generally characterized in size
and shape by Transmission Electron Microscopy (TEM) analysis
[17] is commonly opposed to the eventual precipitation of inactive
crystalline Pd black. Combined electrostatic and steric stabilizing
effects of the IL on the nanoparticles have been invoked.
2.2. Diaminocarbene Precursor
The formation of diaminocarbene transition metal ligands
through the somewhat favorable abstraction of the hydrogen in the
2-position of an imidazolium nucleus is well documented [18]. The
participation of imidazolium based ILs as carbenic species precur-
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