FULL PAPER
DOI: 10.1002/ejoc.200900779
An Efficient (2-Aminoarenethiolato)copper(I) Complex for the
Copper-Catalysed Huisgen Reaction (CuAAC)
Pierangelo Fabbrizzi,*
[a]
Stefano Cicchi,*
[a]
Alberto Brandi,
[a]
Elena Sperotto,
[b][‡]
and
Gerard van Koten
[b]
Keywords: Azides / Alkynes / Click chemistry / Cycloaddition / Dendrimers / N ligands
A (2-aminoarenethiolato)copper(I) complex has been used as
an efficient catalyst (1 mol-%) for the copper-catalysed
Huisgen reaction (CuAAC) of azides and terminal alkynes in
an organic solvent. The reaction was also extremely effective
Introduction
The Huisgen reaction, the 1,3-dipolar cycloaddition of
azides to terminal alkynes, has probably become one of the
most frequently used reactions in organic chemistry, espe-
cially after the development by Sharpless and Fokin of a
copper-catalysed version (CuAAC).
[1]
This reaction was the
first of a restricted group of reactions generally known by
the term “click chemistry”.
[2]
The efficiency of this reaction
is demonstrated by the huge number of applications in sup-
ramolecular chemistry,
[3]
peptidomimetics,
[4]
dendrimer
synthesis,
[5]
bioconjugation, polymer and materials synthe-
sis
[6,7]
and many other fields.
[8]
Such a wide variety of applications requires the reaction
to be performed under many different conditions, for exam-
ple, organic and aqueous solvents, and heterogeneous con-
ditions. Despite this variety of reaction conditions a very
limited set of catalysts are available. The use of Cu
II
salts
with a sacrificial reducing agent such as sodium ascorbate
is the most common procedure: sodium ascorbate provides
the Cu
I
ions that are needed for the catalytic reaction.
[1,9]
However, even a copper wire can afford the required Cu
I
ions by comproportionation of Cu
II
and Cu
0
. Simple Cu
I
salts have also been used, but the thermodynamic instability
of Cu
I
can lead to oxidation to catalytically inactive Cu
II
.
The use of ligands such as tris(1-benzyltriazol-4-ylmethyl)-
amine (TBTA)
[10]
or sulfonated bathophenanthroline
[11]
im-
[a] Dipartimento di Chimica Organica “Ugo Schiff”, Università
degli Studi di Firenze,
Via della Lastruccia 13, 50019 Sesto Fiorentino, Firenze, Italy
Fax: +39-055-4573531
E-mail: pfabbrizzi@gmail.com
[b] Chemical Biology & Organic Chemistry, Utrecht University,
Padualaan 8, 3584 CH, Utrecht, The Netherlands
[‡] Present address: Physikalische Chemie, Universität Siegen,
Adolf-Reichwein-Str. 2, 57076 Siegen, Germany
Eur. J. Org. Chem. 2009, 5423–5430 © 2009 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 5423
in CH
2
Cl
2
allowing the complete decoration of dendrimeric
scaffolds.
(© Wiley-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim,
Germany, 2009)
proves the rate and efficiency of more delicate reactions.
The limited solubility of cuprous salts in organic solvents
restricts the choice to soluble preformed coordination com-
plexes of Cu
I
, for example, under these circumstances
[Cu(PPh
3
)
3
]Br
[12]
and (EtO)
3
PCuI
[13]
are the catalysts of
choice. The availability of new Cu
I
complexes, which have
been shown to be active in other reactions, allows the effi-
ciency of these compounds to be tested in another useful
reaction.
In this work we report the results obtained by using the
(aminoarenethiolato)copper(I) complex 1
[14]
(Figure 1) as a
catalyst in the 1,3-dipolar cycloaddition of azides to ter-
minal alkynes. In (aminoarenethiolato)copper(I) complexes,
the copper(I) cation is bonded to a monoanionic, poten-
tially S,N-bidentate-coordinating 2-aminoarenethiolate li-
gand. These complexes show excellent solubility in a range
of useful solvents. They exist, both in the solid state and in
solution, as aggregate species, for example, as dimers, tri-
mers, tetramers or nonamers,
[15]
and exhibit good thermal
stability. In addition, electronic and physical properties can
easily be fine-tuned by introducing substituents onto the
arene ring or the amino functionality. These (aminoarene-
thiolato)copper(I) complexes have already been tested as
catalysts in allylic substitution,
[16]
1,4-
[17]
and 1,6-addition
[18]
reactions and aromatic N-arylation reactions
[19]
and have
shown good catalytic properties.
Figure 1. {[2-(Dimethylamino)methyl]thiophenolato}copper(I) (1).