TETRAHEDRON
LETTERS
Tetrahedron Letters 44 (2003) 5777–5780 Pergamon
Facile and reversible synthesis of an acidic water-soluble
poly(amidoamine) fullerodendrimer
Yutaka Takaguchi,
a,
* Yuuki Sako,
b
Yasushi Yanagimoto,
a
Sadao Tsuboi,
a
Jiro Motoyoshiya,
b
Hiromu Aoyama,
b
Takatsugu Wakahara
c
and Takeshi Akasaka
c
a
Faculty of Environmental Science and Technology, Okayama University, Okayama, Okayama 700 -8530, Japan
b
Faculty of Textile Science & Technology, Shinshu University, Ueda, Nagano 386 -8567, Japan
c
Center for Tsukuba Advanced Research Alliance, University of Tsukuba, Tsukuba, Ibaraki 305 -8577, Japan
Received 28 April 2003; revised 6 June 2003; accepted 9 June 2003
Abstract—Water-soluble fullerodendrimer was obtained by the use of a Diels–Alder reaction of C
60
with a newly designed anthryl
dendron under an extremely mild condition in 70% yield, which is more than five times as high as the yield described in our
previous report.
© 2003 Elsevier Ltd. All rights reserved.
Fullerene-based derivatives have been attracting a great
interest in the field of structural and synthetic organic
chemistry.
1
In particular, there is an increasing focus on
developing applications for fullerene-functionalized
dendrimers, fullerodendrimers, because of a variety of
interesting features in supramolecular chemistry and
material science.
2
However, the chemistry of dendrimer
containing a C
60
core had been very much limited,
because only a few efficient reactions in construction of
fullerodendrimer were reported.
1b,2–6
The elegant and
pioneering studies reported by Fre ´chet,
3
Hirsch,
4
Diederich
1b
and Nierengarten
1b,5
are not so easy to be
performed by almost chemist. Recently, we have
described the reversible formation of fullerodendrimers
by the use of a Diels–Alder reaction of C
60
with anthryl
dendron (1).
7
During our studies on the reactivity of the
anthracene derivatives with C
60
, we found that the yield
was dramatically improved by changing the substituent
on the anthracene moiety. This paper describes the
facile preparation and characterization of a water-solu-
ble poly(amidoamine) fullerodendrimer (2).
In order to improve on the yield of fullerodendrimer
which can be obtained by a Diels–Alder reaction, we
refine upon the molecular design of anthracenyl den-
dron 1 which was employed in a previous paper.
7
First,
a bulky dendritic substituent was moved from 9-posi-
tion to 2-position, since it might not be preferred at a
bridge head of [4+2]cycloadduct arisen from 9-substi-
tuted anthracene derivatives.
Second, we used an electron-withdrawing group as a
tether between an anthracene and a dendron wedge,
because the cycloadducts of C
60
with electron-deficient
dienes were found to be quite stable.
8
This newly
designed anthryl dendron (3) was actually prepared
according to our strategy previously reported (Scheme
1).
9
A focal point of dendron, compound (4), was obtained
by reaction of 2-anthracenecarboxylic acid methyl ester
(5) with ethylenediamine. Subsequently, treatment of 4
with methyl acrylate produced a dendron (3a) in 85%
yield. This two-step process can be repeated to prepare
(3b) and (3c) in 85 and 50% yields, respectively. The
structures of 3a, 3b, and 3c were confirmed by
1
H,
13
C
Keywords : fullerodendrimer; anthracene; cycloaddition; water-soluble
fullerene.
* Corresponding author. Tel.: +81-86251-8903; fax: +81-86251-8903.
0040-4039/$ - see front matter © 2003 Elsevier Ltd. All rights reserved.
doi:10.1016/S0040-4039(03)01425-4