SHORT COMMUNICATION
CHINESE JOURNAL OF CATALYSIS
Volume 31, Issue 5, 2010
Online English edition of the Chinese language journal
Cite this article as: Chin. J. Catal., 2010, 31: 518–520.
Received date: 28 January 2010.
*Corresponding author. Tel: +91-80-22961337; Fax: +91-80-22961331; E-mail: m_af_pasha@ymail.com
Copyright © 2010, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier BV. All rights reserved.
DOI: 10.1016/S1872-2067(09)60064-4
Amberlite IR-120: A Reusable Catalyst for N-Formylation of
Amines with Formic Acid Using Microwaves
Madhusudana Reddy MUTHUKUR BHOJEGOWD, Aatika NIZAM, Mohamed Afzal PASHA*
Department of Studies in Chemistry, Central College Campus, Bangalore University, Bengaluru 560 001, India
Abstract: A rapid and practical green route for the N-formylation of amines with formic acid using Amberlite IR-120 as a catalyst is de-
scribed. This method provides an efficient and much improved modification over the reported methods in terms of yield, reaction time, and
work-up procedure. A wide variety of substituents is tolerated, which is not the case for existing procedures.
Key words: N-formylation; Amberlite IR-120; formic acid; amine; microwave
Since the first report by Fieser et al. [1] on the N-formylation
of amines, a number of strategies have been developed for their
synthesis because of their importance as intermediates in the
preparation of several fine chemicals [1] and pharmaceutically
important compounds such as substituted aryl imidazoles [2],
1,2-dihydroquinolines [3], fluoroquinolines [4], nitrogen-
bridged heterocycles [5], etc. Formamides act as catalysts in
the allylation [6] and hydrosilylation [7] reaction of carbonyl
compounds. The asymmetric allylation of aldehydes using
chiral formamides has also been reported recently [8]. For-
mamides serve as very useful reagents in Vilsmeier formyla-
tion [9] and in the synthesis of formamidines and isocyanides
[10]. In addition, a formyl group is used for the protection of
the amino group during peptide synthesis [11,12].
Generally, the N-formylation of amines can be carried out
using the esters of formic acid such as pentafluorophenyl
formate and phenyl formate for direct N-formylation in the
absence of a catalyst [13,14]. Apart from this, aryl formates
and ethyl formate are useful for N-formylation in the presence
of catalysts like TiCl
3
(OTf) [15] and silica-bonded
N-propylsulfamic acid [16]. Chandra Shekhar et al. [17] have
recently reported the N-formylation of amines using ZnCl
2
as a
catalyst, where the reaction requires a longer time for comple-
tion.
In addition to the above-mentioned reports, a number of
other methods have been documented on the N-formylation of
amines [18–20]. Many of the N-formylation methods have
disadvantages such as the use of expensive reagents, the for-
mation of side products, thermal instability, and difficult to
access reagents. Therefore, the pursuit of more convenient and
practical synthetic methods for these compounds still remains
an active research area.
On the other hand, a “green” reaction should ideally be
conducted under solvent-free conditions with minimal or no
side products and with the utmost atom economy [21]. One
way to achieve this is by microwave heating. It is also well
known that microwave heating dramatically accelerates the
rate of many organic reactions and improves yields, and the
reactions are highly selective [22–27]. Because of these ad-
vantages there is great interest in the use of environmentally
benign reagents and procedures [28].
Recently, the use of solid acidic catalysts has gained im-
portance in organic synthesis because of several advantages
such as operational simplicity, non-toxicity, reusability, low
cost, and ease of separation after completion of the reaction
[29–32]. Amberlite IR-120[H
+
] resin has emerged as an effi-
cient heterogeneous catalyst for various organic reactions [33].
Because of the numerous advantages associated with this in-
expensive and non-hazardous recyclable catalyst we herein
report a protocol for a solvent-free reaction using microwave
activation for the synthesis of N-formamides using Amberlite
IR-120 as a catalyst. To the best of our knowledge this is the
first report on the N-formylation of amines with formic acid
where the reaction is catalyzed by a reusable resin. The method