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z Organic & Supramolecular Chemistry
Monochlorotriazinyl-β-cyclodextrin Grafted on Graphene
Oxide as an Attractive Green Heterogeneous Nanoreactor
for Selective Oxidation Reaction with NBS in Water
Shadi Rasoul Pour,
[a]
Mohammad Dinari,
[a]
and Amir Abdolmaleki*
[a, b]
Graphene oxide supported monochlorotriazinyl-β-cyclodextrin
(GO-MCT- β-CD) as a green nanoreactor was synthesized via a
simple chemical bonding method and analyzed by XRD, FT-IR,
CHNS, FESEM and Raman spectroscopy. The prepared GO-MCT-
β-CD worked as a nanoreactor for the green oxidation reactions
of benzyl alcohol derivatives with N-bromo succinimide to their
corresponding aldehydes under green conditions. Depending
on the different substituents of various benzyl alcohols, good
to excellent yields were obtained and no over-oxidation was
observed. It can be considered an attractive methodology due
to the use of water in the presence of “solid metal-free
nanoreactor” as a green reaction system at the room temper-
ature. Easy separation and excellent reusability of the catalyst
were other advantages of this methodology.
Introduction
Nowadays, green chemistry has been becoming an important
issue in both industrial and academic research.
[1]
Thus,
introducing environmentally gentle synthetic strategies has
been the main target of today’s researchers. Among different
strategies, using supramolecular compounds as organic reac-
tors for reaction in aqueous media (as green and environmental
friendly solvents) is really interesting.
[2]
During the past
decades, the applications of supramolecular host-guest
chemistry are of fascinating interest. The 2016 Nobel Prize in
chemistry was awarded to organic chemists for the synthesis of
molecular machines based on supramolecular interaction
through reversible formation of host–guest complexes
[3,4]
Host
molecules can form inclusion complexes with guest molecules,
providing the selective and reversible interaction by non-
covalent intermolecular bonds and, finally, release the products
and regenerate the reagents for a new run.
[5,6]
β-Cyclodextrin
(β-CD) is a cone-shaped cyclic oligomer that consists of seven
α-linked D-Glucopyranose units joined from ‘‘head to tail’’. It
has a hydrophobic nanocavity at the center and hydrophilic
outside edge, which can form non-covalent reversible host-
guest complexes with a variety of suitably sized aliphatic and
aromatic molecules, preferably in water.
[7,8]
This property makes
β-CD an interesting compound in organic synthesis as a
nanocatalyst and nanoreactor since it is a water-soluble natural
material, non-toxic, inexpensive, and metabolically safe.
[9,10]
The
use of water as a green, gentle, safe, and inexpensive solvent
(compared with organic toxic solvents) in the oxidation
reactions is of importance to develop safer manufacturing
protocols.
[11]
Water as a solvent is limited because of the
insolubility of starting materials “in the water”.
[12–14]
On the
other hand, the high solubility of β-CD in water, restricts its
catalytic application in the aqueous dissolution, motivating
chemists to develop a water-insoluble β-CD (but water-
dispersible) in a solid state. A general strategy is the attach-
ment of β-CD via chemical linkers to solid supporting
materials.
[15,16]
Native β-CD cannot form a direct covalent bond
with solid supports. Monochlorotriazinyl-β-cyclodextrin (MCT-β-
CD), the first cyclodextrin derivative in the industrial scale,
solves this problem. It was presented in 1996, possesses on
average two to three monochlorotriazinyl groups on β-CD as
the reactive anchor, and can create covalent bonds with
nucleophilic groups on supports.
[16–19]
There are some reports in
the literature concerning the potential of applications of these
types of compound in organic reactions.
[20–22]
Cyclodextrins are commonly immobilized on different
supports and covalent immobilization is considered one of the
most frequently used ones. Among different support for
immobilization, GO has attracted more attention recently. The
abundant number of functional groups (carboxyl, carbonyl,
hydroxyl, and epoxide) at the surface and edges of GO facilities
its functionalization. In addition, functionalized graphene oxide
causes easy adsorption of aromatic reactant by a strong π-π
stacking interaction between GO sheet and aromatic rings of
the reactant.
[23,24]
These types of supported reactors have been
applied to several important organic reactions in the aqueous
dissolution.
[25–29]
The oxidation of benzyl alcohol and its
derivatives to their respective aldehydes is an important
reaction in organic chemistry. Traditional processes through
heavy metal-based catalysts are costly and cause environ-
mental pollution due to the exhausting separation of the
soluble catalysts.
[17]
Most of them give low yield as well as poor
selectivity and are commonly available in organic solvents and
[a] S. R. Pour, Dr. M. Dinari, Dr. A. Abdolmaleki
Chemistry group, Pardis College, Isfahan University of Technology,
Isfahan 84156–83111, I.R. Iran
E-mail: abdolmaleki@cc.iut.ac.ir
[b] Dr. A. Abdolmaleki
Department of chemistry, College of science, Shiraz University, Shiraz
71467–13565, I.R. Iran
Supporting information for this article is available on the WWW under
https://doi.org/10.1002/slct.201900962
Full Papers DOI: 10.1002/slct.201900962
6390 ChemistrySelect 2019, 4, 6390 – 6396 © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim