FULL PAPER
DOI: 10.1002/ejoc.201403531
Iodine-Catalyzed Oxidative Amination of Sodium Sulfinates: A Convenient
Approach to the Synthesis of Sulfonamides under Mild Conditions
Chonchanok Buathongjan,
[a]
Danupat Beukeaw,
[a,b]
and Sirilata Yotphan*
[a,b]
Keywords: Iodine / Sulfonamides / Sodium sulfinates / Amines / Oxidative amination
The iodine-catalyzed oxidative amination of sodium sulfin-
ates in the presence of sodium percarbonate as the oxidant
has been developed. The reaction shows good substrate
scope and tolerates a wide range of functionalities in both
amine and sodium sulfinate substrates. Aliphatic amines,
heteroaromatic amines and hydrochloride salts of amines can
Introduction
Sulfonamides are a privileged class of pharmaceutical
compounds with a broad spectrum of activities.
[1]
They are
employed widely in medicinal chemistry as essential struc-
tural motifs for the development of new therapeutic agents.
Sulfonamide drugs have various clinical applications, in-
cluding as antibacterials, diuretics, anticonvulsants, and
HIV protease inhibitors.
[2]
Examples of important sulfon-
amide drugs are azosemide (diureatic), piroxicam (anti-in-
flammatory drug), sumatriptan (anti-migraine agent), and
amprenavir (protease inhibitor for treatment of HIV infec-
tion). Other applications of sulfonamides include their use
as nitrogen protecting groups and incorporation into or-
ganic dyes to improve stability and lubrication.
[3]
Because
of their significance, a number of advancements in sulfon-
amide synthesis have been developed, in order to provide
the sulfonamide products in decent yields and with high
selectivity and good functional group compatibility.
[4]
Ex-
amples of effective methods for sulfonamide formation in-
clude the traditional synthesis from sulfonyl chlorides and
amino compounds,
[5]
catalytic cross-coupling of sulfon-
amides with halides,
[6]
oxidation of sulfinamides,
[7]
and
aminosulfonation of hydrocarbons.
[8]
Despite their poten-
[a] Center of Excellence for Innovation in Chemistry
(PERCH-CIC), Department of Chemistry, Faculty of Science,
Mahidol University,
Rama VI Road, Bangkok 10400, Thailand
http://www.perch-cic.org/index.php
[b] Center of Catalysis, Department of Chemistry, Faculty of
Science, Mahidol University,
Rama VI Road, Bangkok 10400, Thailand
E-mail: sirilata.yot@mahidol.ac.th
http://chemistry.sc.mahidol.ac.th/en
Supporting information for this article is available on the
WWW under http://dx.doi.org/10.1002/ejoc.201403531.
Eur. J. Org. Chem. 2015, 1575–1582 © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 1575
be employed as the amine sources in this transformation.
Mechanistic studies indicated that a radical pathway might
be involved in the reaction process. This transition-metal-
free protocol offers an alternative and convenient approach
for a preparation of a series of sulfonamides in moderate to
good yields under mild conditions.
tial utility, many of these methods have some limitations
such as vigorous conditions, side reactions, tedious isolation
procedures, poor functional group tolerance, difficulty in
handling, and problems with long-term storage.
Recently, Jiang and co-workers reported a new route to
sulfonamide synthesis through Cu-catalyzed oxidative cou-
pling of amines and the bench-stable, nonhygroscopic so-
dium sulfinates.
[9,10]
This study offered a method for the
preparation of sulfonamides in good yields and with excel-
lent chemoselectivity; however, a high temperature is re-
quired to facilitate product formation. Inspired by this
work, we became interested in exploring the possibility of
replacing the copper catalyst by employing the transition-
metal-free catalyzed oxidative coupling strategy. In particu-
lar, catalysis involving molecular iodine (I
2
) and its salts
attracted our attention, due to the ease of handling, low
toxicity, commercial availability, and mild reactivity of the
reagents. A number of recent studies have demonstrated the
utility of iodine catalysis as an efficient and powerful tool
for formation of carbon–carbon and carbon–heteroatom
bonds.
[11]
The combination of catalytic amounts of iodine
or iodide salts and oxidants such as tert-butyl hydroperox-
ide (TBHP) or hydrogen peroxide (H
2
O
2
) has proven to
provide versatile oxidation conditions for many oxidative
coupling transformations.
[12]
Herein we report a method for the formation of sulfon-
amides by I
2
-catalyzed oxidative amination of sodium sulfi-
nates. Readily available sodium percarbonate – Na
2
CO
3
·
1.5 H
2
O
2
, a solid carrier of hydrogen peroxide
[13]
– is an
effective oxidant for this transformation. Our approach has
several advantages, including being transition-metal-free,
using bench-stable reagents, involving simple handling un-
der mild and air-stable conditions, accommodating a broad
scope of substrates, and avoiding the generation of toxic
byproducts.