ISSN 1070-3632, Russian Journal of General Chemistry, 2017, Vol. 87, No. 4, pp. 842–845. © Pleiades Publishing, Ltd., 2017.
842
1,4-Bis(triphenylphosphonium)-2-butene Peroxodisulfate
as an Efficient Oxidizing Agent for One-Pot Synthesis
of Ethyl Pyrimidin-2(1H)-one-5-carboxylates
1
M. Gorjizadeh* and M. Afshari
Department of Chemistry, Shoushtar Branch, Islamic Azad University, Shoushtar, Iran
*e-mail: m.gorjizadeh@iau-shoushtar.ac.ir
Received January 11, 2017
Abstract—An efficient one-pot synthesis of pyrimidin-2(1H)-ones via three-component condensation of aldehyde,
ethyl acetoacetate and urea using 1,4-bis(triphenylphosphonium)-2-butene peroxodisulfate [BTPBPDS] as an
oxidant is described.
Keywords: pyrimidin-2(1H)-ones, 1,4-bis(triphenylphosphonium)-2-butene peroxodisulfate, oxidation, one-pot
1
The text was submitted by the authors in English.
INTRODUCTION
Multi-component reactions (MCRs), leading to
interesting heterocyclic scaffolds, are particularly
useful for construction of diverse chemical libraries of
“drug-like” molecules. Typically, purification of products
accumulated in MCRs is simple because all organic
reagents involved are consumed and incorporated into
the structure of a target compound [1].
Pyrimidines revealed a wide range of pharma-
ceutical activities including antiviral, antimicrobial,
gastric antisecretory, diuretic, antimalarial, and anti-
HIV [2–7]. Itami and co-workers [8] have reported that
pyrimidine cores with extended π-systems exhibited
unusual fluorescent properties. Despite of high bio-
logical activity of pyrimidines and particularly
pyrimidin-2(1H)-ones, only a limited number of syn-
thetic approaches to those are available [9]. One of the
common methods involves oxidation of 3,4-dihydro-
pyrimidin-2(1H)-ones (DHPMs) to pyrimidin-2(1H)-
ones. 3,4-Dihydropyrimidin-2(1H)-ones can be easily
synthesized from ethyl acetoacetate, an aromatic
aldehyde and urea [10]. Dehydrogenation of DHPMs
by an oxidizing agent could provide an efficient ap-
proach to pyrimidin derivatives. Phosphonium salts
have attracted close attention due to their thermal
stability, easy handling, non-toxicity, high reactivity,
and recyclability [11–13].
As a part of our ongoing study devoted to develop-
ing versatile and efficient methods for the synthesis of
important heterocyclic compounds [14, 15], we report
herein a new procedure for one-pot synthesis of
pyrimidin-2(1H)-ones.
RESULTS AND DISCUSSION
A two-step synthesis of pyrimidin-2(1H)-ones
under study is presented in Scheme 1. Thus, the reac-
tion of an aromatic aldehyde with ethyl acetoacetate
and urea in the presence of catalytic amount of 1,4-bis-
(triphenylphosphonium)-2-butene peroxodisulfate
(BTPBPDS) led to formation of the corresponding 3,4-
dihydropyrimidin-2(1H)-ones 4.
3,4-Dihydropyrimidin-2(1H)-ones 4 bearing a
variety of functional groups were prepared in high
yields in a short period of time (Table 1). BTPBPDS
could play a crucial role in accelerating the steps of
dehydration and enolization of the β-ketoester.
Subsequently, compounds 4 underwent oxidation by
BTPBPDS (Scheme 1, Table 1). This step proceeded
within 55–110 min in CH
3
CN under reflux. Sensitive
functional groups such as methoxy, nitro, and furyl
remained unaffected in the process.
According to the recent study [16] adsorption on
solid supports (alumina, silica gel, or montmorillonite
K-10 clay) can change the reactivity and selectivity of
oxidants. The test oxidation of 4 by peroxodisulfate
adsorbed by solid supports in the process of dehydro-
DOI: 10.1134/S1070363217040284