Reductive Denitrogenation of Six-membered Cyclic Nitronates to
Densely Substituted Dihydrofurans with Raney
®
Nickel/AcOH
System
Evgeny V. Pospelov,
a
Alexander V. Zhirov,
a, b
Baglan Kamidolla,
a, c
and
Alexey Yu. Sukhorukov
a,
*
a
N. D. Zelinsky Institute of Organic Chemistry, 119991, Leninsky prospect, 47, Moscow, Russia
E-mail: sukhorukov@ioc.ac.ru; a.yu.sukhorukov@gmail.com
b
Department of Chemistry, M.V. Lomonosov Moscow State University, 119991, Leninskie gory, 1, str. 3, Moscow, Russia
c
D. Mendeleev University of Chemical Technology of Russia, 125047, Miusskaya sq., 9, Moscow, Russia
Manuscript received: May 30, 2023; Revised manuscript received: July 12, 2023;
Version of record online: August 1, 2023
Supporting information for this article is available on the WWW under https://doi.org/10.1002/adsc.202300573
Abstract: A protocol for the synthesis of 2,3-
dihydrofurans by reductive denitrogenation/ring
contraction of 6-membered cyclic nitronates was
developed. The process utilizes cheap Raney
®
nickel
both as catalyst and stoichiometric agent without the
need for high-pressure equipment. The products are
formed in high purity and column chromatography
is often not required. Studies on the substrate scope,
functional group tolerance, and mechanism were
performed. The developed approach provides a
straightforward two-step access to densely substi-
tuted 2,3-dihydrofurans from nitrostyrenes and
alkenes.
Keywords: Dihydrofurans; Denitrogenation; Ring
contraction; Heterogeneous catalysis; Nitronates
2,3-Dihydrofuran is an important five-membered het-
erocycle that is present in many natural compounds
and active pharmaceutical ingredients. Representative
examples include anti-inflammatory drug Polmacoxib
(Acelex
®
),
[1]
herbicide (R)-flurtamone,
[2]
and Austocys-
tin D, a natural compound with potent cytotoxic
activity (Scheme 1, a).
[3]
2,3-Dihydrofurans serve as
key intermediates in organic synthesis as reactive π-
nucleophiles, dipolarophiles, dienophiles in the in-
verse-electron demand Diels-Alder reaction, and surro-
gates of γ-hydroxycarbonyl compounds in heterocycli-
zation reactions.
[4]
Apart from this, simple 2,3-
dihydrofurans were recently shown to be useful
monomers for production of degradable thermoplastic
elastomers.
[5]
Though numerous methods to assemble
Scheme 1. Background of the study.
COMMUNICATIONS doi.org/10.1002/adsc.202300573
Adv. Synth. Catal. 2023, 365, 2850 – 2857 © 2023 Wiley-VCH GmbH 2850