Angewandte
Communications
Chemie
BN heterocycles
A Modular Synthetic Approach to Monocyclic 1,4-Azaborines
Xuguang Liu, Yuanzhe Zhang, Bo Li, Lev N. Zakharov, Monica Vasiliu, David A. Dixon,* and
Shih-Yuan Liu*
Abstract: A simple and general method for the synthesis of
a wide range of monocyclic 1,4-azaborines, including the first
examples containing B heteroatoms is described. Post-hetero-
cycle-formation olefin isomerization was employed as a key
strategy. This new synthetic method provides fundamental
insight into the resonance stabilization and photophysical
properties of 1,4-azaborines.
BN/CC isosterism, which is the replacement of a CC unit
with the isoelectronic and isostructural BN unit, has emerged
as a viable strategy to increase the chemical space of
compounds relevant to materials science and biomedical
research.[1] The application of BN/CC isosterism to the
benzene motif leads to three structural isomers: 1,2-dihy-
drido-1,2-azaborine, 1,3-dihydrido-1,3-azaborine, and 1,4-
dihydrido-1,4-azaborine (from hereon, abbreviated as 1,2-
azaborine, 1,3-azaborine, and 1,4-azaborine, respectively).
While significant advances have been made in the develop-
ment of 1,2-azaborine derivatives,[1,2] less progress has been
reported for 1,3-[3] and 1,4-azaborine[4] derivatives, which is
arguably due to a lack of general synthetic access to these
families of compounds. For 1,4-azaborines, most of the
pioneering work has centered on polycyclic dibenzofused
derivatives (Scheme 1), which can be prepared from stable
halogenated diarylamines.[5] Recently, we reported the syn-
thesis of monobenzofused 1,4-azaborines and described their
potential application in coordination chemistry and cataly-
sis.[6,7] However, the chemistry of the simplest monocyclic 1,4-
azaborine has remained virtually unexplored. Braunschweig
and co-workers reported the only synthesis and isolation of
a monocyclic 1,4-azaborine to date, which involves Rh-
mediated cyclization of N-tBu-B-tBu iminoborane with
acetylene.[8] Although elegantly simple, the reported synthetic
scope was limited to one example, namely, N-tBu-B-tBu-1,4-
azaborine (Scheme 1).
Scheme 1. Development of 1,4-azaborines.
In order to unleash the full potential of the chemistry of
1,4-azaborines as a new benzene isostere, a more versatile
synthesis needs to be developed that can access a wide range
of substituted monocyclic 1,4-azaborine derivatives. In this
work, we disclose a modular synthetic approach to the
preparation of N- and B-substituted monocyclic 1,4-azabor-
ines.
Scheme 2 illustrates our retrosynthetic analysis for the
assembly of the 1,4-azaborine ring. In analogy to the synthesis
of dibenzofused 1,4-azaborines,[4,5] a monocyclic 1,4-azabor-
ine could potentially be prepared through coupling of the
dilithium reagent produced from the dibromide A with
a boron electrophile (Scheme 2, route I). However, in con-
[*] Dr. X. Liu, Y. Zhang, Dr. B. Li, Prof. Dr. S.-Y. Liu
Department of Chemistry, Boston College
Chestnut Hill, MA 02467 (USA)
E-mail: shihyuan.liu@bc.edu
Dr. L. N. Zakharov
Department of Chemistry, University of Oregon (USA)
Dr. M. Vasiliu, Prof. Dr. D. A. Dixon
Department of Chemistry, The University of Alabama
Tuscaloosa, AL 35487 (USA)
E-mail: dadixon@as.ua.edu
Dr. X. Liu
Present address: College of Chemistry and Chemical Engineering
Tianjin University of Technology (China)
Supporting information for this article can be found under:
Scheme 2. Retrosynthetic analysis.
Angew. Chem. Int. Ed. 2016, 55, 1 – 6
ꢀ 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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