ARTICLE
DOI: 10.1002/zaac.201300082
Copper(II) Complex with the Tridentate Ligand N,N-bis(2-ethyl-4-methyl-
imidazol-5-ylmethyl)phenylethylamine (biaq). X-ray Crystal Structure and
Biological Activity on Bacillus subtilis of [Cu(biaq)Cl
2
].
Ángeles Mendoza,
[a]
Guillermo Mendoza-Díaz,*
[b]
Mario Pedraza-Reyes,
[c]
and
Sylvain Bernès
[d]
Keywords: Antibacterial properties; Copper; Imidazole derivatives; Mutagenic activity
Abstract. The ligand N,N-bis(2-ethyl-4-methyl-imidazol-5-ylmethyl)-
1-phenylethylamine (biaq) was prepared by Mannich reaction of 2-
ethyl-4-methyl-1H-imidazole, (R)-1-phenylethylamine and formalde-
hyde. It was characterized by FTIR and NMR spectroscopy. This li-
gand reacts with CuCl
2
to give a coordination compound with formula
[Cu(biaq)Cl
2
]. In this compound, biaq acts as a tridentate ligand with
one tertiary amine and two azole nitrogen atoms coordinated to the
central metal atom. The complex was characterized by FTIR spec-
troscopy, elemental analysis, and X-ray diffraction. The X-ray struc-
1 Introduction
Imidazole-based ligands have been matter of medical inter-
est because they may have some biological activities as anti-
bacterial and antiparasitic agents. Also, the development of
such ligands is related to the preparation of small molecules
that may mimic some copper-containing enzymes, and there-
fore may have some interesting catalytic effects. The interest
in having a better understanding of how central copper atoms
work in biological systems, in order to develop new metal-
based drugs, is still a growing topic. In particular, this interest
has been directed toward the synthesis of copper complexes
with imidazole derivatives. Some of these imidazole-based li-
gands, NL
3
(L = imidazole
[1–3]
), have a tripodal shape. The
interest in this type of ligands comes from the fact that in
* Prof. Dr. G. Mendoza-Díaz
E-Mail: mendozag@ugto.mx
[a] Departamento de Química
División de Ciencias Naturales y Exactas
Campus Guanajuato, Universidad de Guanajuato
Noria Alta s/n
Guanajuato, Gto. 36050, Mexico
[b] Departamento de Ingenierías Química
Electrónica y biomédica, División de Ciencias e Ingenierías
Campus León, Universidad de Guanajuato
Loma del Bosque 103
Lomas del Campestre, León, Guanajuato. 37150, Mexico
[c] Departamento de Biología
División de Ciencias Naturales y Exactas
Campus Guanajuato, Universidad de Guanajuato
Noria Alta s/n
Guanajuato, Gto. 36050 Mexico
[d] DEP Facultad de Ciencias Químicas, UANL
Guerrero y Progreso s/n Col. Treviño
64570 Monterrey, NL, Mexico
Z. Anorg. Allg. Chem. 2013, 639, (8-9), 1455–1460 © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 1455
ture of [Cu(biaq)Cl
2
] shows a pentacoordinate cooper(II) atom, where
two chloride ions and the three nitrogen atoms of the biaq ligand are
coordinated in a distorted square pyramidal arrangement. The bio-
logical activity of the complex [Cu(biaq)Cl
2
] was tested using the
Gram positive bacterium Bacillus subtilis as a model. Results revealed
that the copper complex interfered with bacterial growth, inducing cell
death, most probably by altering the primary structure of the chromo-
some, since a significant increase of the mutation frequency to rifampi-
cin resistance was observed.
many copper metalloproteins imidazole residues from histidine
appear to be coordinated to copper.
[4,5]
Therefore, the synthesis
of small complexes that could mimic the coordination environ-
ment, catalytic behavior or spectroscopic properties of such
metalloproteins, is currently a challenge for many groups. Se-
lected examples of ligands and complexes reported in the
literature related to the present work may be cited: The
linear tridentate ligand N,N-bis(2-ethyl-5-methylimidazol-4-yl-
methyl)aminopropane (biap) and the coordination compounds
of biap with Co
II
, Ni
II
, Zn
II
,
[6]
Fe
III
,
[7]
and Cu
II[8]
have been
reported. The copper complex of biap has been used success-
fully for modeling nitrite reductase.
[9]
Similar ligands as
N,N-bis(2-ethyl-5-methylimidazol-4-ylmethyl)aminomethane
(biam), N,N-bis(2-ethyl-5-methylimidazol-4-ylmethyl)amino-
ethanol (biae), and N,N-bis(2-ethyl-5-methylimidazol-4-yl-
methyl)amino-2-ethylpyridine (biapy) form complexes with
copper(II) featuring a distorted square pyramidal environ-
ment.
[8]
All the above mentioned ligands were prepared by a
Mannich condensation, a straightforward reaction using simple
reagents like formaldehyde, amines, and imidazoles.
[6,9]
in a
one pot procedure.
On the other hand, antibiotic rifampicin, a potent inhibitor
of prokaryotic transcription
[10]
has been used as a highly clini-
cally effective drug, particularly in the treatment of tuberculo-
sis. Mutations conferring rifampicin resistance (Rif
R
) occur at
specific clusters within the gene encoding the β subunit of
the prokaryotic RNA polymerase. Rif
R
RNA polymerases have
been extensively characterized in E. coli; these have altered
properties in transcription elongation and/or termination.
[11]
In
E. coli, Rif
R
mutations are usually located in the central region