ARTICLE
DOI: 10.1002/zaac.200900300
Two-Dimensional Lanthanide-Containing Coordination Frameworks:
Structure, Magnetic and Luminescence Properties
Ting Gao,
[a,b]
Guang-Ming Li,
[a,b]
Peng-Fei Yan,*
[a,b]
Ju-Wen Zhang,
[a,b]
Wen-Bin Sun,
[a,b]
Masayuki Suda,
[c]
and Yasuaki Einaga*
[c]
Keywords: Salen; Lanthanides; Magnetic properties; Luminescence; Polymers
Abstract. Two lanthanide-containing 2D coordination polymers,
[Ln(H
2
salen)
1.5
(NO
3
)
3
]
n
[H
2
salen = N,N'- ethylenebis(salicylideneim-
ine); Ln = Gd (1), Dy (2)], have been prepared by self-assembly
method. The molecular magnetism and luminescence of the metal
Introduction
Lanthanide complexes are currently of great interest because
of their unique physicochemical properties and various appli-
cations as new materials [1]. Especially, the luminescence [2]
and magnetism [3] of lanthanide complexes have aroused
much attention recently. The lanthanide ions have narrow
emission bands and relatively long luminescence lifetimes as
a result of transitions within the partially filled 4f shell of the
ions [4]. Lanthanide complexes are the most employed for ap-
plications such as fluoroimmunoassays and fluorescence mi-
croscopy [5]. In addition, lanthanide ions have long been ex-
ploited to influence the properties of magnets by introducing
anisotropic contributions [6]. Since few simple compounds
containing magnetically coupled f-block ions were available,
little is known about the nature of the exchange interactions
among rare earth ions and other magnetic groups. Generally,
the interaction between the adjacent lanthanide ions is ferro-
magnetic or antiferromagnetic in nature [7]. In the past years,
few homodinuclear or homopolynuclear lanthanide complexes
have been reported and their magnetic behaviors were found
to be ferromagnetic or antiferromagnetic interactions between
the Ln···Ln ions because of the different bridging ligands or
atoms [8]. Typical salen ligands, tetradentate Schiff bases de-
rived from salicylaldehyde and diamines with two N-donor and
two O-donor chelating centers suitable for the lanthanide ions
* Prof. Dr. P.-F. Yan
E-Mail: yanpf@vip.sina.com
* Prof. Dr. Y. Einaga
E-Mail: einaga@chem.keio.ac.jp
[a] Key Laboratory of Functional Inorganic Chemistry
Heilongjiang University
Harbin 150080, P. R. China
[b] School of Chemistry and Materials Science
Heilongjiang University
Harbin 150080, P. R. China
[c] Department of Chemistry
Keio University
Yokohama 223–8522, Japan
624 © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Z. Anorg. Allg. Chem. 2010, 636, 624–628
complexes had been studied. Complex 1 exhibits antiferromagnetic in-
teraction between spin carriers. Complex 2 emits the H
2
salen ligand
luminescence.
to form homodinuclear [9] or homopolynuclear complexes
[10].
As a contribution to the understanding of the molecular mag-
netism and luminescence of lanthanide complexes with flexi-
ble salen ligands, we present herein the synthesis, structural,
luminescence, and magnetic properties of two 2D complexes
based on the salen ligand N,N'-ethylenebis(salicylideneimine),
generally formulated as [Ln(H
2
salen)
1.5
(NO
3
)
3
]
n
[Ln = Gd (1),
Dy (2)]. Although a number of salen and salen-like lanthanide
complexes with different compositions have been reported de-
pending on the preparative procedures, to the best of our
knowledge, structurally characterized salen and/or salen-like
lanthanide complexes are rare [11]. The coordination modes of
salen and/or salen-like ligand are usually proposed on the basis
of the spectroscopic data [12].
Results and Discussion
Synthesis and Characterization
Reactions of the salen ligand with Ln(NO
3
)
3
·6H
2
O in a molar
ratio of 1:1 were carried out in MeOH/CH
2
Cl
2
at ambient tem-
perature. Methylene dichloride was employed to increase the
solubility of salen ligand. The immediate color change of the
solution upon addition of Gd(NO
3
)
3
·6H
2
O and Dy(NO
3
)
3
·
6H
2
O indicates instant occurrence of the coordination reaction.
Single crystals suitable for X-ray analysis were obtained by
slow diffusion of ethyl ether into the methanol solution of the
powder sample. Complexes 1 and 2 are stable in air and mod-
erately soluble in polar organic solvent such as methanol, etha-
nol, and DMF. X-ray crystal analyses reveal that one type co-
ordination complexes, [Ln(H
2
salen)
1.5
(NO
3
)
3
]
n
[Ln = Gd (1),
Dy (2)] (Scheme 1) are isolated.