Six lanthanide(III)-2,5-dihydroxy-1,4-benzenedicarboxylate frameworks, namely, [Ln(H(2)-DHBDC)(1.5)(H(2)O)(2)](n) (Ln = La (1) and Pr (2); H(4)-DHBDC = 2,5-dihydroxy-1,4-benzenedicarboxylic acid), {[Nd(H(2)-DHBDC)(1.5)(H(2)O)(3)](H(2)O)}(n) (3), {[Eu(H(2)-DHBDC)(NO(3))(H(2)O)(4)](H(2)O)(2)}(n) (4), and {[Ln(2)(H(2)-DHBDC)(2)(DHBDC)(0.5)(H(2)O)(3)](H(2)O)(4)}(n) (Ln = Gd (5) and Dy (6)), with four different structural types ranging from 1D chain, 2D layer to 3D networks have been synthesized and structurally characterized. Compounds La (1) and Pr (2) are isomorphous and exhibit 3D frameworks with the unique 1D tubular channels. Compounds Nd (3) and Eu (4) are 2D layer and 1D zigzag chain, respectively, which are further extended to 3D supramolecular frameworks through extensive hydrogen bonds. Isomorphous compounds of Gd (5) and Dy (6) are 3D frameworks constructed from secondary infinite rod-shaped metal-carboxylate/hydroxyl building blocks. While the hydroxyl groups as secondary functional groups in the 1D chain of Eu (4) and 2D layer of Nd (3) are not bonded to the lanthanide centers, the hydroxyl groups in the 3D frameworks of La (1), Pr (2), Gd (5), and Dy (6) participate in coordinating to lanthanide centers and thus modify the structural types of theses compounds. The magnetic data of compounds Pr (2), Nd (3), Gd (5), and Dy (6) have been investigated in detail. In addition, elemental analysis, IR spectra, powder X-ray diffraction (PXRD) patterns and thermogravimetric analysis of these compounds are described.
An organic ligand 4-(1,2,4-triazol-1-yl) benzoic acid
(Htzbc) with a nonlinear optical (NLO) chromophore has been synthesized.
Reaction of Zn(NO3)2 with Htzbc ligand in 1-n-butyl-3-methylimidazolium tetrafluoroborate ionic liquid
afforded compound Zn(tzbc)2 (1). The Htzbc
organic solid and 1 crystallize in the acentric Pn and Cc space groups, respectively. The
tetrahedral Zn2+ center in 1 coordinates to
two triazole nitrogen atoms and two carboxylate oxygen atoms from
four tzbc– ligands, leading to a noncentrosymmetric
5-fold interpenetrating diamondoid network. Second-harmonic generation
(SHG) measurements revealed the Htzbc solid and 1 have
SHG activities. The Htzbc compound has a large SHG effect, which is
approximately 3 times that of KDP and is type-I phase matchable, while 1 also belongs to phase-matchable class with a SHG response
of about 1.2 times that of KDP. The SHG active of the organic solid
can be derived from the inherently dipolar Htzbc molecule as well
as the optimal relative orientation of the molecular NLO-phores in
the crystal packing. The odd number-fold interpenetrated diamondoid
network with dipolar NLO chromophoric units based on asymmetrical
bridging ligands and metal centers results in the SHG activity of 1. In addition, elemental analysis, IR spectra, powder X-ray
diffraction patterns (PXRD), and thermogravimetric analysis of both
compounds are described.
The title compound, [CuNa(C(4)H(3)O(7)S)(C(10)H(8)N(2))(H(2)O)(3)](n), consists of one Cu(II) cation, one Na(I) cation, one 2-sulfonatobutanedioate trianion (SSC(3-)), one 2,2'-bipyridyl (bpy) ligand and three coordinated water molecules as the building unit. The coordination of the Cu(II) cation is composed of two pyridyl N atoms, one water O atom and two carboxylate O atoms in a distorted square-pyramidal coordination geometry with an axial elongation. The Na(I) cation is six-coordinated by three water molecules and three carboxylate O atoms from three SSC(3-) ligands in a distorted octahedral geometry. Two SSC(3-) ligands link two Cu(II) cations to form a Cu(2)(SSC)(2)(bpy)(2) macrocyclic unit lying across an inversion centre, which is further linked by Na(I) cations via Na-O bonds to give a one-dimensional chain. Interchain hydrogen bonds link these chains to form a two-dimensional layer, which is further extended into a three-dimensional supramolecular framework through π-π stacking interactions. The thermal stability of the title compound has also been investigated.
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