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Construction of Metallosupramolecular Coordination Complexes: From Lanthanide Helicates to Octahedral Cages Showing Single-Molecule Magnet Behavior.

Inorganic Chemistry 2019 Februrary 19
The construction of metallosupramolecular complexes toward interesting topological structures is a critical challenge for chemists. The fluctuation in the synthetic strategy, by keeping the same metal-ligand combination, has proved a very significant approach to construct metallosupramolecular architectures. Herein, by varying the reaction conditions four new DyIII -supramolecular complexes based on a flexible dihydrazone ligand H2 L (H2 L = bis(2-hydroxy-3-methoxybenzylidene)adipohydrazide) in cooperation with different anions and solvents having formulas [Dy4 L4 (μ2 -N3 )2 ](NO3 )2 ·6CH3 OH·2H2 O (1), [Dy8 L8 (μ2 -CH3 OH)4 ]Cl8 ·6CH3 OH·14H2 O (2), [Dy12 L12 (μ2 -OH)2 (OH)6 (CH3 O)2 ](NO3 )2 ·2CH3 OH·14H2 O (3), and [Dy12 L12 (μ2 -OH)2 (NO3 )2 (OH)3 (CH3 O)](NO3 )4 ·22H2 O (4), have been successfully synthesized and their crystal structures confirmed by single crystal X-ray diffraction studies. The structural study reveals that 1 and 2 have quadruple-stranded helicate and dual triple-stranded helicate supramolecular structures, respectively, while 3 and 4 display "octahedron" cagelike supramolecular structures. The magnetic studies reveal that complexes 1-3 exhibit slow magnetic relaxation behavior, while complex 4 displays a series of typical frequency-dependent relaxation signals at 0 Oe applied dc field which is a rare case in polynuclear 4f single-molecule magnet (SMM) family to date. Interestingly, the distinct magnetic dynamic behavior was noticed for nearly isoskeletal complexes 3 and 4, which can be attributed to the modification of the coordination environment around DyIII ions.

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