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Synthesis and Characterization of Functionalized Metal-organic Frameworks
Published on: September 5, 2014
Six uranyl-organic frameworks with naphthalene-dicarboxylic acid and bipyridyl-based spacers: syntheses, structures,
Wei Xu1, Ya-Nan Ren1, Miao Xie1
1Joint Laboratory for Environmental Test and Photocatalytic Research of Ningbo University-Zhejiang Zhonghao Applied Engineering Technology Institute Co., Ltd, Research Center of Applied Solid State Chemistry, Chemistry Institute for Synthesis and Green Application, Ningbo University, Ningbo, Zhejiang, 315211 P.R. China. zhengyueqing@nbu.edu.cn.
Abstract:
A new series of uranium coordination polymers have been hydrothermally synthesized by using 1,4-naphthalene dicarboxylic acid (H2NDC), namely, (H3O)2[(UO2)2(NDC)3]·H2O (1), (H2-bpp)[(UO2)2(NDC)3]·EtOH·5H2O (2), (H2-bpe)2/2[(UO2)2(NDC)3]·EtOH (3), (H2-bpp)[(UO2)2(NDC)3]·5H2O (4), (H2-bpp)[(UO2)(HNDC)(NDC)]2·2H2O (5), and (H2-bpy)[(UO2)(NDC)2] (6) [bpp = 1,3-di(4-pyridyl) propane, bpe = 4,4'-vinylenedipyridine, bpy = 4,4'-bipyridine]. Single-crystal X-ray diffraction demonstrates that complex 1 represents the uranyl-organic polycatenated framework derived from a simple two-dimensional honeycomb grid network structure via a H2NDC linker. Complexes 2-4 contain the dinuclear motifs of the two UO7 pentagonal and one UO8 hexagonal bipyramids which are linked by NDC2- anions creating a (UO2)4(NDC)2 unit, and further extend to a 2D layer through NDC2- anions. Complex 5 displays a 1D zigzag double chain structure, in which the carboxylate groups of the NDC2- anions adopt a chelate mode and further extends to a 2D framework via hydrogen bonds. The 1D structure of complex 6 is similar to the zigzag chain of complex 5. In addition, powder X-ray diffraction, elemental analysis, IR, thermal stability and luminescence properties of all complexes have also been investigated in this paper. The photocatalytic properties of the six complexes for the degradation of tetracycline hydrochloride (TC) under UV irradiation have been examined. Moreover, density functional theory (DFT) calculations were carried out to explore the electronic structural and bonding properties of the uranyl complexes 1-6.
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