Novel Uranyl Coordination Polymers Based on Quinoline-Containing Dicarboxylate by Altering Auxiliary Ligands: From 1D Chain to 3D Framework

铀酰 结晶学 化学 配体(生物化学) 氢键 戒指(化学) 喹啉 质子化 配位聚合物 配位几何学 晶体结构 分子 立体化学 离子 有机化学 受体 生物化学
作者
Kong‐Qiu Hu,Liu-Zheng Zhu,Cong‐Zhi Wang,Lei Mei,Yunhai Liu,Zengqiang Gao,Zhifang Chai,Wei‐Qun Shi
出处
期刊:Crystal Growth & Design [American Chemical Society]
卷期号:16 (9): 4886-4896 被引量:29
标识
DOI:10.1021/acs.cgd.6b00429
摘要

Novel uranyl coordination polymers, UO2(bqdc)(phen)·H2O (1), [UO2(μ-OH)(bqdc)(H2bpy)0.5(H2O)] (2), Na[(UO2)2(bqdc)3Na(H2O)2] (3), and [Na(bqdc)0.5(bpp)(H2O)] (4) (H2bqdc = 2,2′-biquinoline-4,4′-dicarboxylic acid; phen = 1,10-phenanthroline; bpy = 4,4′-bipyridine; bpp = 1,3-di(4-pyridyl)propane), with bqdc2– ligands have been successfully synthesized by hydrothermal reactions and characterized by single-crystal X-ray diffraction, Infrared spectroscopy (IR), thermogravimetric analysis (TGA), and powder X-ray diffraction (PXRD). The topological structures feature 1D chain to 3D framework by altering N-donor ancillary ligands. Compound 1 shows a 1D wave-shaped zigzag chain structure and further extends to a two-dimensional (2D) layer through π···π interactions between the quinoline ring of bqdc2– ligand and benzene ring of phen ligand. The uranium adopts an approximate hexagonal bipyramidal coordination geometry with the equatorial plane warped to the unusual chair conformation. Compound 2 features rectangular-shaped units with space range of 12.28(2) Å × 7.16(3) Å, exhibiting an intriguing 2D uranyl double layered motif formed by 1D ladder chains. The protonated bpy molecules provide space filling and form hydrogen bonds with the layers. Compound 3 is based upon 3D heterometallic frameworks constructed from UO22+, Na+, and bqdc2– ligands. The most striking feature of compound 3 is that one sodium ion is located in the middle of two adjacent uranyl ions, forming the trinuclear heterometal clusters (U2Na), which are further connected by bqdc2– ligands to generate UOFs with the cavity size of 10.07(0) Å × 13.86(2) Å. The local 1D structure of compound 3 is similar to the zigzag chain of compound 1. Compound 4 displays 1D chain structure and further extends to 3D framework via hydrogen bond and π···π interactions. Moreover, the electronic structural and bonding properties of the uranyl compounds 1–3 have been systematically explored by density functional theory (DFT) calculations.

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