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Auxiliary Ligand-Dependent Adaptive Regulation of Uranyl Coordination in Mixed-Ligand Uranyl Compounds of Flexible Biphenyltetracarboxylic Acid
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-11-13 , DOI: 10.1021/acs.inorgchem.0c02904
Jun-Feng Qian 1 , Wen-Jiang Tian 2 , Song Yang 1 , Zhong-Hua Sun 1 , Le Chen 1 , Mei-Jun Wei 1 , Zhong Wu 1 , Ming-Yang He 1 , Zhi-Hui Zhang 1 , Lei Mei 2
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2020-11-13 , DOI: 10.1021/acs.inorgchem.0c02904
Jun-Feng Qian 1 , Wen-Jiang Tian 2 , Song Yang 1 , Zhong-Hua Sun 1 , Le Chen 1 , Mei-Jun Wei 1 , Zhong Wu 1 , Ming-Yang He 1 , Zhi-Hui Zhang 1 , Lei Mei 2
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The mixed-ligand strategy is one of the important methods for preparing new materials and regulating the properties of materials. In this work, by introducing different auxiliary ligands (ALs), we have obtained a series of mixed-ligand uranyl complexes (1–6) from a flexible biphenyltetracarboxylic acid (H4bptc) with an adjustable orthogonal conformation and studied the influence of different organic base molecules on the coordination and assembly of H4bptc with a uranyl cation. It is found that the coordinated ALs, including 4,4′-bipyridine-1,1′-dioxide and 1,10-phenanthroline, partially occupy the coordination sites of the uranyl center and directly affect the molecular conformations and uranyl coordination of flexible bptc linkers. On the other hand, noncoordinated ALs such as protonated 4,4′-bipyridine ([H2(4,4′-bpy)]2+) or dimethylammonium, which work as counterions in the form of encapsulated guests or hydrogen-bonded templates, also have a nonnegligible impact on the conformation and coordination of bptc linkers. Most interestingly, the AL-mediated evolution of uranyl coordination by the bptc linker and coordination geometry of the uranyl center is clearly observed, which suggests the adaptability of flexible bptc linkers to take suitable molecular configurations and uranyl coordination modes so as to adapt to the external regulator agents and varying environment. The physicochemical characterization of these uranyl compounds, especially photoluminescence, is addressed and discussed, and the results reveal that compound 5 has the potential to serve as a multifunctional radiation detection material for UV light and X-ray radiation.
中文翻译:
柔性联苯四甲酸混合配体铀酰化合物中铀配位的辅助配体依赖性自适应调节
混合配体策略是制备新材料和调节材料性能的重要方法之一。在这项工作中,通过引入不同的辅助配体(ALS),我们获得了一系列的混合配体铀酰复合物(的1 - 6由柔性联苯四羧酸(H)4 BPTC)具有可调节的正交构象和研究的不同的影响有机碱分子对H 4的配位和组装具有铀酰阳离子的bptc。发现4,4'-联吡啶-1,1'-二氧化物和1,10-菲咯啉等配位的AL部分占据了铀酰中心的配位部位,直接影响了柔性bptc的分子构象和铀酰配位。连接器。另一方面,非配位的AL,如质子化的4,4'-联吡啶([H 2(4,4'-bpy)] 2+)或二甲基铵,它们以包封的客体或氢键合模板的形式作为抗衡离子,对bptc接头的构象和配位也具有不可忽略的影响。最有趣的是,清楚地观察到了bptc接头通过AL介导的铀酰配位演化以及铀酰中心的配位几何结构,这表明柔性bptc接头可采用合适的分子构型和铀酰配位模式以适应外部环境。调节剂和变化的环境。这些铀酰化合物的物理化学特征,特别是光致发光,已得到解决和讨论,结果表明化合物5 有潜力用作紫外线和X射线辐射的多功能辐射检测材料。
更新日期:2020-12-07
中文翻译:

柔性联苯四甲酸混合配体铀酰化合物中铀配位的辅助配体依赖性自适应调节
混合配体策略是制备新材料和调节材料性能的重要方法之一。在这项工作中,通过引入不同的辅助配体(ALS),我们获得了一系列的混合配体铀酰复合物(的1 - 6由柔性联苯四羧酸(H)4 BPTC)具有可调节的正交构象和研究的不同的影响有机碱分子对H 4的配位和组装具有铀酰阳离子的bptc。发现4,4'-联吡啶-1,1'-二氧化物和1,10-菲咯啉等配位的AL部分占据了铀酰中心的配位部位,直接影响了柔性bptc的分子构象和铀酰配位。连接器。另一方面,非配位的AL,如质子化的4,4'-联吡啶([H 2(4,4'-bpy)] 2+)或二甲基铵,它们以包封的客体或氢键合模板的形式作为抗衡离子,对bptc接头的构象和配位也具有不可忽略的影响。最有趣的是,清楚地观察到了bptc接头通过AL介导的铀酰配位演化以及铀酰中心的配位几何结构,这表明柔性bptc接头可采用合适的分子构型和铀酰配位模式以适应外部环境。调节剂和变化的环境。这些铀酰化合物的物理化学特征,特别是光致发光,已得到解决和讨论,结果表明化合物5 有潜力用作紫外线和X射线辐射的多功能辐射检测材料。