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首页> 外文期刊>Crystal growth & design >Role of N-Donor Sterics on the Coordination Environment and Dimensionality of Uranyl Thiophenedicarboxylate Coordination Polymers
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Role of N-Donor Sterics on the Coordination Environment and Dimensionality of Uranyl Thiophenedicarboxylate Coordination Polymers

机译：N-施主化合物对铀酰噻吩二羧酸酯配位聚合物配位环境和尺寸的影响

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摘要

Thiophene 2,5-dicarboxylic acid (TDC) was reacted with uranyl acetate dihydrate and one (or none) of six N-donor chelating ligands (2,2'-bipyridine (BPY), 4,4'-dimethyl-2,2'-bipyridine (4-MeBPY), 5,5'-dimethyl-2,2'-bipyridine (5-MeBPY), 6,6'-dimethyl-2,2'-bipyridine (6-MeBPY), 4,4',6,6'-tetramethyl-2,2'-bipyridine (4,6-MeBPY), and tetrakis(2-pyridyl)pyrazine (TPPZ) to result in the crystallization of seven uranyl coordination polymers, which were characterized by their crystal structures and luminescence properties. The seven coordination polymers, Na-2[(UO2)(2)(C6H2O4S)(3)]center dot 4H(2)O (1), [(UO2)(4)(C6H2O4S)(5)(C10H8N2)(2)]center dot C10H10N2 center dot 3H(2)O (2), [(UO2)(C6H2O4S)(C12H12N3)] (3), [(UO2)(C6H2O4S)(C12H12N3)]center dot H2O (4), [(UO2)(2)(C6H2O4S)(3)]center dot(C12H14N2)center dot 5H(2)O (5), [(UO2)(3)(CH3CO2)(C6H2O4S)(4)](C14H17N2)(3)center dot(C14H16N2)center dot H2O (6), and [(UO2)(2)(C6H2O4S)(3)](C24H18N6) (7), consist of either uranyl hexagonal bipyramidal or pentagonal bipyramidal coordination geometries. In all structures, structural variations in the local and global structures of 1-7 are influenced by the positions (or number) of methyl groups or pyridyl rings on the N-donor species, thus resulting in a wide diversity of structures ranging from single chains, double chains, or 2-D sheets. Direct coordination of N-donor ligands to uranyl centers is observed in the chain structures of 2-4 using BPY, 4-MeBPY, and 5-MeBPY, whereas the N-donor species participate as guests (as either neutral or charge balancing species) in the chain and sheet structures of 5-7 using 6-MeBPY, 4,6-MeBPY, and TPPZ, respectively. Compound 1 is the only structure that does not contain any N-donor ligands and thus crystallizes as a 2-D interpenetrating sheet. The luminescent properties of 1-7 are influenced by the direct coordination or noncoordination of N-donor species to uranyl centers. Compounds 2-4 exhibit typical UO22+ emission upon direct coordination of N-donors, but its absence is observed in 1, 5, 6, and 7, when N-donor species participate as guest molecules. These results suggest that direct coordination of N-donor ligands participate as chromophores, thus resulting in possible UO22+ sensitization. The lack of emission in 1, 5, 6, and 7 may be explained by the extended conjugation of the TDC ligands within their structures.
机译：噻吩2,5-二羧酸（TDC）与乙酸铀酰二水合物和六个N-给体螯合配体（2,2'-联吡啶（BPY），4,4'-二甲基-2,2）之一（或不反应） '-联吡啶（4-MeBPY），5,5'-二甲基-2,2'-联吡啶（5-MeBPY），6,6'-二甲基-2,2'-联吡啶（6-MeBPY），4,4 '，6,6'-四甲基-2,2'-联吡啶（4,6-MeBPY）和四（2-吡啶基）吡嗪（TPPZ）导致7种铀酰配位聚合物的结晶Na-2 [（UO2）（2）（C6H2O4S）（3）]中心点4H（2）O（1），[（UO2）（4）（C6H2O4S）（ 5）（C10H8N2）（2）]中心点C10H10N2中心点3H（2）O（2），[（UO2）（C6H2O4S）（C12H12N3）]（3），[（UO2）（C6H2O4S）（C12H12N3）]中心点H2O（4），[（UO2）（2）（C6H2O4S）（3）]中心点（C12H14N2）中心点5H（2）O（5），[（UO2）（3）（CH3CO2）（C6H2O4S）（ 4）]（C14H17N2）（3）中心点（C14H16N2）中心点H2O（6）和[（UO2）（2）（C6H2O4S）（3）]（C24H18N6）（7），由铀酰六角双锥体或p对角双锥体协调几何。在所有结构中，N-供体物种上甲基或吡啶基环的位置（或数量）都会影响局部结构和整体结构中1-7的结构变化，从而导致结构范围很广，从单链开始，双链或二维纸。使用BPY，4-MeBPY和5-MeBPY在2-4的链结构中观察到N-供体配体与铀酰中心的直接配位，而N-供体以客体的形式参与（作为中性或电荷平衡物质）分别使用6-MeBPY，4,6-MeBPY和TPPZ形成5-7的链状结构和片状结构。化合物1是唯一不包含任何N-供体配体的结构，因此结晶为2-D互穿片。 1-7的发光特性受N-供体物种与铀酰中心的直接配位或不配位影响。在N供体直接配位时，化合物2-4表现出典型的UO22 +发射，但是当N供体物种作为客体分子参与时，在1、5、6和7中观察到不存在。这些结果表明，N-供体配体的直接配位作为生色团参与，从而导致可能的UO22 +致敏。 1、5、6和7中缺少发射，可以通过TDC配体在其结构内的扩展共轭来解释。

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