Varied role of organic carboxylate dizwitterions and anionic donors in mixed-ligand uranyl ion coordination polymers
Varied role of organic carboxylate dizwitterions and anionic donors in mixed-ligand uranyl ion coordination polymers
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有机羧酸盐双性离子和阴离子供体在混合配体铀酰离子配位聚合物中的不同作用
DOI：
10.1039/d2ce01187e
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发表时间：
2022
期刊：
影响因子：
3.1
通讯作者：
Thury Pierre
中科院分区：
文献类型：
--
作者：
Kusumoto Sotaro;Atoini Youssef;Masuda Shunya;Koide Yoshihiro;Kim Jee Young;Hayami Shinya;Kim Yang;Harrowfield Jack;Thury Pierre
二阴离子二羧酸配体1,1′-[（2,3,5,6-四甲基苯-1,4-二基）双（亚甲基）]双（吡啶-1-ium-4-羧酸酯）（pL）和1,1′-[（2,3,5,6-四甲基苯-1,4-二基）双（亚甲基）]双（吡啶-1-ium-3-羧酸酯）（mL）在溶剂水热条件下与铀酰阳离子反应，生成了一系列含有其他阴离子供体的五种配合物。[UO2(pL)(H2PM)(H2O)2]·DMA·H2O(1)，其中H4PM是邻苯二甲酸，DMA是二甲基乙酰胺，[(UO2)2(pL)3(3- sb)2]·8H2O(2)，其中3- sb2−是3-磺酸盐，结晶为单周期配位聚合物，分别为线性或包括双核环，其中pL配体桥接，阴离子只是修饰并参与氢键。pL在[(UO2)2(pL)(2- sb)2]·1.5H2O(3)中连接4个金属阳离子，并与螯合和桥接2-磺酸盐（2- sb2−）配体结合，形成具有kgm拓扑结构的双周期网络。[(UO2)3(mL)(O)2(OH)(H2O)](NO3)0.8Cl0.2·3H2O(4)含有氧和羟基桥接的带状链，由mL连接剂连接形成阳离子双周期网络。相反，在[(UO2)2(mL)3(H2O)2][(UO2)2(TDC)3]2·10H2O(5)中形成了两个独立的2:1比例的聚阴离子和聚阳离子网络，涉及mL或TDC2−（2,5-噻吩二羧酸盐）配体；这两种网络都具有HCB拓扑类型，尽管具有非常不同的细胞形状。
The dizwitterionic dicarboxylate ligands 1,1′-[(2,3,5,6-tetramethylbenzene-1,4-diyl)bis(methylene)]bis(pyridin-1-ium-4-carboxylate) (pL) and 1,1′-[(2,3,5,6-tetramethylbenzene-1,4-diyl)bis(methylene)]bis(pyridin-1-ium-3-carboxylate) (mL) have been reacted with uranyl cations under solvo-hydrothermal conditions to generate a series of five complexes containing also additional anionic donors. [UO2(pL)(H2PM)(H2O)2]·DMA·H2O (1), where H4PM is pyromellitic acid and DMA is dimethylacetamide, and [(UO2)2(pL)3(3-SB)2]·8H2O (2), where 3-SB2− is 3-sulfobenzoate, crystallize as monoperiodic coordination polymers, linear or including dinuclear rings, respectively, in which the pL ligands are bridging and the anionic species are merely decorating and involved in hydrogen bonding. pL connects four metal cations in [(UO2)2(pL)(2-SB)2]·1.5H2O (3) and, associated with the chelating and bridging 2-sulfobenzoate (2-SB2−) ligand, it gives a diperiodic network with the kgm topology. [(UO2)3(mL)(O)2(OH)(H2O)](NO3)0.8Cl0.2·3H2O (4) contains oxo- and hydroxo-bridged ribbon-like chains connected by mL linkers to form a cationic diperiodic network. In contrast, two independent, polyanionic and polycationic networks in a 2 : 1 ratio are formed in [(UO2)2(mL)3(H2O)2][(UO2)2(TDC)3]2·10H2O (5), involving either mL or TDC2− (2,5-thiophenedicarboxylate) ligands; both networks have the hcb topological type, albeit with very different cell shapes.