New Three-Fold Interpenetrated Uranyl Organic Framework Constructed by Terephthalic Acid and Imidazole Derivative

A new
3-fold interpenetrated uranyl organic framework, UO2(bdc)­(dmpi),
was hydrothermally synthesized using 1,4-benzenedicarboxylic acid
(H2bdc) and 1-(4-(1H-imidazol-1-yl)-2,5-dimethylphenyl)-1H-imidazole (dmpi). This framework, which was determined
by synchrotron radiation X-ray, exhibited a new 3-fold interpenetrated
(2,4)-connected topology with the Schläfli symbol of (126)­(12)2. Additionally, large incurvation happened
to the bond angle of [OUO]2+, which was
always arranged in a rigorous line. Computational results based on
density functional theory (DFT) indicated that the bent geometry of
uranyl in UO2(bdc)­(dmpi) was mainly due to the higher charge
populations in the valence 6d shells of uranium, rendered by the electronegative
imidazoles.

一种新型的三重交联铀酰有机框架，UO2(bdc)­(dmpi)，通过使用1,4-苯二甲酸(H2bdc)和1-(4-(1H-咪唑-1-基)-2,5-二甲基苯基)-1H-咪唑(dmpi)进行水热合成。经同步辐射X射线表征，该框架呈现出一种新颖的三重交联(2,4)-连通拓扑结构，其Schläfli符号为(126)­(12)2。此外，[OUO]2+键角发生了显著弯曲，始终保持严格的线性排列。基于密度泛函理论(DFT)的计算结果表明，UO2(bdc)­(dmpi)中铀酰的弯曲几何形状主要归因于铀的价态6d轨道中较高的电荷分布，这是由电子亲和力较高的咪唑类化合物所引起的。