On the synthesis and characterization of two different titanium-based supramolecular structures of identical stoichiometry

On the synthesis and characterization of two different titanium-based supramolecular structures of identical stoichiometry
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DOI:
10.1080/00958972.2022.2109149
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发表时间:
2022-08
影响因子:
1.9
通讯作者:
Ryan J. Bujol;F. Fronczek;Noémie Elgrishi
Ryan J. Bujol;F. Fronczek;Noémie Elgrishi
中科院分区:
化学4区
文献类型:
--
作者:
Ryan J. Bujol;F. Fronczek;Noémie Elgrishi

文献摘要

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自组装的超分子配位配合物可以具有多种不同金属配位比的三维结构。控制将要采用的体系结构可能很难维护,因为许多体系结构可能从初始材料和现有条件中形成。描述最终形成的体系结构可能具有挑战性,特别是在区分相同化学计量的低阶或高阶结构时。在这里,我们报告了一种Ti2L3足球状或药丸状胶囊的合成和表征,这种胶囊出乎意料地形成于试图合成Ti4L6四面体的变异。两个阴离子核是由相同的化学计量比的有机连接和金属节点形成的。结构的高度对称性和相同的m/z比给表征带来了挑战。结晶是唯一能精确测定其结构的方法。在适当的反离子客体存在的情况下,Ti2L3胶囊在几天的高温下转化为Ti4L6四面体。图形抽象
Abstract Self-assembled supramolecular coordination complexes can take on a wide range of three-dimensional architectures with varying ratios of metal-to-ligand. Control over which architecture will be adopted can be difficult to maintain, as many may form from the starting materials and conditions present. Characterizing the resulting architectures formed can be challenging, in particular when discerning between lower or higher ordered structures of identical stoichiometry. Here we report the synthesis and characterization of a Ti2L3 football-like or pill-shaped capsule, unexpectedly formed from attempts to synthesize variations on a Ti4L6 tetrahedron. The two anionic cores are formed from identical stoichiometric ratios of organic linkers and metal nodes. The high symmetry of the structures, and identical m/z ratios, posed characterization challenges. Crystallization was the only method that allowed for precise structural determination. In the presence of appropriate counter ion guests, the Ti2L3 capsule converts into the Ti4L6 tetrahedron at elevated temperatures over several days. Graphical Abstract