Design and Crystallization of Water-Stable Uranyl Phosphonates Using a Metalloligand Strategy

IF 3.2 2区化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Crystal Growth & Design Pub Date : 2024-10-06 DOI:10.1021/acs.cgd.4c0093510.1021/acs.cgd.4c00935

Sheng-Bo Liu, Song-Song Bao* and Li-Min Zheng*,

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Abstract

The uranyl ion can form strong metal–ligand bonds with phosphonate groups, making it an excellent choice for constructing water-stable MOFs. However, reactions of uranyl ion and phosphonate ligands often occur too quickly, resulting in powders rather than single crystals. In this work, we employed a metalloligand strategy and synthesized four coordination polymers with layered structures, (UO₂)Fe(notpH)·0.5H₂O (1), (UO₂)Fe₂(notpH₂)₂·0.75H₂O (2), (UO₂)Co(notpH)(H₂O)·5H₂O (3), and (UO₂)₂Co₂(notpH)₂(H₂O)₂·7H₂O (4), by reacting metalloligands M^III(notpH₃) [M = Co, Fe; notpH₆ = 1,4,7-triazacyclononane-1,4,7-triyl-tris(methylenephosphonic acid)] with UO₂(OAc)₂ under hydrothermal conditions. By optimizing the synthesis conditions, we obtained pure phases of compounds 1, 3, and 4 and studied their stability in water. Compounds 1 and 3 were stable even in boiling water, whereas compound 4 converted to 3 after 2 days in boiling water. We also investigated the proton conductive properties of compounds 1 and 3.

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利用金属配体策略设计水稳定的铀基膦酸盐并使其结晶

铀酰离子能与膦酸盐基团形成牢固的金属配体键，因此是构建水稳定 MOF 的绝佳选择。然而，铀酰离子与膦酸配体的反应往往发生得太快，导致生成的是粉末而非单晶。在这项工作中，我们采用了金属配体策略，合成了四种具有层状结构的配位聚合物：(UO2)Fe(notpH)-0.5H2O (1)、(UO2)Fe2(notpH2)2-0.75H2O (2)、(UO2)Co(notpH)(H2O)-5H2O (3)和(UO2)2Co2(notpH)2(H2O)2-7H2O (4)；notpH6 = 1,4,7-三氮杂环壬烷-1,4,7-三基-三（亚甲基膦酸）]与 UO2(OAc)2 在水热条件下反应。通过优化合成条件，我们获得了化合物 1、3 和 4 的纯相，并研究了它们在水中的稳定性。化合物 1 和 3 即使在沸水中也很稳定，而化合物 4 在沸水中 2 天后就转化为 3。我们还研究了化合物 1 和 3 的质子传导特性。

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来源期刊

Crystal Growth & Design 化学-材料科学：综合

CiteScore

6.30

自引率

10.50%

发文量

650

审稿时长

1.9 months

期刊介绍： The aim of Crystal Growth & Design is to stimulate crossfertilization of knowledge among scientists and engineers working in the fields of crystal growth, crystal engineering, and the industrial application of crystalline materials. Crystal Growth & Design publishes theoretical and experimental studies of the physical, chemical, and biological phenomena and processes related to the design, growth, and application of crystalline materials. Synergistic approaches originating from different disciplines and technologies and integrating the fields of crystal growth, crystal engineering, intermolecular interactions, and industrial application are encouraged.