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Cage-Based Metal–Organic Framework Featuring a Double-Yolk Core–Shell U<sub>6</sub>L<sub>3</sub>@U<sub>18</sub>L<sub>14</sub> Structure for Iodine Capture

Shuang Deng, Xiang‐he Kong, Xuan Fu, Zhiwei Huang, Zhiheng Zhou, Lei Mei, Jipan Yu, Li‐Yong Yuan, Yanqiu Zhu, Nannan Wang, Kong‐Qiu Hu, Wei‐Qun Shi

2024Inorganic Chemistry12 citationsDOI

Abstract

Cage-based MOFs, with their customizable chemical environments and precisely controllable nanospaces, show great potential for the selective adsorption of guest molecules with specific structures. In this work, we have constructed a novel cage-based MOF [(CH 3 ) 2 NH 2 ] 2 [(UO 2 ) 2 (TMTTA)]·11.5DMF·2H 2 O (IHEP-51), utilizing a triazine derivative poly(carboxylic acid), 4,4′,4″-(((1,3,5-triazine-2,4,6-triyl)tris(((4-carboxycyclohexyl)methyl)azanediyl))tris(methylene))tribenzoic acid (H 6 TMTTA), as an organic ligand and uranyl as a metal node. The 2-fold interpenetrated (3,6,6)-connected framework of IHEP-51 features two types of supramolecular cage structures: the Pyrgos[2]cage U 6 L 3 and the huge cage U 18 L 14 . They are further assembled into a double-yolk core–shell U 6 L 3 @U 18 L 14 structure, making it suitable for I 2 capture. The maximum adsorption capacities of IHEP-51 for iodine in solution and gaseous iodine are 420.4 and 1561.2 mg·g –1, respectively. XPS, Raman spectra, single-crystal X-ray diffraction, and DFT calculations reveal that the adsorbed iodine is located inside the U 6 L 3 Pyrgos[2]cage in the form of I 3 –, thus resulting in the formation of a (I 3 ) 2 @U 6 L 3 @U 18 L 14 ternary core–shell structure.

Topics & Concepts

ChemistryAdsorptionMetal-organic frameworkMoleculeCrystallographySupramolecular chemistryX-ray photoelectron spectroscopyCrystal structurePhysical chemistryOrganic chemistryChemical engineeringEngineeringMetal-Organic Frameworks: Synthesis and ApplicationsCovalent Organic Framework ApplicationsRadioactive element chemistry and processing