De novo synthesis of bifunctional conjugated microporous polymers for synergistic coordination mediated uranium entrapment
Autor: | Jiongli Li, Jing Chen, Yu Boxuan, Qingzhi Liu, Xudong Wang, Lei Zhang, Shengqian Ma, Gang Ye, Shengming Xu |
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Rok vydání: | 2020 |
Předmět: |
Metal ions in aqueous solution
02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology Condensed Matter Physics Oxime Uranyl 01 natural sciences Combinatorial chemistry Atomic and Molecular Physics and Optics 0104 chemical sciences Conjugated microporous polymer chemistry.chemical_compound Adsorption chemistry Covalent bond General Materials Science Thermal stability Electrical and Electronic Engineering 0210 nano-technology Bifunctional |
Zdroj: | Nano Research. 14:788-796 |
ISSN: | 1998-0000 1998-0124 |
Popis: | This work reports a de novo synthesis of novel bifunctional conjugated microporous polymers (CMPs) exhibiting a synergistic-effect involved coordination behavior to uranium. It is highlighted that the synthetic strategy enables the engineering of the coordination environment within amidoxime functionalized CMP frameworks by specifically introducing ortho-substituted amino functionalities, enhancing the affinity to uranyl ions via forming synergistic complexes. The CMPs exhibit high Brunauer-Emmett-Teller (BET) surface area, well-developed three-dimensional (3D) networks with hierarchical porosity, and favorable chemical and thermal stability because of the covalently cross-linked structure. Compared with the amino-free counterparts, the adsorption capacity of bifunctional CMPs was increased by almost 70%, from 105 to 174 mg/g, indicating evidently enhanced binding ability to uranium. Moreover, new insights into coordination mechanism were obtained by in-depth X-ray photoelectron spectroscopy (XPS) analysis and density functional theory (DFT) calculation, suggesting a dominant role of the oxime ligands forming a 1:1 metal ions/ligands (M/L) coordination model with uranyl ions while demonstrating the synergistic engagement of the amino functionalities via direct binding to uranium center and hydrogen-bonding involved secondary-sphere interaction. This work sheds light on the underlying principles of ortho-substituted functionalities directed synergistic effect to promote the coordination of amidoxime with uranyl ions. And the synthetic strategy established here would enable the task-specific development of more novel CMP-based functional materials for broadened applications. |
Databáze: | OpenAIRE |
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