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De novo synthesis of bifunctional conjugated microporous polymers for synergistic coordination mediated uranium entrapment

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Abstract

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.

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Acknowledgements

The study was financially supported by the National Natural Science Foundation of China (Nos. 21922604 and 51673109) and Innovative Research Team in University (No. IRT13026). Partial support from the U.S. National Science Foundation (No. CBET-1706025) and the Robert A. Welch Foundation (No. B-0027) is also acknowledged (S. Q. M.).

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Author notes

  1. Shengqian Ma

    Present address: Present address: Department of Chemistry, University of North Texas, 1508 W. Mulberry St, Denton, TX, 76201, USA

  2. Boxuan Yu and Lei Zhang contributed equally to this work.

Authors and Affiliations

  1. Collaborative Innovation Center of Advanced Nuclear Energy Technology, Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing, 100084, China

    Boxuan Yu, Lei Zhang, Gang Ye, Jing Chen & Shengming Xu

  2. Beijing Institute of Graphene Technology, Beijing, 100094, China

    Boxuan Yu, Jiongli Li & Xudong Wang

  3. Beijing Institute of Aeronautical Materials, Beijing, 100085, China

    Boxuan Yu, Jiongli Li & Xudong Wang

  4. Department of Chemistry, University of South Florida, 4202 E. Fowler Avenue, Tampa, FL, 33620, USA

    Lei Zhang, Qingzhi Liu & Shengqian Ma

  5. Beijing Key Lab of Radioactive Waste Treatment, Tsinghua University, Beijing, 100084, China

    Gang Ye, Jing Chen & Shengming Xu

  6. College of Chemistry and Pharmaceutical Sciences, Qingdao Agricultural University, Qingdao, 266109, China

    Qingzhi Liu

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  1. Boxuan Yu
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De novo synthesis of bifunctional conjugated microporous polymers for synergistic coordination mediated uranium entrapment

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Yu, B., Zhang, L., Ye, G. et al. De novo synthesis of bifunctional conjugated microporous polymers for synergistic coordination mediated uranium entrapment. Nano Res. 14, 788–796 (2021). https://doi.org/10.1007/s12274-020-3217-7

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