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Employing metal-organic cage for selective capture of UO22+ and Sr2+

利用金属-有机笼子选择性吸附铀酰和二价锶离子

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Abstract

Selective capture of UO22+ and Sr2+ ions represents a key component in the nuclear fuel reprocessing, nuclear accident prevention, and environmental protection. We report herein a proof of concept, employing metal-organic cage (MOC) for the selective capture of UO22+ or Sr2+ ions, through using a C3-symmetrical multiple-carboxylate ligand (H3L) to fix uranyl ions together. By means of such MOC approach, we can facilitate the extraction of uranyl ions from a multiple metallic mixed solution by using the H3L ligands as an extractant, showing an ultrahigh extraction efficiency of 97% and UO22+ selectivity of 19.4–97, suggesting its superior application in the UO22+ capture. The mechanism for such outstanding performance is due to the formation of a polyoxouranyl-based MOC. Moreover, this MOC compound can be also used as a solid adsorbent to selectively capture Sr2+ ions through a unique mechanism with the formation of a SrO4N2 octahedral coordination.

摘要

铀酰与二价锶离子的选择性捕获是核燃料后处理、核事故预防和环境保护的关键组成部分. 我们在此报道了一个概念验证, 通过使用C3对称的多羧酸配体(H3L)将铀酰离子固定在一起, 使用金属有机笼(MOC)选择性捕获铀酰与二价锶离子. 通过这种金属有机笼方法, 我们可以通过使用H3L配体作为萃取剂, 从多种金属混合溶液中高效提取铀酰离子, 萃取效率高达97%, 且铀酰选择性高达19.4–97, 展示了MOC在铀酰捕获中的应用. 此外, MOC也可用作固相吸附剂, 并通过形成一种SrO4N2 八面体来选择性捕获二价锶离子.

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References

  1. Veliscek-Carolan J. Separation of actinides from spent nuclear fuel: A review. J Hazard Mater, 2016, 318: 266–281

    Article  CAS  Google Scholar 

  2. Mathur JN, Murali MS, Nash KL. Actinide partitioning—A review. Solvent Extraction Ion Exchange, 2001, 19: 357–390

    Article  CAS  Google Scholar 

  3. Li J, Wang X, Zhao G, et al. Metal-organic framework-based materials: Superior adsorbents for the capture of toxic and radioactive metal ions. Chem Soc Rev, 2018, 47: 2322–2356

    Article  CAS  Google Scholar 

  4. Martell EA. Atmospheric aspects of strontium-90 fallout. Science, 1959, 129: 1197–1206

    Article  CAS  Google Scholar 

  5. Burns PC, Ewing RC, Navrotsky A. Nuclear fuel in a reactor accident. Science, 2012, 335: 1184–1188

    Article  CAS  Google Scholar 

  6. Slovic P, Flynn JH, Layman M. Perceived risk, trust, and the politics of nuclear waste. Science, 1991, 254: 1603–1607

    Article  CAS  Google Scholar 

  7. Zhang J, Chen L, Dai X, et al. Distinctive two-step intercalation of Sr2+ into a coordination polymer with record high 90Sr uptake capabilities. Chem, 2019, 5: 977–994

    Article  CAS  Google Scholar 

  8. Abney CW, Mayes RT, Saito T, et al. Materials for the recovery of uranium from seawater. Chem Rev, 2017, 117: 13935–14013

    Article  CAS  Google Scholar 

  9. Sun X, Luo H, Dai S. Ionic liquids-based extraction: A promising strategy for the advanced nuclear fuel cycle. Chem Rev, 2012, 112: 2100–2128

    Article  CAS  Google Scholar 

  10. Wang Z, Ma R, Meng Q, et al. Constructing uranyl-specific nanofluidic channels for unipolar ionic transport to realize ultrafast uranium extraction. J Am Chem Soc, 2021, 143: 14523–14529

    Article  CAS  Google Scholar 

  11. Cheng L, Liang C, Liu W, et al. Three-dimensional polycatenation of a uranium-based metal-organic cage: Structural complexity and radiation detection. J Am Chem Soc, 2020, 142: 16218–16222

    Article  CAS  Google Scholar 

  12. Zheng T, Yang Z, Gui D, et al. Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system. Nat Commun, 2017, 8: 15369

    Article  CAS  Google Scholar 

  13. Song Y, Zhu C, Sun Q, et al. Nanospace decoration with uranyl-specific “hooks” for selective uranium extraction from seawater with ultrahigh enrichment index. ACS Cent Sci, 2021, 7: 1650–1656

    Article  CAS  Google Scholar 

  14. Zhang M, Liang C, Cheng GD, et al. Intrinsic semiconducting behavior in a large mixed-valent uranium(V/VI) cluster. Angew Chem Int Ed, 2021, 60: 9886–9890

    Article  CAS  Google Scholar 

  15. Zhang H, Liu W, Li A, et al. Three mechanisms in one material: Uranium capture by a polyoxometalate-organic framework through combined complexation, chemical reduction, and photocatalytic reduction. Angew Chem Int Ed, 2019, 58: 16110–16114

    Article  CAS  Google Scholar 

  16. Sather AC, Berryman OB, Rebek Jr. J. Selective recognition and extraction of the uranyl ion. J Am Chem Soc, 2010, 132: 13572–13574

    Article  CAS  Google Scholar 

  17. Pasquale S, Sattin S, Escudero-Adán EC, et al. Giant regular polyhedra from calixarene carboxylates and uranyl. Nat Commun, 2012, 3: 785

    Article  Google Scholar 

  18. Mei L, Ren P, Wu Q, et al. Actinide separation inspired by self-assembled metal-polyphenolic nanocages. J Am Chem Soc, 2020, 142: 16538–16545

    Article  CAS  Google Scholar 

  19. Wang LJ, Bai S, Han YF. Water-soluble self-assembled cage with tri-angular metal-metal-bonded units enabling the sequential selective separation of alkanes and isomeric molecules. J Am Chem Soc, 2022, 144: 16191–16198

    Article  CAS  Google Scholar 

  20. Wang LJ, Li X, Bai S, et al. Self-assembly, structural transformation, and guest-binding properties of supramolecular assemblies with triangular metal–metal bonded units. J Am Chem Soc, 2020, 142: 2524–2531

    Article  CAS  Google Scholar 

  21. Hosono N, Kitagawa S. Modular design of porous soft materials via self-organization of metal-organic cages. Acc Chem Res, 2018, 51: 2437–2446

    Article  CAS  Google Scholar 

  22. Fujita M, Oguro D, Miyazawa M, et al. Self-assembly of ten molecules into nanometre-sized organic host frameworks. Nature, 1995, 378: 469–471

    Article  CAS  Google Scholar 

  23. Percástegui EG, Ronson TK, Nitschke JR. Design and applications of water-soluble coordination cages. Chem Rev, 2020, 120: 13480–13544

    Article  Google Scholar 

  24. Zhang X, Dong X, Lu W, et al. Fine-tuning apertures of metal-organic cages: Encapsulation of carbon dioxide in solution and solid state. J Am Chem Soc, 2019, 141: 11621–11627

    Article  CAS  Google Scholar 

  25. Niu Z, Fang S, Liu X, et al. Coordination-driven polymerization of supramolecular nanocages. J Am Chem Soc, 2015, 137: 14873–14876

    Article  CAS  Google Scholar 

  26. Liu J, Duan W, Song J, et al. Self-healing hyper-cross-linked metal-organic polyhedra (HCMOPs) membranes with antimicrobial activity and highly selective separation properties. J Am Chem Soc, 2019, 141: 12064–12070

    Article  CAS  Google Scholar 

  27. Yin M, Krishna R, Wang W, et al. A [Th8Co8] nanocage-based metalorganic framework with extremely narrow window but flexible nature enabling dual-sieving effect for both isotope and isomer separation. CCS Chem, 2022, 4: 1016–1027

    Article  CAS  Google Scholar 

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Acknowledgements

This work was supported by the Training Program for Academic and Technical Leaders of Major Disciplines in Jiangxi Province (20194BCJ22010), the National Natural Science Foundations of China (21966002), the Youth Leading Talent Project of Fuzhou (2020ED64), and Jiangxi Project (DHSQT22021007). The authors also thank Wenqian Liu from Shiyanjia Lab (www.Shiyanjia.com) for the XRD analysis.

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Authors and Affiliations

  1. School of Chemistry, Biology and Materials Science, East China University of Technology, Nanchang, 330013, China

    Liecheng Guo  (郭裂成), Huiping Zhang  (张辉平) & Feng Luo  (罗峰)

  2. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing, 100029, China

    Yongming Xia  (夏永明), Lele Gong  (龚乐乐) & Lipeng Zhang  (张利鹏)

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  1. Liecheng Guo  (郭裂成)
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  6. Feng Luo  (罗峰)
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Contributions

Guo L and Zhang H conducted the experiment; Xia Y, Gong L, and Zhang L carried out the computational calculation; Luo F designed this study, analyzed the data and wrote the paper. All authors contributed to the general discussion.

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Correspondence to Feng Luo  (罗峰).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

Experimental details and supporting data are available in the online version of the paper.

Liecheng Guo received his Bachelor degree from the East China University of Technology (ECUT) in 2018, and is now a graduate student at the ECUT. His research interest focuses on the synthesis and function of metal-organic frameworks (MOFs), covalent organic frameworks (COFs), and metal-organic cages (MOCs).

Huiping Zhang received his Master degree from the ECUT in 2022. He is now a PhD candidate at Jinan University. His research interest focuses on the synthesis, properties, and application of MOFs and MOCs.

Yongming Xia received his Bachelor degree from Changsha University of Science and Technology in 2019. He is now a graduate student at Beijing University of Chemical Technology. His research interests focus on the theoretical calculation of electronic adsorption structures.

Feng Luo received his PhD degree from Nankai University in 2009, and then joined the faculty of the School of Biology, Chemistry and Material Science, ECUT in 2009, and got the full professorship in 2016. His current research interests include the molecular design and properties of MOFs, COFs, and MOCs.

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Guo, L., Zhang, H., Xia, Y. et al. Employing metal-organic cage for selective capture of UO22+ and Sr2+. Sci. China Mater. 66, 3285–3291 (2023). https://doi.org/10.1007/s40843-023-2454-4

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  • DOI: https://doi.org/10.1007/s40843-023-2454-4

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