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Siderophore-inspired chelator hijacks uranium from aqueous medium

Author

Listed:
  • Alexander S. Ivanov

    (Oak Ridge National Laboratory)

  • Bernard F. Parker

    (Lawrence Berkeley National Laboratory
    University of California)

  • Zhicheng Zhang

    (Lawrence Berkeley National Laboratory)

  • Briana Aguila

    (University of South Florida)

  • Qi Sun

    (University of South Florida)

  • Shengqian Ma

    (University of South Florida)

  • Santa Jansone-Popova

    (Oak Ridge National Laboratory)

  • John Arnold

    (Lawrence Berkeley National Laboratory
    University of California)

  • Richard T. Mayes

    (Oak Ridge National Laboratory)

  • Sheng Dai

    (Oak Ridge National Laboratory)

  • Vyacheslav S. Bryantsev

    (Oak Ridge National Laboratory)

  • Linfeng Rao

    (Lawrence Berkeley National Laboratory)

  • Ilja Popovs

    (Oak Ridge National Laboratory)

Abstract

Over millennia, nature has evolved an ability to selectively recognize and sequester specific metal ions by employing a wide variety of supramolecular chelators. Iron-specific molecular carriers—siderophores—are noteworthy for their structural elegance, while exhibiting some of the strongest and most selective binding towards a specific metal ion. Development of simple uranyl (UO22+) recognition motifs possessing siderophore-like selectivity, however, presents a challenge. Herein we report a comprehensive theoretical, crystallographic and spectroscopic studies on the UO22+ binding with a non-toxic siderophore-inspired chelator, 2,6-bis[hydroxy(methyl)amino]-4-morpholino-1,3,5-triazine (H2BHT). The optimal pKa values and structural preorganization endow H2BHT with one of the highest uranyl binding affinity and selectivity among molecular chelators. The results of small-molecule standards are validated by a proof-of-principle development of the H2BHT-functionalized polymeric adsorbent material that affords high uranium uptake capacity even in the presence of competing vanadium (V) ions in aqueous medium.

Suggested Citation

  • Alexander S. Ivanov & Bernard F. Parker & Zhicheng Zhang & Briana Aguila & Qi Sun & Shengqian Ma & Santa Jansone-Popova & John Arnold & Richard T. Mayes & Sheng Dai & Vyacheslav S. Bryantsev & Linfeng, 2019. "Siderophore-inspired chelator hijacks uranium from aqueous medium," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-08758-1
    DOI: 10.1038/s41467-019-08758-1
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