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Siderophore-inspired chelator hijacks uranium from aqueous medium.

  • Author(s): Ivanov, Alexander S;
  • Parker, Bernard F;
  • Zhang, Zhicheng;
  • Aguila, Briana;
  • Sun, Qi;
  • Ma, Shengqian;
  • Jansone-Popova, Santa;
  • Arnold, John;
  • Mayes, Richard T;
  • Dai, Sheng;
  • Bryantsev, Vyacheslav S;
  • Rao, Linfeng;
  • Popovs, Ilja
  • et al.
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.

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