Siderophore-inspired chelator hijacks uranium from aqueous medium

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 Rao () and Ilja Popovs ()
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Alexander S. Ivanov: Oak Ridge National Laboratory
Bernard F. Parker: Lawrence Berkeley National Laboratory
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
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

Nature Communications, 2019, vol. 10, issue 1, 1-7

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-08758-1

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