Siderophore-inspired chelator hijacks uranium from aqueous medium

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

doi:10.1038/s41467-019-08758-1

Title: Siderophore-inspired chelator hijacks uranium from aqueous medium

Journal Article · Mon Feb 18 00:00:00 EST 2019 · Nature Communications

DOI:https://doi.org/10.1038/s41467-019-08758-1· OSTI ID:1495975

^[1];

^[2]; Zhang, Zhicheng ^[3];

^[4]; Sun, Qi ^[4];

^[4]; Jansone-Popova, Santa ^[1]; Arnold, John ^[2]; Mayes, Richard T. ^[1];

^[1];

^[1]; Rao, Linfeng ^[3];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of South Florida, Tampa, FL (United States)

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 pK_a 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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC05-00OR22725; AC02-05CH11231; NE0008281

OSTI ID:: 1495975

Alternate ID(s):: OSTI ID: 1559186

Journal Information:: Nature Communications, Vol. 10, Issue 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 64 works

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