TY - JOUR
T1 - Siderophore-inspired chelator hijacks uranium from aqueous medium
AU - Ivanov, Alexander S.
AU - Parker, Bernard F.
AU - Zhang, Zhicheng
AU - Aguila, Briana
AU - Sun, Qi
AU - Ma, Shengqian
AU - Jansone-Popova, Santa
AU - Arnold, John
AU - Mayes, Richard T.
AU - Dai, Sheng
AU - Bryantsev, Vyacheslav S.
AU - Rao, Linfeng
AU - Popovs, Ilja
N1 - Publisher Copyright:
© 2019, The Author(s).
PY - 2019/12/1
Y1 - 2019/12/1
N2 - 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 (UO 2 2+ ) recognition motifs possessing siderophore-like selectivity, however, presents a challenge. Herein we report a comprehensive theoretical, crystallographic and spectroscopic studies on the UO 2 2+ binding with a non-toxic siderophore-inspired chelator, 2,6-bis[hydroxy(methyl)amino]-4-morpholino-1,3,5-triazine (H 2 BHT). The optimal pK a values and structural preorganization endow H 2 BHT 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 H 2 BHT-functionalized polymeric adsorbent material that affords high uranium uptake capacity even in the presence of competing vanadium (V) ions in aqueous medium.
AB - 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 (UO 2 2+ ) recognition motifs possessing siderophore-like selectivity, however, presents a challenge. Herein we report a comprehensive theoretical, crystallographic and spectroscopic studies on the UO 2 2+ binding with a non-toxic siderophore-inspired chelator, 2,6-bis[hydroxy(methyl)amino]-4-morpholino-1,3,5-triazine (H 2 BHT). The optimal pK a values and structural preorganization endow H 2 BHT 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 H 2 BHT-functionalized polymeric adsorbent material that affords high uranium uptake capacity even in the presence of competing vanadium (V) ions in aqueous medium.
UR - http://www.scopus.com/inward/record.url?scp=85061723065&partnerID=8YFLogxK
U2 - 10.1038/s41467-019-08758-1
DO - 10.1038/s41467-019-08758-1
M3 - Article
C2 - 30778071
AN - SCOPUS:85061723065
SN - 2041-1723
VL - 10
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 819
ER -