Advances in heavy alkaline earth chemistry provide insight into complexation of weakly polarizing Ra2+, Ba2+, and Sr2+ cations

被引:3
作者
Gilhula, J. Connor [1 ]
Xu, Lei [1 ]
White, Frankie D. [1 ]
Adelman, Sara L. [1 ]
Aldrich, Kelly E. [1 ]
Batista, Enrique R. [1 ]
Dan, David [1 ]
Jones, Zachary R. [1 ]
Kozimor, Stosh A. [1 ]
Mason, Harris E. [1 ]
Meyer, Rachel L. [1 ,2 ]
Thiele, Nikki A. [3 ]
Yang, Ping [1 ]
Yuan, Mingbin [1 ]
机构
[1] Los Alamos Natl Lab, Los Alamos, NM 87545 USA
[2] Univ Rochester, Dept Chem Engn, Rochester, NY 14627 USA
[3] Oak Ridge Natl Lab, Chem Sci Div, Oak Ridge, TN 37831 USA
关键词
METAL-COMPLEXES; CATALYSTS; ISOTOPES; ELEMENTS; EXCHANGE; ETHERS; ENERGY; RADIUM; AMINES; IMPACT;
D O I
10.1126/sciadv.adj8765
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Numerous technologies-with catalytic, therapeutic, and diagnostic applications-would benefit from improved chelation strategies for heavy alkaline earth elements: Ra2+, Ba2+, and Sr2+. Unfortunately, chelating these metals is challenging because of their large size and weak polarizing power. We found 18-crown-6-tetracarboxylic acid (H4COCO) bound Ra2+, Ba2+, and Sr2+ to form M(HxCOCO)(x-2). Upon isolating radioactive Ra-223 from its parent radionuclides (Ac-227 and Th-227), Ra-223(2+) reacted with the fully deprotonated COCO4- chelator to generate Ra(COCO)(2-)((aq)) (log KRa(COCO)2- = 5.97 +/- 0.01), a rare example of a molecular radium complex. Comparative analyses with Sr2+ and Ba2+ congeners informed on what attributes engendered success in heavy alkaline earth complexation. Chelators with high negative charge [-4 for Ra(COCO)(2-)((aq))] and many donor atoms [>= 11 in Ra(COCO)(2-)((aq))] provided a framework for stable complex formation. These conditions achieved steric saturation and overcame the weak polarization powers associated with these large dicationic metals.
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页数:14
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