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

Gilhula, James Connor; Xu, Lei; White, Jr., Frankie Don; Adelman, Sara Linnae; Aldrich, Kelly Elise; Batista, Enrique Ricardo; Dan, David; Jones, Zachary Robert; Kozimor, Stosh Anthony; Mason, Harris E.; Meyer, Rachel L.; Thiele, Nikki A.; Yang, Ping; Yuan, Mingbin

doi:10.1126/sciadv.adj8765

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

Journal Article · 05 January 2024 · Science Advances

DOI: https://doi.org/10.1126/sciadv.adj8765 · OSTI ID:2283876

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Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Los Alamos National Laboratory, Los Alamos, NM 87545 (USA).
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Univ. of Rochester, NY (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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(H_xCOCO)^x–2. Upon isolating radioactive ²²³Ra from its parent radionuclides (²²⁷Ac and ²²⁷Th), ²²³Ra²⁺ reacted with the fully deprotonated COCO^4- chelator to generate Ra(COCO)^2-_(aq) (log K_Ra(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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Nuclear Physics (NP); USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC05-00OR22725; 89233218CNA000001

OSTI ID:: 2283876

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 1 Vol. 10; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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

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