Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides

Pilgrim, Corey D.; Grimes, Travis S.; Smith, Clayn; Heathman, Colt R.; Mathew, Jopaul; Jansone-Popova, Santa; Roy, Santanu; Ray, Debmalya; Bryantsev, Vyacheslav S.; Zalupski, Peter R.

doi:10.1038/s41598-023-44106-6

Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides

Journal Article · Thu Oct 19 00:00:00 EDT 2023 · Scientific Reports

DOI:https://doi.org/10.1038/s41598-023-44106-6· OSTI ID:2290359

^[1]; ^[1]; Smith, Clayn ^[1]; ^[1]; ^[2]; ^[2]; ^[2]; ^[2]; ^[2]; ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

The complexation of trivalent lanthanides and minor actinides (Am³⁺, Cm³⁺, and Cf³⁺) by the acyclic aminopolycarboxylate chelators 6,6'-((ethane-1,2-diylbis–((carboxymethyl)azanediyl))bis–(methylene))dipicolinic acid (H₄octapa) and 6,6'-((((4-(1-(2-(2-(2-hydroxyethoxy)ethoxy)ethyl)-1H-1,2,3-triazol-4-yl)pyridine-2,6-diyl)bis–(methylene))bis–((carboxymethyl)azanediyl))bis–(methylene)) dipicolinic acid (H₄pypa-peg) were studied using potentiometry, spectroscopy, competitive complexation liquid–liquid extraction, and ab initio molecular dynamics simulations. Two studied reagents are strong multidentate chelators, well-suited for applications seeking radiometal coordination for in-vivo delivery and f-element isolation. The previously reported H₄octapa forms a compact coordination packet, while H₄pypa-peg is less sterically constrained due to the presence of central pyridine ring. The solubility of H₄octapa is limited in a non-complexing high ionic strength perchlorate media. However, the introduction of a polyethylene glycol group in H₄pypa-peg increased the solubility without influencing its ability to complex the lanthanides and minor actinides in solution.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Compute and Data Environment for Science (CADES)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; AC07-05ID14517

OSTI ID:: 2290359

Alternate ID(s):: OSTI ID: 2376299

Report Number(s):: INL/JOU--23-72426-Rev000

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 13; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides

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