Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine-N,N',N",N"-tetraacetic acid

Heathman, Colt R.; Grimes, Travis S.; Jansone-Popova, Santa; Ivanov, Alexander S.; Bryantsev, Vyacheslav S.; Zalupski, Peter R.

doi:10.1039/c7dt04104g

Title: Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine-N,N',N",N"-tetraacetic acid

Journal Article · Thu Dec 14 00:00:00 EST 2017 · Dalton Transactions

DOI:https://doi.org/10.1039/c7dt04104g· OSTI ID:1427624

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Idaho National Lab. (INL), Idaho Falls, ID (United States). Aqueous Separations and Radiochemistry Dept.
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division

The novel metal ion complexant N-butyl-2-acetamide-diethylenetriamine-N,N',N'',N''-tetraacetic acid (DTTA-BuA) uses an amide functionalization to increase the total ligand acidity and attain efficient 4f/5f differentiation in low pH conditions. The amide, when located on the diethylenetriamine platform containing four acetate pendant arms maintains the octadentate coordination sphere for all investigated trivalent f-elements. This compact coordination environment inhibits the protonation of LnL? complexes, as indicated by lower K111 constants relative to the corresponding protonation site of free ligand. For actinide ions, the enhanced stability of AnL? lowers the K111 for americium and curium beyond the aptitude of potentiometric detection. Density functional theory computations indicate the difference in the back-donation ability of Am3+ and Eu3+ f orbitals is mainly responsible for stronger proton affinity of EuL? compared to AmL?. The measured stability constants for the formation of AmL? and CmL? complexes are consistently higher, relative to ML? complexes with lanthanides of similar charge density. When compared with the conventional aminopolycarboxylate DTPA, the modified DTTA-BuA complexant features higher ligand acidity and the important An3+/Ln3+ differentiation when deployed on a liquid-liquid distribution platform.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Idaho National Lab. (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE)

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

OSTI ID:: 1427624

Alternate ID(s):: OSTI ID: 1499585

Report Number(s):: INL/JOU-17-43032-Rev001; ICHBD9

Journal Information:: Dalton Transactions, Vol. 47, Issue 4; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 6 works

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Title: Synthesis and characterization of a novel aminopolycarboxylate complexant for efficient trivalent f-element differentiation: N-butyl-2-acetamide-diethylenetriamine-N,N',N",N"-tetraacetic acid

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