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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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Abstract

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 the 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 diethylenetriamine pentaacetic acid (DTPA), the modified DTTA-BuA complexant features higher ligand acidity and the important An3+/Ln3+ differentiation when deployed on a liquid–liquid distribution platform.

Graphical abstract: 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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Publication details

The article was received on 31 Oct 2017, accepted on 14 Dec 2017 and first published on 14 Dec 2017


Article type: Paper
DOI: 10.1039/C7DT04104G
Citation: Dalton Trans., 2018, Advance Article
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    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

    C. R. Heathman, T. S. Grimes, S. Jansone-Popova, A. S. Ivanov, V. S. Bryantsev and P. R. Zalupski, Dalton Trans., 2018, Advance Article , DOI: 10.1039/C7DT04104G

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