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Opportunities and challenges of applying advanced X-ray spectroscopy to actinide and lanthanide N-donor ligand systems.

ABSTRACT: N-donor ligands such as n-Pr-BTP [2,6-bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine] preferentially bind trivalent actinides (An3+) over trivalent lanthanides (Ln3+) in liquid-liquid separation. However, the chemical and physical processes responsible for this selectivity are not yet well understood. Here, an explorative comparative X-ray spectroscopy and computational (L3-edge) study for the An/Ln L3-edge and the N K-edge of [An/Ln(n-Pr-BTP)3](NO3)3, [Ln(n-Pr-BTP)3](CF3SO3)3 and [Ln(n-Pr-BTP)3](ClO4)3 complexes is presented. High-resolution X-ray absorption near-edge structure (HR-XANES) L3-edge data reveal additional features in the pre- and post-edge range of the spectra that are investigated using the quantum chemical codes FEFF and FDMNES. X-ray Raman spectroscopy studies demonstrate the applicability of this novel technique for investigations of liquid samples of partitioning systems at the N K-edge.

SUBMITTER: Pruessmann T 

PROVIDER: S-EPMC8733980 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Opportunities and challenges of applying advanced X-ray spectroscopy to actinide and lanthanide N-donor ligand systems.

Pruessmann Tim T   Nagel Peter P   Simonelli Laura L   Batchelor David D   Gordon Robert R   Schimmelpfennig Bernd B   Trumm Michael M   Vitova Tonya T  

Journal of synchrotron radiation 20220101 Pt 1

N-donor ligands such as n-Pr-BTP [2,6-bis(5,6-dipropyl-1,2,4-triazin-3-yl)pyridine] preferentially bind trivalent actinides (An<sup>3+</sup>) over trivalent lanthanides (Ln<sup>3+</sup>) in liquid-liquid separation. However, the chemical and physical processes responsible for this selectivity are not yet well understood. Here, an explorative comparative X-ray spectroscopy and computational (L<sub>3</sub>-edge) study for the An/Ln L<sub>3</sub>-edge and the N K-edge of [An/Ln(n-Pr-BTP)<sub>3</sub  ...[more]

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