Spectroscopic investigation of the different complexation and extraction properties of diastereomeric diglycolamide ligands

Weßling, Patrik; Trumm, Michael; Sittel, Thomas; Geist, Andreas; Panak, Petra J.

doi:10.1515/ract-2021-1134

Cited by 8 publications

(8 citation statements)

References 25 publications

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“…These emission bands correspond to [Cm(TEDGA)] 3+ , [Cm(TEDGA) 2 ] 3+ , and Cm(TEDGA) 3 ] 3+ . The distinctive characteristics of these narrow emission bands and their maxima are consistent with those found in diglycolamide complexes in the existing literature [3a,6b,10] . The measured emission spectrum represents a superposition of individual Cm(III) species.…”

Section: Resultssupporting

confidence: 88%

Spectroscopic Study on the Complexation of trivalent Actinide and Lanthanide ions with TEDGA in Solution

Sittel,

Meißner,

Keller

et al. 2024

Eur J Inorg Chem

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NMR spectroscopy studies on the complexation of La(III), Sm(III), Lu(III), Y(III) and Am(III) with N,N,N’,N’‐tetraethyldiglycolamide (TEDGA) have been performed. Initial studies concerning the stoichiometry of the complexes prove the formation of [M(TEDGA)3]3+ in D2O and [M(TEDGA)1‐3]3+ in CD3CN. Decreasing the solvent polarity translates to an increase of the complex stability as shown by complementary TRLFS studies with Cm(III). Due to delocalization of the lone electron pair of the amide nitrogen atom, the M(III)‐O interaction has been studied indirectly by collecting 13C and 15N NMR data. The observed chemical shifts prove that the interaction of the trivalent ions, An(III) and Ln(III), and TEDGA is almost identical.

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Section: Resultssupporting

confidence: 88%

Spectroscopic Study on the Complexation of trivalent Actinide and Lanthanide ions with TEDGA in Solution

Sittel,

Meißner,

Keller

et al. 2024

Eur J Inorg Chem

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“…This was added to the evaporation residue of the 243 Am(OTf) 3 solution containing 1 mg of 243 Am(III). The solution was then transferred into a J. Young-type NMR tube. − …”

Section: Methodsmentioning

confidence: 99%

2,6-Bis(5-(tert-butyl)-1H-pyrazol-3-yl)pyridine: Effects of the Peripheral Aliphatic Side Chain on the Coordination of Actinides(III) and Lanthanides(III)

Stracke,

Weßling,

Sittel

et al. 2024

Inorg. Chem.

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To improve our understanding of the interaction mechanism in trivalent lanthanide and actinide complexes, studies with structurally different hard and soft donor ligands are of great interest. For that reason, the coordination chemistry of An(III) and Ln(III) with 2,6bis(5-(tert-butyl)-1H-pyrazol-3-yl)pyridine (C4-BPP) has been explored. Time-resolved laser fluorescence spectroscopy (TRLFS) studies have revealed the formation of [Cm(C4-BPP) n ] 3+ (n = 1−3) (log β 1 ′ = 7.2 ± 0.4, log β 2 ′ = 10.1 ± 0.5, and log β 3 ′ = 11.8 ± 0.6) and [Eu(C4-BPP) m ] 3+ (m = 1−2) (log β 1 ′ = 4.9 ± 0.2 and log β 2 ′ = 8.0 ± 0.4). The absence of the [Eu(C4-BPP) 3 ] 3+ complex shows a more favorable complexation of Cm(III) over that of Eu(III). Additionally, complementary NMR measurements have been conducted to examine the M(III)−N bond in Ln(III) and Am(III) C4-BPP complexes. 15 N NMR data have revealed notable differences in the chemical shifts of the coordinating nitrogen atoms between the Am(III) and Ln(III) complexes. In the Am(III) complex, the coordinating nitrogen atoms have shown a shift by 260 ppm, indicating a higher fraction of covalent bonding in the Am(III)−N bond compared with the Ln(III)−N bond. This observation aligns excellently with the differences in the stability constants obtained from TRLFS studies.

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“…Short explanations were only given at the molecular scale. Finally, a major step forward was done with the works of Wilden and Weßling who showed that diastereoisomerism of some chiral diglycolamide (DGA) derivatives (Figure 13C) could significantly affect the organization of the ligand and its interaction with other partners than the metal cation (lanthanide or actinide), on the inner-and the outer-sphere of coordination [122,123].…”

Section: A Foreword About Significance Of the Stereoisomerism In The ...mentioning

confidence: 99%

Solvent extraction of uranium from an acidic medium for the front-end of nuclear fuel cycle: from mechanisms understanding to innovative process design

Giusti,

Guerinoni,

Lemire

et al. 2024

Comptes Rendus. Chimie

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Despite the fact that methods for uranium extraction from an acidic medium (sulfuric, phosphoric or nitric) are relatively robust processes, the search for more efficient systems in terms of extraction efficiency and selectivity with respect to competitor ions remains relevant. To address this challenge, researchers have developed a wide range of new extracting molecular agents that allow efficient and selective liquid-liquid extraction of the target metal. After delivering a synoptic reminder of the former hydrometallurgical processes on which dogmas have been based, we present an exhaustive report of the structures that have been designed, synthesized and evaluated as useful hydrometallurgical tools for the extraction of uranium focused on the front-end of the nuclear fuel cycle. Moreover, peculiar emphasis has been given to theoretical aspects related to parameters, such as amphiphilic properties, which influence the extraction mechanism involved in each system, be it mono-or multifunctional ligand. Concluding remarks were afforded as consistent milestones of a prospective and promising route for the next hydrometallurgy including the influence of the stereochemistry.

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Spectroscopic investigation of the different complexation and extraction properties of diastereomeric diglycolamide ligands

Cited by 8 publications

References 25 publications

Spectroscopic Study on the Complexation of trivalent Actinide and Lanthanide ions with TEDGA in Solution

Spectroscopic Study on the Complexation of trivalent Actinide and Lanthanide ions with TEDGA in Solution

2,6-Bis(5-(tert-butyl)-1H-pyrazol-3-yl)pyridine: Effects of the Peripheral Aliphatic Side Chain on the Coordination of Actinides(III) and Lanthanides(III)

Solvent extraction of uranium from an acidic medium for the front-end of nuclear fuel cycle: from mechanisms understanding to innovative process design

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