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Exploring the Subtle Effect of Aliphatic Ring Size on Minor Actinide-Extraction Properties and Metal Ion Speciation in Bis-1,2,4-Triazine Ligands

Zaytsev, A. V.; Bulmer, R.; Kozhevnikov, V. N.; Sims, M.; Modolo, G.; Wilden, A.; Waddell, P. G.; Geist, A. ORCID iD icon 1; Panak, P. J. 1; Weßling, P. 1; Lewis, F. W.
1 Institut für Nukleare Entsorgung (INE), Karlsruher Institut für Technologie (KIT)

Abstract:

Calling all actinides! Bis-1,2,4-triazine ligands bearing five-membered rings were synthesized and evaluated as actinide-selective extractants. Tuning the size of the aliphatic ring leads to subtle changes in actinide-extraction properties. The origins of these changes were elucidated at the molecular level, paving the way for the rational design of improved actinide-selective extractants for reprocessing of spent nuclear fuel.,

The synthesis and evaluation of three novel bis-1,2,4-triazine ligands containing five-membered aliphatic rings are reported. Compared to the more hydrophobic ligands 1–3 containing six-membered aliphatic rings, the distribution ratios for relevant f-block metal ions were approximately one order of magnitude lower in each case. Ligand 10 showed an efficient, selective and rapid separation of AmIII and CmIII from nitric acid. The speciation of the ligands with trivalent f-block metal ions was probed using NMR titrations and competition experiments, time-resolved laser fluorescence spectroscopy and X-ray crystallography. While the tetradentate ligands 8 and 10 formed Ln$^{III}$ complexes of the same stoichiometry as their more hydrophobic analogues 2 and 3, significant differences in speciation were observed between the two classes of ligand, with a lower percentage of the extracted 1:2 complexes being formed for ligands 8 and 10. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000100228
Veröffentlicht am 28.11.2021
Originalveröffentlichung
DOI: 10.1002/chem.201903685
Scopus
Zitationen: 19
Web of Science
Zitationen: 18
Dimensions
Zitationen: 17
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nukleare Entsorgung (INE)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2020
Sprache Englisch
Identifikator ISSN: 0947-6539, 1521-3765
KITopen-ID: 1000100228
HGF-Programm 32.01.11 (POF III, LK 01) Extraktions- und Koordinationschemie der Actiniden
Erschienen in Chemistry - a European journal
Verlag John Wiley and Sons
Band 26
Heft 2
Seiten 428-437
Vorab online veröffentlicht am 05.09.2019
Nachgewiesen in Scopus
Web of Science
Dimensions
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