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Stoichiometry of An(III)–DMDOHEMA complexes formed during solvent extraction

Weßling, Patrik 1; Trumm, Michael 1; Geist, Andreas ORCID iD icon 1; Panak, Petra J. 1
1 Institut für Nukleare Entsorgung (INE), Karlsruher Institut für Technologie (KIT)

Abstract (englisch):

N,N’-Dimethyl,N,N’-dioctylhexylethoxymalonamide (DMDOHEMA) is used to separate An(III) and Ln(III)
from fission products in several liquid–liquid extraction processes that aim at recycling actinides. The stoichiometry
of the extracted complexes is important for a complete understanding of the processes. The
presented work focuses on the complexation of Cm(III) with DMDOHEMA studied by TRLFS in mono- and
biphasic (solvent extraction) systems. The formation of [Cm(DMDOHEMA)n]3+ (n = 1–3) in 1-octanol containing
1.7 mol L−1 of water with log β’1 = 2.6 ± 0.3, log β’2 = 4.0 ± 0.5, log β’3 = 4.3 ± 0.5 was confirmed.
In addition, fluorescence lifetime measurements indicated the formation of a 1 : 4 complex. Furthermore,
solvent extraction experiments were performed, varying the proton and nitrate concentrations. TRLFS
measurements of organic phases confirmed the existence of two species, [Cm(DMDOHEMA)3(NO3)
(H2O)1–2]2+ (dominant at high proton and nitrate concentrations) and [Cm(DMDOHEMA)4(H2O)]3+ (dominant
at low proton and nitrate concentrations). To support the proposed stoichiometries, vibronic sideband
spectroscopy (VSBS) was employed, allowing the observation of vibrations of functional groups coordinated
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Postprint §
DOI: 10.5445/IR/1000085317
Veröffentlicht am 03.07.2020
DOI: 10.1039/c8dt02504e
Zitationen: 12
Web of Science
Zitationen: 12
Zitationen: 12
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Nukleare Entsorgung (INE)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2018
Sprache Englisch
Identifikator ISSN: 1477-9226, 1477-9234
KITopen-ID: 1000085317
HGF-Programm 32.01.11 (POF III, LK 01) Extraktions- und Koordinationschemie der Actiniden
Erschienen in Dalton transactions
Verlag Royal Society of Chemistry (RSC)
Band 47
Heft 32
Seiten 10906–10914
Projektinformation GENIORS (EU, H2020, 755171)
Nachgewiesen in Dimensions
Web of Science
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