Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf
1 PublicationStructural characterization of Am(III) and Pu(III)-DOTA complexes
Audras, M.; Berthon, L.; Berthon, C.; Guillaumont, D.; Dumas, T.; Illy, M. C.; Martin, N.; Zilbermann, I.; Ben-Eliyahu, Y.; Moissev, Y.; Bettelheim, A.; Camelli, S.; Hennig, C.; Moisy, P.
Abstract
The complexation of DOTA ligand (1,4,7,10-tetrazacyclodecane-1,4,7,10-tetraacetic acid) with two trivalent actinides (Am3+ and Pu3+) was investigated by UV-visible spectrophotometry, Nuclear Magnetic Resonance (NMR) spectroscopy and extended X-ray absorption fine structure (EXAFS) in conjunction with computational methods. The complexation process of these two cations is similar to what has been previously observed with lanthanides(III) of similar ionic radius. The complexation takes places in different steps and ends up with the formation of a (1:1) complex [(An(III)DOTA)(H2O)]- where the cation is bonded to the nitrogen atoms of the ring, the four carboxylate arms and a water molecule is completing the coordination sphere. Nevertheless, the formation of An(III)-DOTA complexes is faster than the Ln(III)-DOTA systems of equivalent ionic radius. Furthermore, it is found that An-N distances are slightly shorter than Ln-N distances. Theoretical calculations have shown that the slightly higher affinity of DOTA toward Am over Nd is correlated with slightly enhanced Ligand-to-metal charge donation arising from oxygen and nitrogen atoms.
Keywords: DOTA; UV-visible spectrophotometry; NMR; EXAFS; DFT calculations; Americium; Plutonium; lanthanides
Involved research facilities
- Rossendorf Beamline at ESRF DOI: 10.1107/S1600577520014265
Related publications
- DOI: 10.1107/S1600577520014265 is cited by this (Id 25773) publication
-
Inorganic Chemistry 56(2017), 12248-12259
DOI: 10.1021/acs.inorgchem.7b01666
Cited 22 times in Scopus
Permalink: https://www.hzdr.de/publications/Publ-25773
Years: 2023 2022 2021 2020 2019 2018 2017 2016 2015