Structural Characterization of Am(III)- and Pu(III)-DOTA Complexes

Matthieu Audras, Laurence Berthon, Claude Berthon, Dominique Guillaumont, Thomas Dumas, Marie Claire Illy, Nicolas Martin, Israel Zilbermann, Yulia Moiseev, Yeshayahu Ben-Eliyahu, Armand Bettelheim, Sebastiano Cammelli, Christoph Hennig, Philippe Moisy

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

Abstract

The complexation of 1,4,7,10-tetrazacyclodecane-1,4,7,10-tetraacetic acid (DOTA) ligand with two trivalent actinides (Am3+ and Pu3+) was investigated by UV-visible spectrophotometry, NMR spectroscopy, and extended X-ray absorption fine structure 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 place in different steps and ends 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 to complete the coordination sphere. 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 showed 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.

Original languageEnglish
Pages (from-to)12248-12259
Number of pages12
JournalInorganic Chemistry
Volume56
Issue number20
DOIs
StatePublished - 16 Oct 2017

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

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