AVS 65th International Symposium & Exhibition
    Actinides and Rare Earths Focus Topic Thursday Sessions
       Session AC-ThA

Invited Paper AC-ThA1
Complexation, Characterization and Separation of the Lanthanides and Actinides: Shedding Light to Subtle Differences within the f-element Series

Thursday, October 25, 2018, 2:20 pm, Room 202C

Session: Early Career Scientists
Presenter: Gauthier Deblonde, Lawrence Berkeley National Laboratory
Authors: G. Deblonde, Lawrence Berkeley National Laboratory
C.H. Booth, Lawrence Berkeley National Laboratory
M. Kelley, Los Alamos National Laboratory
J. Su, Los Alamos National Laboratory
E. Batista, Los Alamos National Laboratory
P. Yang, Los Alamos National Laboratory
A. Müller, Lawrence Berkeley National Laboratory
P. Ercius, Lawrence Berkeley National Laboratory
A.M. Minor, Lawrence Berkeley National Laboratory
R.J. Abergel, Lawrence Berkeley National Laboratory
Correspondent: Click to Email

From the nuclear fuel cycles to the therapeutic use of radioisotopes for cancer diagnostics and treatment, the solution chemistry of lanthanides and actinides has become increasingly relevant to a number of applied problems. Understanding the fundamental bonding interactions of selective metal assemblies and the intrinsic differences between f-elements presents a rich set of scientific challenges and is critical to the development of highly efficient separation reagents and new actinide- or lanthanide-based therapeutics.

Our approach to these challenges uses a combination of techniques (EXAFS, liquid-liquid extraction, protein crystallization, UV-vis, fluorescence, DFT…) to characterize f-block aqueous complexes with highly selective and bio-inspired chelators or with more classical aminocarboxylate ligands. With the goal of always minimizing the amount of radioactive material needed and the worker’s radiation exposure, we are also investigating the use of TEM spectroscopy to characterize inorganic salts of heavy actinides (BkCl3, CfCl3...) while using only a few nanograms of actinides.

Our journey into the chemistry of the f-elements, and especially that of Am, Cm, Bk, and Cf, led us to capture subtle difference within the trivalent actinide series. A broad study on the aminocarboxylate complexes of Am3+, Cm3+, Bk3+, and Cf3+ by EXAFS spectroscopy revealed an unexpected change in speciation between the Cf chelates and its Am, Cm, and Bk analogues. Similarly, the study of the chelation of the lanthanide and actinide cations by some bio-inspired chelators (ex: siderophore derivatives), led us to develop versatile and highly efficient liquid-liquid extraction processes for the purification radioisotopes.