Soft-donor dipicolinamide derivatives for selective actinide(III)/lanthanide(III) separation: the role of S- vs. O-donor sites

Ingrid Lehman-Andino; Jing Su; Konstantinos E. Papathanasiou; Teresa M. Eaton; Jiwen Jian; David Dan; Thomas E. Albrecht-Schmitt; Christopher J. Dares; Enrique R. Batista; Ping Yang; John K. Gibson; Konstantinos Kavallieratos

doi:10.1039/C8CC07683A

Soft-donor dipicolinamide derivatives for selective actinide(iii)/lanthanide(iii) separation: the role of S- vs. O-donor sites†

Ingrid Lehman-Andino,^a Jing Su,

^b Konstantinos E. Papathanasiou,^a Teresa M. Eaton,‡^c Jiwen Jian,^c David Dan,

^d Thomas E. Albrecht-Schmitt,

^d Christopher J. Dares,

^a Enrique R. Batista,

*^b Ping Yang,

*^b John K. Gibson

*^c and Konstantinos Kavallieratos

*^a

Author affiliations

* Corresponding authors

^a Department of Chemistry and Biochemistry and Biomolecular Sciences Institute, Florida International University, USA
E-mail: kavallie@fiu.edu

^b Theoretical Division, Los Alamos National Laboratory, USA
E-mail: pyang@lanl.gov, erb@lanl.gov

^c Chemical Sciences Division, Lawrence Berkeley National Laboratory, USA
E-mail: jkgibson@lbl.gov

^d Department of Chemistry and Biochemistry, Florida State University, USA

Abstract

Selectivity for An(III) vs. Ln(III) binding and extraction using dipicolinamide analogs containing the C [double bond, length as m-dash] O vs. CS groups was investigated in solution and the gas-phase, and by DFT calculations. The results show higher selectivity for complex formation and extraction for Am(III) vs. Eu(III) for the softer dithioamide vs. the diamide ligand, while in CH₃CN the diamide binds more strongly than the thioamide to several Ln(III), forming 1 : 1 complexes.

This article is part of the themed collection: New molecules and materials from the f-block

Chemical Communications

Soft-donor dipicolinamide derivatives for selective actinide(iii)/lanthanide(iii) separation: the role of S- vs. O-donor sites†

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Soft-donor dipicolinamide derivatives for selective actinide(III)/lanthanide(III) separation: the role of S- vs. O-donor sites

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