Research into ligand complexation reactions with f-element cations is motivated by both the desire to understand the electronic structure and bonding of these elements, as well as to further develop the use of their complexes in applications such as nuclear fuel cycles and radioactive waste remediation.  Exploring the fundamental chemistry that underpins a range of actinide separation strategies is vital to facilitate development and implementation of fuel recycling and waste disposition/minimization options.  For example, soft donor extractants have attracted a lot of attention due to their ability to selectively complex An(III) versus Ln(III) ions, a challenging separation as a result of the chemical similarity of these ions.  In order to probe the role that covalency plays in effecting selectivity, we are studying structurally similar Ln(III) and An(III) complexes featuring N, O, S and Se donor ligands.  Bonding comparisons across the An(IV) series are also considered.  In particular, we incorporate transuranic molecules into our studies, of which far less is known compared to the chemistry of the lanthanides or thorium/uranium.  The syntheses and characterization of these complexes, which include �-ketoiminates, diselenophosphinates, and tri(amidato)amine ligands, will be described.  We will analyze for bonding differences that have implications for ligand design in actinide separation technology.

f-Element coordination chemistry with relevance to nuclear fuel cycle separation challenges

243rd National Meeting (2012)

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