One of the most significant challenges affecting the development of a closed nuclear fuel cycle is the separation of minor actinides from lanthanide contaminants.  While several methods have been explored, one of the most promising is the Trivalent Actinide-Lanthanide Separation by Phosphorous reagent Extractant from Aqueous Komplexes process (TALSPEAK), although the fundamental chemistry driving the separation is still not completely understood.  Most published TALSPEAK work has been focused on measuring LnIII/AnIII separation factors with fewer studies on analysis of basic principles.  The experimental data available for TALSPEAK establishes a sound foundation for studying the fundamental factors that dictate the chemical separations process.  We will describe our efforts evaluating the specific interactions of AmIII with DTPA through a combination of Raman spectroscopy and hybrid density functional theory (DFT) directed at the metal-ligand interactions.  The results from the DFT and Raman will help explain the selectivity of DTPA for minor actinide species through changes in the electronic structure and metal-ligand bonding structure.

Using Raman spectroscopy and calculated vibrational levels to investigate Am-DTPA complexation under TALSPEAK conditions

245th National Meeting (2013)

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