One of the most significant challenges affecting the devleopment of a closed nuclear fuel cycle is the separation of minor actinides from lanthanide contaminants in spent nuclear fuel.  While several methods have been explored, the TALSPEAK process remains one of the most promising although, the fundamental chemistry behind the separation is still not fully understood.  The vast quantity of data available for TALSPEAK provides an excellent platform for studying the basic fundamental factors that dictate the chemical separations process.  In this contribution, we will describe our efforts evaluating the specific interactions of AmIII with DTPA for the pH range 2.5 - 4.5 through a combination of Raman spectroscopy and hybrid density functional theory (DFT) to understand the metal-ligand interactions.  Since the AmIII - DTPA complexes can exist at various degrees of protonation, the experimental data allows for determination of the ratios of those complexes at their respective degrees of protonation across the pH range investigated.  The DFT results will tie experimental trends in preferred protonation sites to Am-DTPA orbital interactions.  Also, we will describe how the electronic structure and bonding associated with DTPA leads to selectivity of minor actinide species.

Experimental-theoretical approach to understanding Am-DTPA complexation under TALSPEAK conditions

244th National Meeting (2012)

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