Argonne National Laboratory (ANL) grew out of Fermi's experiment under Stagg field and subsequent follow-up studies at Argonne Laboratory Site A, located at Red Gate Woods, in the Chicago suburbs. At its inception in 1946 ANL was tasked with developing nuclear power for electricity. By the late 1970’s the fundamental chemistry efforts associated with this task had expressed themselves in two well-established efforts, one focusing on the separation and isolation of transuranic elements and their fission products and the other on building an understanding of the chemical and physical properties of these new elements. Out of this effort came new selective extractants, including the class of organophosphates associated with the TRUEX process and efficient intra-lanthanide selectivity, both important for the advancement of spent fuel reprocessing. Characterization of the new elements included a significant synthesis effort, and a systematic study of <i>f</i>-ion optical properties within the context of a parametric crystal-field scheme. This body of work provides the underpinning of the fundamental studies ongoing at ANL today. The combined programs are conducted in purpose-designed hot laboratories, co-located on a site with the Advanced Photon Source, a third-generation synchrotron, and with the guidance provided by theoretical calculations conducted on state-of-the-art large computing facilities. Conceptually built primarily around understanding the partitioning of free-energy in liquid-liquid separations processes, the current scientific program is centered on characterizing metal-ion solution speciation at varying length scales and using this information to build predictive modeling capabilities. To be discussed are recent results on aqueous-phase correlations and their correspondence to solid-state structures, the multiple length-scale organization of metal-extractant complexes in organic phases and their similarities with more broadly studied soft-matter systems, and new, atomic-scale information on ion-correlations at aqueous interfaces. The implications of this work will be outlined in terms of underpinning new separations opportunities and more broadly in terms of predicting metal-ion behavior in complex systems, including those found in the geosphere. This work was performed for the U.S. DOE, OBES, Division of Chemical Sciences, Geosciences, and Biosciences, Heavy Elements Chemistry, funded at Argonne National Laboratory under contract DE-AC02-06CH11357

Heavy element chemistry and separations science at Argonne National Laboratory: A current perspective

249th National Meeting (2015)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.