Lanthanides play a critical role in advanced technology relevant to the growth and health of the US economy. There is great need to optimize the separation methods to be highly selective, since separating contiguous lanthanides is particularly challenging. Lanthanide complexation processes related to their solvent-extraction separations have been theoretically examined. Selected results will be discussed from over 300 compound configurations investigated and correlated in a heavily intensive computational study performed with OLCF and NICS supercomputers at Oak Ridge National Laboratory.The ultimate goal of our research is to enable knowledge-based design of separation agents, and in the short term, to develop practical computational protocols with sufficient accuracy and robustness to be predictive yet sufficiently fast to be applied to many systems. Through a collaborative experimental and theoretical project, we seek to explain trends observed experimentally in the separation of lanthanides between solvent phases as a function of solvent and complexing agent. Our work provides a fundamental understanding of the coordination preferences involved in a typical extraction process. The theoretical protocol involves an in-depth analysis of the reactions involved in a two-phased extraction method by considering different possible coordination environments, thereby gaining fundamental understanding of the mechanism of complex formation. The thermodynamic and structural information obtained from computations present a unique contribution to separations chemistry.Harrison and Penchoff gratefully acknowledge the support of the National Science Foundation under grant OCI-0904972 �Computational chemistry and physics beyond the petascale.�

Integrated theoretical and experimental study for optimization and design of extracting agents for separations of lanthanides

247th National Meeting (2014)

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