We are designing design, synthesizing, and testing reusable mesoporous materials for actinide and lanthanide sequestration, separation, and sensing. Our experimental-computational collaboration studies three types of materials with a high binding capacity for selected actindes and lanthanides: functionalized mesoporous silica, mesoporous carbon, and ferrihydrite. The affinity for target actinides of several ligands grafted to mesoporous silica, as well as their binding geometry, has been predicted by ab initio relativistic density functional theory (DFT) geometry optimization calculations, and compared to experimental batch sorption and X-ray absorption spectroscopy (XAS) measurements. Additionally, these batch studies have established the ability to reuse the materials as high-capacity sorbents. Ordered mesoporous carbon (OMC) has proven far superior to activated carbon in terms of Pu(VI) capacity and sorption kinetics. Batch and XAS studies of mesoporous and nanoparticulate ferrihydrite interactions with Pu(VI) have revealed interesting light-induced redox chemistry at the iron-oxide surface that may yield separation capabilities. We are also studying the effects of the presence of competing ions, as well as systematic ligand variation. We are exploring OMC-based electrodes offer a promising route for electrochemical separation and sensing of actinides and lanthanides.

Novel mesoporous materials for actinide and lanthanide sequestration and separation

245th National Meeting (2013)

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