Hydrolysis and subsequent condensation reactions play an important role in the aqueous chemistry of tetravalent actinide ions. The resultant oligomers are known to exhibit a chemistry very different from that of their monomeric counterparts. Long thought to be intractable, amorphous, and chemically ill-defined, our recent structural and property characterization, both in solution and in the solid state, is revealing a very different picture. The hydrolysis products are often well defined nanoparticles that can be crystallized and structurally characterized via standard single-crystal techniques. The presence of these oligomeric species in solution, often as monodisperse nanoclusters, is verified by high-energy x-ray scattering (HEXS). Included in this presentation will be the impact of our results on understanding the role of colloids in both geochemical modeling and nuclear-waste reprocessing.This work was performed for the U.S. DOE, OBES, Division of Chemical Sciences, Geosciences, and Biosciences, under contract DE-AC02-06CH11357.

Tetravalent actinide nanoparticles in aqueous solution: Structure and reactivity

243rd National Meeting (2012)

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