Hydrolysis and subsequent condensation reactions play an important role in the aqueous chemistry of tetravalent actinide ions. The resultant oligomers are known to exhibit chemistries very different from that of their monomeric counterparts. First forming in solution, the resulting precipitates have been historically characterized as chemically ill-defined and amorphous. Recent studies have begun to change this perception as the characterization of structural correlations in solutions reveals well-defined metal interactions, suggesting the possibility of harnessing this intractable chemistry.  Our investigations have found that tetravalent-actinide 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 and quantified by high-energy x-ray scattering (HEXS).The results from these structural studies are being used as input for electronic calculations that in turn are providing a wealth of insight into the means by which these clusters form, including the important role played by pH, temperature, and anion. This work was performed for the U.S. DOE, OBES, Division of Chemical Sciences, Geosciences, and Biosciences, under contract DE-AC02-06CH11357.

Tetravalent actinide nanparticles in aqueous solution: Structure and reactivity

247th National Meeting (2014)

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