Mineral–Water Interface Reactions of Actinides

We review the analysis of lanthanide speciation at solid-water interfaces. We summarize the various mechanisms of lanthanide interaction with sorbent surfaces, such as surface complexation, precipitation and surface-induced redox reactions. There are a wide variety of available analytical techniques for understanding the speciation of lanthanides on surfaces and the reaction mechanisms of sorption. We also review recent advances in the utilization of quantum chemistry that widen the scope of lanthanide speciation studies. We review, summarize and discuss in detail the speciation of lanthanides, mainly Eu(III), at natural or synthetic mineral surfaces, and the available analytical techniques. We aim to collate valuable information about recent results for surface speciation analysis of lanthanides at solid-water interfaces.

Analytical approaches to the speciation of lanthanides at solid-water interfaces

The adsorption of selenite ions (SeO~-) from a dilute aqueous solution onto a freshly-cleaved calcite (1014) surface was studied with the X-ray standing wave (XSW) technique. The complex ion SeO z- is found to selectively adsorb at the CO~ site via ionic exchange, forming a two-dimensional solid-solution of the form Ca(SeO3)x(CO3) 1 x at the interface. The calcite (1014), (0006) and (1120) Bragg reflections were used to triangulate the Se position with respect to the calcite lattice. The local surface structure at the SeO~- adsorbate site, derived from the XSW results, is consistent with a model in which the base of the SeO~- trigonal pyramid aligns with (and replaces) the CO3 z- equilateral triangular group. The SeO~- adsorption saturated at a coverage of 0.02 monolayers. Under identical chemical conditions, selenate (SeO]) adsorption was inhibited. © 1997 Elsevier Science B.V.

Surface Science Letters X-ray standing wave investigation of the surface structure of selenite anions adsorbed on calcite

Sorption of tetravalent thorium on muscovite

The formation of Pu(IV)-oxo-nanoparticles from Pu(III) solutions by a surface-enhanced redox/polymerization reaction at the muscovite (001) basal plane is reported, with a continuous increase in plutonium coverage observed in situ over several hours. The sorbed Pu extends >70 A from the surface with a maximum concentration at 10.5 A and a total coverage of >9 Pu atoms per unit cell area of muscovite (0.77 μg Pu/cm2) (determined independently by in situ resonant anomalous X-ray reflectivity and by ex-situ alpha-spectrometry). The presence of discrete nanoparticles is confirmed by high resolution atomic force microscopy. We propose that the formation of these Pu(IV) nanoparticles from an otherwise stable Pu(III) solution can be explained by the combination of a highly concentrated interfacial Pu-ion species, the Pu(III)–Pu(IV) redox equilibrium, and the strong proclivity of tetravalent Pu to hydrolyze and form polymeric species. These results are the first direct observation of such behavior of plutonium on...

Surface-mediated formation of Pu(IV) nanoparticles at the muscovite-electrolyte interface.

Interaction of muscovite (0 0 1) with Pu3+ bearing solutions at pH 3 through ex-situ observations

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Interaction of muscovite (0 0 1) with Pu3+ bearing solutions at pH 3 through ex-situ observations