Incorporation of hydroxypyridinone ligands into self-assembled monolayers on mesoporous supports for selective actinide sequestration

In this study, three isomers of hydroxypyridinones (1,2-HOPO, 3,2-HOPO, and 3,4-HOPO) were attached to self-assembled monolayers on mesoporous silica (SAMMS). The HOPO-SAMMS materials have superior solid adsorbents properties: they do not suffer from solvent swelling; their rigid, open pore structure allows rapid sorption kinetics; their extremely high surface area enables the installation of high functional density; and being silica-based, they are compatible with vitrification into a final vitreous waste form. Kinetics, equilibrium, and selectivity of the adsorptions of actinide on the HOPO-SAMMS at various pH values and in the presence of other metal cations, anions, and competing ligands are reported. Rapid sequestration of U(VI), Np(V), and Pu(IV) was observed. Very little competition from transition metal cations and common species was observed.