Quantitative UO bond activation in uranyl complexes silyl radical transfer.

Reductive silylation of the uranyl dication with 1,4-bis(trimethylsilyl)dihydropyrazine, or "Mashima's reagent", is detailed. The reagent simultaneously delivers silylium ions and electrons to multiple uranyl complexes, a pyridine dipyrrolide uranyl complex and a common uranyl-containing starting material, UOCl(OPPh). This reaction results in quantitative activation of thermodynamically robust UO bonds. The reductive functionalization of environmentally persistent actinyl species with Mashima's reagent is seen as a promising solution for nuclear waste remediation.