Intrinsic reactivity of [OUCH] : Apparent synthesis of [OUS] by reaction with CS.

Rationale: Building on our report that collision-induced dissociation (CID) can be used to create the highly reactive U-alkylidyne species [O=U≡CH] , our goal was to determine whether the species could be as an intermediate for synthesis of [OUS] by reaction with carbon disulfide (CS ).

Methods: Cationic uranyl-propiolate precursor ions were generated by electrospray ionization, and multiple-stage CID in a linear trap instrument was used to prepare [O=U≡CH] . Neutral CS was admitted into the trap through a modified He inlet and precision leak valves.

Results: The [O=U≡CH] ion reacts with CS to generate [OUS] . CID of [OUS] causes elimination of the axial sulfide ligand to generate [OU] . Using isotopically labeled reagent, we found that [OUS] reacts with O to create [UO ] .

Conclusions: [O=U≡CH] proves to be a useful reagent ion for synthesis of [OUS] , a species that to date has only been created by gas-phase reactions of U and U . Dissociation of [OUS] to create [OU] , but not [US] , and the efficient conversion of the species into [UO ] , is consistent with the relative differences in U-O and U-S bond energies.