Conversion of a UO(2)(2+) Precursor to UH(+) and U(+) Using Tandem Mass Spectrometry to Remove Both “yl” Oxo Ligands

[Image: see text] Multiple-stage collision-induced dissociation (CID) of a uranyl propiolate cation, [UO(2)(O(2)C–C≡CH)](+), can be used to prepare the U-methylidyne species [O=U≡CH](+) [J. Am. Soc. Mass Spectrom.2019, 30, 796–805]. Here, we report that CID of [O=U≡CH](+) causes elimination of CO to create [UH](+), followed by a loss of H(•) to generate U(+). A feasible, multiple-step pathway for the generation of [UH](+) was identified using DFT calculations. These results provide the first demonstration that multiple-stage CID can be used to prepare both U(+) and UH(+) directly from a UO(2)(2+) precursor for the subsequent investigation of ion–molecule reactivity.