Our group has been interested in studying uranyl peroxide nanoclusters (UPCs) since their discovery in 2005 to study property-size-composition-stability relationships. We have now utilized electrospray ionization mass spectrometry (ESI-MS) with collision-induced dissociation (CID) to probe clusters bridging ligands through fragment ion products. The interpretation has revealed clusters transfer into the gas phase through electrochemistry at the electrospray source, considering the fragment ions do not equate to the expected mass to charge of monomeric units if we were to assume the initial known solid-state chemistry. We have utilized the CID technique on nanoclusters U24, [(UO2)24(O2)24(OH)24]24–, U28, [(UO2)28(O2)42]28–, U24Py12, [(UO2)24(O2)24(P2O7)12]48–, U60, [(UO2)60(O2)60(OH)60]60–, and U60Ox30, [(UO2)60(O2)60(C2O4)30]60–. Gas phase reactions complicate the ultimate interpretation, yet nanoclusters with pyrophosphate and oxalate bridging ligands can easily be distinguished by the fragmentation pattern. The technique and interpretation will allow us to probe UPCs speciation in an aqueous solution as a function of time to study stability relationships amongst nanoclusters.

Electrospray ionization tandem mass spectrometry with collision induced dissociation: Probing uranyl-bridging ligands

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