The core ions [MLn](2+) with n = 1-3, where L = 1,10-phenanthroline and M is a first-row transition metal, have been successfully transferred from aqueous solution into the gas phase by electrospraying and then probed for their stabilities by collision-induced dissociation in a triple quadrupole mass spectrometer. The triply ligated metal dications [ML3](2+) were observed to dissociate by the extrusion of a neutral ligand, while ligand loss from both [ML2](2+) and [ML](2+) was accompanied by electron transfer. Comparisons are provided between gas-phase stabilities and stabilities for ligand loss measured in aqueous solution at 298 K. The measured onset for ligand loss from [ML3](2+) is quite insensitive to the metal, while a distinct stability order has been reported for aqueous solution. Low level density functional theory (DFT) calculations predict an intrinsic stability order for loss of ligand from [ML2](2+), but it differs from that in aqueous solution. Substantial agreement was obtained for the stability order for the loss of ligand from [ML](2+) deduced from onset energies measured for charge separation, computed with DFT, and reported for aqueous solution where hydration seems less decisive in influencing this stability order. A qualitative potential-energy diagram is presented that allows the energy for charge separation to be related to the energy for neutral ligand loss from [ML](2+) and shows that IE(M+) is decisive in determining the intrinsic stability order for loss of ligand from [ML](2+).