Abstract: | The treatment of chloridobis(4‐methylthiazolyl)isoindoline]palladium(II) (4‐Mebti)PdCl] with sodium tetrakisbis‐3,5(trifluoromethyl)phenyl]boranate NaBArF] in the absence of donor ligands or solvents results in the exclusive formation of the dinuclear cationic complex {(4‐Mebti)Pd}2Cl]+ independent of the stoichiometry of the reactants. The new compound crystallizes either in the space group or in C2/c depending on the amount of co‐crystallized solvent. In both cases, the molecular structure of the dinuclear cation reveals a sterically crowded situation with the Pd2+ ion bound in a non‐planar coordination environment. In solution, {(4‐Mebti)Pd}2Cl]+ reacts with acetonitrile to form the neutral (4‐Mebti)PdCl] and an equilibrium mixture of different complexes, from which the mononuclear species (4‐Mebti)Pd(NCCH3)]+ can be isolated as the pure BArF derivative. |