Abstract
AbstractFour heterotrinuclear strings of metal atoms stabilized by dipyridylamide (dpa–) ligands were synthesized and characterized. The metal frameworks of Ru2Cu(dpa)4Cl2 (1), its monooxidized counterpart [Ru2Cu(dpa)4Cl2]PF6 (2), and their nickel homologues, Ru2Ni(dpa)4Cl2 (3) and [Ru2Ni(dpa)4Cl2]PF6 (4), were shown by X‐ray diffraction to be nonsymmetric, in spite of a severe disorder affecting the metal positions. The metal string is composed of a Ru dimer with a short Ru–Ru bond that is completed with the heterometal at a longer distance from the central ruthenium atom. This nonsymmetric structure was confirmed from NMR spectroscopy. The [Ru2M]6+ framework of 1 and 3 was shown from spectroelectrochemical analysis and DFT calculations to exist in the form of a mixed‐valent [Ru2]5+ moiety coupled to a formally M+ heterometal. The temperature‐dependant magnetic susceptibility of these compounds is reported and interpreted by means of a model previously applied to [Ru2]5+ complexes. The redox chemistry of 1 and 3 was investigated by cyclic voltammetry, and the electronic structure of the mono‐ and dioxidized species was assigned from the observed changes in the UV/Vis spectra and from DFT calculations.(© Wiley‐VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2008)
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