Synthesis, Structure, and Redox Properties of a trans-Diaqua Ru Complex That Reaches Seven-Coordination at High Oxidation States

Inorganic Chemistry
Roc MatheuAntoni Llobet

Abstract

In this work we have prepared and characterized two Ru complexes that contain the pentadenatate tda2-ligand (tda2-= [2,2':6',2″-terpyridine]-6,6″-dicarboxylate) that occupies the equatorial positions and two monodentate ligands aqua and/or dmso that occupy the axial positons: [trans-RuIII(tda-κ-N3O)(OH2ax)2]+, 3III(OH2)2+, and [RuII(tda-κ-N3O)(dmso)(OH2ax)], 4II. The latter is a useful synthetic intermediate for the preparation of Ru-tda complexes with different axial ligands. The two complexes have been characterized in the solid state by single-crystal XRD and by elemental analysis. In solution, complex 4IIhas been characterized by NMR spectroscopy as well as the one-electron reduction of complex 3III(OH2)2+. The electrochemical properties of 3III(OH2)2+and 4IIhave been assessed by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Complex 3III(OH2)2+shows the presence of four redox waves that are assigned to the VI/V, V/IV, IV/III, and III/II redox couples. The variation of the redox potentials is analyzed as a function of pH and is graphically presented as a Pourbaix diagram. Finally, the redox potentials displayed by both 3III(OH2)2+and 4IIare compared to related complexes previously reported in the literatu...Continue Reading

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