Abstract
AbstractMononuclear ruthenium complexes with a pentadentate ligand, N,N‐bis[(isoquinolin‐1‐yl)methyl][6‐(pyridin‐2‐yl)pyridin‐2‐yl]methanamine (DIQ‐Bpy), were synthesized and characterized by 1H NMR spectroscopy, elemental analysis, electrochemistry, and theoretical calculations. The oxidation of water by [Ru(DIQ‐Bpy)(H2O)]2+ was observed in the presence of excess amounts of CeIV. Relative to [Ru(DPA‐Bpy)(H2O)]2+ [DPA‐Bpy = N,N‐bis(2‐pyridinylmethyl)‐2,2′‐bipyridine‐6‐methanamine], the substitution of pyridine groups in DPA‐Bpy with electron‐withdrawing isoquinolines results in higher redox potential and lower activity for the oxidation of water by [Ru(DIQ‐Bpy)(H2O)]2+. A kinetic study of water oxidation by [Ru(DPA‐Bpy)(H2O)]2+ suggests a mononuclear pathway for the oxidation of water. The noncovalent interaction between isoquinoline groups in [Ru(DIQ‐Bpy)(H2O)]2+, which favors the formation of dinuclear species, might account for the lower activity for water oxidation by [Ru(DIQ‐Bpy)(H2O)]2+.
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