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Enabling light-driven water oxidation via a low-energy RuIV=O intermediate

The discovery of catalysts capable of driving water oxidation at relatively low overpotential is a key challenge for efficient photoinduced water oxidation. The mononuclear Ru(II) polypyridyl complex (1) has been examined as a catalyst for visible-light-driven water oxidation in a three-component homogeneous system containing [Ru(bpy)3]2+ as a photosensitizer, persulfate as a sacrificial electron acceptor and 1. We have successfully demonstrated that the earlier proposed “direct pathway” takes place by the use of a mild oxidant such as the photogenerated [Ru(bpy)3]3+ (1.26 V vs NHE) to drive water oxidation at pH >3. The overall quantum yield of 9 % and a TOF of 0.12 s-1 were found for photochemical water oxidation. These values render 1 one of the most active mononuclear ruthenium-based catalysts for light-driven water oxidation in a homogeneous system.

PCCP 2013, 15, 14058-14068, DOI: 10.1039/C3CP52038B.