A Molecular Light-Driven
Water Oxidation Catalyst
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Abstract
Two mononuclear Ru(II) complexes, [Ru(ttbt)(pynap)(I)]I
and [Ru(tpy)(Mepy)<sub>2</sub>(I)]I (tpy = 2,2′;6,2″-terpyridine;
ttbt = 4,4′,4″-tri-<i>tert</i>-butyltpy; pynap
= 2-(pyrid-2′-yl)-1,8-naphthyridine;
and Mepy = 4-methylpyridine), are effective catalysts for the oxidation
of water. This oxidation can be driven by a blue (λ<sub>max</sub> = 472 nm) LED light source using [Ru(bpy)<sub>3</sub>]Cl<sub>2</sub> (bpy = 2,2′-bipyridine) as the photosensitizer. Sodium persulfate
acts as a sacrificial electron acceptor to oxidize the photosensitizer
that in turn drives the catalysis. The presence of all four components,
light, photosensitizer, sodium persulfate, and catalyst, are required
for water oxidation. A dyad assembly has been prepared using a pyrazine-based
linker to join a photosensitizer and catalyst moiety. Irradiation
of this intramolecular system with blue light produces oxygen with
a higher turnover number than the analogous intermolecular component
system under the same conditions