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Molecule-Based Water-Oxidation Catalysts (WOCs): Cluster-Size-Dependent Dye-Sensitized Polyoxometalates for Visible-Light-Driven O-2 Evolution
Junkuo Gao, Shaowen Cao, Qiuling Tay, Yi Liu, Lingmin Yu, Kaiqi Ye, Peter Mun Choon Sze, Yongxin Li, , Say Loo Chye JoachimShow More
Published in
Volume: 3
From atomic level to understand the cluster-size-dependant behavior of dye-sensitized photocatalysts is very important and helpful to design new photocatalytic materials. Although the relationship between the photocatalytic behaviors and particles' size/shape has been widely investigated by theoretical scientists, the experimental evidences are much less. In this manuscript, we successfully synthesized three new ruthenium dye-sensitized polyoxometalates (POM-n, n relate to different size clusters) with different-sized POM clusters. Under visible-light illumination, all three complexes show the stable O-2 evolution with the efficient order POM-3 > POM-2 > POM-1. This cluster-size-dependent catalytic behavior could be explained by the different numbers of M = O-t (terminal oxygen) bonds in each individual cluster because it is well-known that Mo = O-t groups are the catalytically active sites for photooxidation reaction. The proposed mechanism of water oxidation for the dye-sensitized POMs is radical reaction process. This research could open up new perspectives for developing new POM-based WOCs.
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