title: Molecule-based water-oxidation catalysts (WOCs): cluster-size-dependent dye-sensitized polyoxometalates for visible-light-driven O2 evolution.
abstract: 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 O2 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 = Ot (terminal oxygen) bonds in each individual cluster because it is well-known that Mo = Ot 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.
authors.affiliation: School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore.
authors.forename: Junkuo
authors.initials: J
authors.lastname: Gao
authors.forename: Shaowen
authors.initials: S
authors.lastname: Cao
authors.forename: Qiuling
authors.initials: Q
authors.lastname: Tay
authors.forename: Yi
authors.initials: Y
authors.lastname: Liu
authors.forename: Lingmin
authors.initials: L
authors.lastname: Yu
authors.forename: Kaiqi
authors.initials: K
authors.lastname: Ye
authors.forename: Peter Choon Sze
authors.initials: PC
authors.lastname: Mun
authors.forename: Yongxin
authors.initials: Y
authors.lastname: Li
authors.forename: Ganguly
authors.initials: G
authors.lastname: Rakesh
authors.forename: Say Chye Joachim
authors.initials: SC
authors.lastname: Loo
authors.forename: Zhong
authors.initials: Z
authors.lastname: Chen
authors.forename: Yang
authors.initials: Y
authors.lastname: Zhao
authors.forename: Can
authors.initials: C
authors.lastname: Xue
authors.forename: Qichun
authors.initials: Q
authors.lastname: Zhang