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      Molecule-based water-oxidation catalysts (WOCs) : cluster-size-dependent dye-sensitized polyoxometalates for visible-light-driven O2 evolution

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      Molecule-based water-oxidation catalysts (WOCs) Cluster-size-dependent.pdf (546.3Kb)
      Author
      Gao, Junkuo
      Cao, Shao-Wen
      Tay, Qiuling
      Liu, Yi
      Yu, Lingmin
      Ye, Kaiqi
      Mun, Peter Choon Sze
      Li, Yongxin
      Rakesh, Ganguly
      Loo, Say Chye Joachim
      Chen, Zhong
      Zhao, Yang
      Xue, Can
      Zhang, Qichun
      Date of Issue
      2013
      School
      School of Materials Science and Engineering
      School of Physical and Mathematical Sciences
      Version
      Published version
      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 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 = 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.
      Subject
      DRNTU::Science
      Type
      Journal Article
      Series/Journal Title
      Scientific reports
      Rights
      © 2013 The Authors(Nature Publishing Group). This paper was published in Scientific Reports and is made available as an electronic reprint (preprint) with permission of The Authors(Nature Publishing Group). The paper can be found at the following official DOI: [http://dx.doi.org/10.1038/srep01853]. One print or electronic copy may be made for personal use only. Systematic or multiple reproduction, distribution to multiple locations via electronic or other means, duplication of any material in this paper for a fee or for commercial purposes, or modification of the content of the paper is prohibited and is subject to penalties under law.
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      http://dx.doi.org/10.1038/srep01853
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