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Issue 7, 2013
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Arrangement effect of the di-μ-oxo dimanganese catalyst and Ru(bpy)32+ photoexcitation centers adsorbed on mica for visible-light-derived water oxidation

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Abstract

A photosynthetic photosystem II (PS II) model was developed by adsorbing [(OH2)(terpy)MnIII(μ-O)2MnIV(terpy)(OH2)]3+ (1, terpy = 2,2′:6′,2′′-terpyridine) as an oxygen evolving center and Ru(bpy)32+ (bpy = 2,2′-bipyridine) as a photoexcitation center onto mica. The mica adsorbates were prepared by three different methods; Adsorbate A was prepared by adsorption of 1 followed by Ru(bpy)32+ on mica, and Adsorbates B and C were prepared by the opposite adsorption order and co-adsorption of 1 and Ru(bpy)32+, respectively. The UV-visible diffuse reflectance (DR) spectroscopic data and emission decay measurements of the photoexcited Ru(bpy)32+ suggested the different arrangements of 1 and Ru(bpy)32+ among the three adsorbates in a mica interlayer. For Adsorbate A, Ru(bpy)32+ could be adsorbed near the mica surface, being shallowly intercalated relative to 1. For Adsorbate B, 1 is adsorbed near the mica surface, Ru(bpy)32+ being deeply intercalated relative to 1. For Adsorbate C, either 1 or Ru(bpy)32+ could be randomly intercalated relative to the other adsorbates. In photochemical water oxidation experiments, a significant amount of O2 was evolved when visible light was used to irradiate an aqueous suspension of Adsorbate A containing a S2O82− electron acceptor in a liquid phase, whereas O2 was not evolved under the same conditions when using Adsorbates B and C. 1 is considered to work for photochemical water oxidation in Adsorbate A due to an efficient electron transport from deeply intercalated 1 to S2O82− ions in a liquid phase via Ru(bpy)32+ photoexcitation near the mica adsorbate surface.

Graphical abstract: Arrangement effect of the di-μ-oxo dimanganese catalyst and Ru(bpy)32+ photoexcitation centers adsorbed on mica for visible-light-derived water oxidation

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Publication details

The article was received on 05 Jan 2013, accepted on 08 Mar 2013 and first published on 08 Mar 2013


Article type: Paper
DOI: 10.1039/C3CY00010A
Catal. Sci. Technol., 2013,3, 1776-1781

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    Arrangement effect of the di-μ-oxo dimanganese catalyst and Ru(bpy)32+ photoexcitation centers adsorbed on mica for visible-light-derived water oxidation

    M. Hirahara, H. Yamazaki, S. Yamada, K. Matsubara, K. Saito, T. Yui and M. Yagi, Catal. Sci. Technol., 2013, 3, 1776
    DOI: 10.1039/C3CY00010A

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