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Photoinduced hole transfer from tris(bipyridine)ruthenium dye to a high-valent iron-based water oxidation catalyst

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Abstract

An efficient water oxidation system is a prerequisite for developing solar energy conversion devices. Using advanced time-resolved spectroscopy, we study the initial catalytic relevant electron transfer events in the light-driven water oxidation system utilizing [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) as a light harvester, persulfate as a sacrificial electron acceptor, and a high-valent iron clathrochelate complex as a catalyst. Upon irradiation by visible light, the excited state of the ruthenium dye is quenched by persulfate to afford a [Ru(bpy)3]3+/SO4˙ pair, showing a cage escape yield up to 75%. This is followed by the subsequent fast hole transfer from [Ru(bpy)3]3+ to the FeIV catalyst to give the long-lived FeV intermediate in aqueous solution. In the presence of excess photosensitizer, this process exhibits pseudo-first order kinetics with respect to the catalyst with a rate constant of 3.2(1) × 1010 s−1. Consequently, efficient hole scavenging activity of the high-valent iron complex is proposed to explain its high catalytic performance for water oxidation.

Graphical abstract: Photoinduced hole transfer from tris(bipyridine)ruthenium dye to a high-valent iron-based water oxidation catalyst

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Publication details

The article was received on 05 Nov 2018, accepted on 19 Dec 2018 and first published on 05 Apr 2019


Article type: Paper
DOI: 10.1039/C8FD00167G
Faraday Discuss., 2019, Advance Article
  • Open access: Creative Commons BY license
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    Photoinduced hole transfer from tris(bipyridine)ruthenium dye to a high-valent iron-based water oxidation catalyst

    S. I. Shylin, Mariia V. Pavliuk, L. D’Amario, I. O. Fritsky and G. Berggren, Faraday Discuss., 2019, Advance Article , DOI: 10.1039/C8FD00167G

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