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Open AccessArticle

Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by Anthraquinone

1
Department of Chemistry, College of Science and Research Center for Smart Molecules, Rikkyo University, 3-34-1, Nishi-Ikebukuro, Toshima-ku, Tokyo 171-8501, Japan
2
School of Science and Engineering, Tokyo Denki University, Hatoyama, Hiki-gun, Saitama 350-0394, Japan
*
Author to whom correspondence should be addressed.
Catalysts 2017, 7(2), 56; https://doi.org/10.3390/catal7020056
Received: 5 January 2017 / Revised: 2 February 2017 / Accepted: 6 February 2017 / Published: 10 February 2017
(This article belongs to the Special Issue Water Oxidation Catalysis)
We synthesized 1,8-bis(2,2′:6′,2″-terpyrid-4′-yl)anthraquinone (btpyaq) as a new dimerizing ligand and determined its single crystal structure by X-ray analysis. The dinuclear Ruthenium complex [Ru2(µ-Cl)(bpy)2(btpyaq)](BF4)3 ([3](BF4)3, bpy = 2,2′-bipyridine) was used as a catalyst for water oxidation to oxygen with (NH4)2[Ce(NO3)6] as the oxidant (turnover numbers = 248). The initial reaction rate of oxygen evolution was directly proportional to the concentration of the catalyst and independent of the oxidant concentration. The cyclic voltammogram of [3](BF4)3 in water at pH 1.3 showed an irreversible catalytic current above +1.6 V (vs. SCE), with two quasi-reversible waves and one irreversible wave at E1/2 = +0.62, +0.82 V, and Epa = +1.13 V, respectively. UV-vis and Raman spectra of [3](BF4)3 with controlled-potential electrolysis at +1.40 V revealed that [Ru(IV)=O O=Ru(IV)]4+ is stable under electrolysis conditions. [Ru(III), Ru(II)] species are recovered after dissociation of an oxygen molecule from the active species in the catalytic cycle. These results clearly indicate that an O–O bond is formed via [Ru(V)=O O=Ru(IV)]5+. View Full-Text
Keywords: water oxidation; Ruthenium complex; mechanism; Raman spectroscopy; electrochemistry water oxidation; Ruthenium complex; mechanism; Raman spectroscopy; electrochemistry
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MDPI and ACS Style

Wada, T.; Nishimura, S.; Mochizuki, T.; Ando, T.; Miyazato, Y. Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by Anthraquinone. Catalysts 2017, 7, 56. https://doi.org/10.3390/catal7020056

AMA Style

Wada T, Nishimura S, Mochizuki T, Ando T, Miyazato Y. Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by Anthraquinone. Catalysts. 2017; 7(2):56. https://doi.org/10.3390/catal7020056

Chicago/Turabian Style

Wada, Tohru; Nishimura, Shunsuke; Mochizuki, Taro; Ando, Tomohiro; Miyazato, Yuji. 2017. "Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by Anthraquinone" Catalysts 7, no. 2: 56. https://doi.org/10.3390/catal7020056

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