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