Mechanism of Water Oxidation Catalyzed by a Dinuclear Ruthenium Complex Bridged by AnthraquinoneReportar como inadecuado


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


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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.



Abstract We synthesized 1,8-bis2,2′:6′,2″-terpyrid-4′-ylanthraquinone btpyaq as a new dimerizing ligand and determined its single crystal structure by X-ray analysis. The dinuclear Ruthenium complex Ru2µ-Clbpy2btpyaqBF43 3BF43, bpy = 2,2′-bipyridine was used as a catalyst for water oxidation to oxygen with NH42CeNO36 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 3BF43 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 3BF43 with controlled-potential electrolysis at +1.40 V revealed that RuIV=O O=RuIV4+ is stable under electrolysis conditions. RuIII, RuII 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 RuV=O O=RuIV5+. View Full-Text

Keywords: water oxidation; Ruthenium complex; mechanism; Raman spectroscopy; electrochemistry water oxidation; Ruthenium complex; mechanism; Raman spectroscopy; electrochemistry





Autor: Tohru Wada 1,* , Shunsuke Nishimura 1, Taro Mochizuki 1, Tomohiro Ando 1 and Yuji Miyazato 2

Fuente: http://mdpi.com/



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